Atomisation Technologies Used in - Spray Drying in The Dairy Industry - A Review
Atomisation Technologies Used in - Spray Drying in The Dairy Industry - A Review
PII: S0260-8774(18)30364-9
DOI: 10.1016/j.jfoodeng.2018.08.027
Please cite this article as: Jonathan J. O’Sullivan, Eve-Anne Norwood, James A. O’Mahony, Alan L.
Kelly, Atomisation technologies used in spray drying in the dairy industry: A review, Journal of Food
Engineering (2018), doi: 10.1016/j.jfoodeng.2018.08.027
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5 aSchool of Food and Nutritional Sciences, University College Cork, Cork, Ireland
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9 Abstract
11 feed is converted to discrete droplets, greatly increasing the surface area of the feed liquid and
12 thereby increasing considerably the achievable rates of evaporation of water. These droplets,
13 through evaporation of water in the main dryer chamber, become individual powder particles
14 during the spray-drying process. This review provides a comprehensive examination of the
15 most recent developments in atomisation technology for spray-drying, with a particular focus
16 upon dairy applications (e.g., skim and whole milk powders, casein- and whey-based powders,
17 and fat-filled milk powders). As well as a review of principles of different technologies for
19 ultrasonic atomisers and electrospray atomisers, the industrial applicability and challenges in
20 use of each approach to atomisation are presented. Approaches for monitoring the atomisation
21 process and other factors that influence atomisation, such as feed composition and key process
23
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26 1. Introduction
27 Spray-drying is a unique unit operation where a bulk fluid stream is converted into discrete
28 solid particles, through the dispersion of the stream, by a process known as atomisation, into
29 individual droplets. These come in intimate contact with a hot gaseous drying medium,
30 resulting in rapid and almost complete moisture evaporation, and thus drying. The application
31 of this process in the dairy industry has been a key enabler in the production of dried milk
32 ingredients (O’Connell and Flynn, 2007). Applications of spray-drying within the dairy
33 industry date from the early 1800s, yet it was not until the 1850s that it became technologically
34 feasible to implement this unit operation industrially, and it was first patented in 1872 by
36 A range of products are produced at large commercial scale by spray-drying in the dairy
37 industry, each with differing characteristics, based on the ratio of protein:fat:carbohydrate, and
38 the type of protein, within a given powder and, to a lesser extent, the process conditions that
39 are employed (Schuck et al., 2016). Dairy products possess an excellent nutritional profile but
40 are inherently perishable, due to their high moisture content (Muir, 1996). As a consequence,
41 a significant proportion of material derived from milk is dried to significantly decrease levels
42 of microbial activity, owing to reduced water activity, and for ease of global distribution and
43 more economic transportation due to reduced overall bulk (O’Connell and Flynn, 2007; Schuck
44 et al., 2016). There has been a progressive increase in the global production of milk products;
45 for instance, between 2012 to 2016 there was a 5.47% increase in production from 771,262 to
46 815,965 thousand tonnes, respectively (FAO, 2016). Thus, it is essential that this greater
47 volume of milk is preserved for the benefit of the global population, in particular in regions
48 where climatic conditions are not conducive for dairy farming and/or are liable to increase the
49 rate of spoilage of liquid dairy systems; for this purpose, manufacture of powder products using
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51 Of the different stages of spray-drying (Fig. 1), one of the most critical is atomisation, as
52 this is where the conversion of the bulk fluid stream into discrete droplets takes place.
53 Atomisation typically occurs at the top of the main chamber of a spray dryer, through a device
54 known as an atomiser (Filkova et al., 2014). The atomiser transforms bulk liquid streams into
55 droplets using one of a number of different approaches, one of the most common of which is
56 pressure nozzle atomisation, whereby the liquid stream is passed through a narrow aperture,
57 generating tandem homogenisation and spray effects (Patel et al., 2009). Other approaches that
58 are used to atomise such liquid streams include rotary wheel nozzles and pneumatic nozzles,
59 and more novel approaches, including ultrasonic nozzles and electrospray technology (Gibbs
61 There are numerous challenges associated with the atomisation process, ranging from
62 considerations prior to the procurement of the technology itself (e.g., available capital,
63 proposed scale of operation, intended product formats and physical properties, etc.), to its
65 the physical properties of the material which is to be atomised and subsequently dried, and the
66 target properties of the resulting powder (e.g., bulk density, flowability and free fat) is required
67 to ensure selection of the most appropriate atomisers (Schuck et al., 2016). However, from a
68 dairy processor’s perspective, the use of a spray dryer will often not be confined to a single
69 product category, and the overall configuration of the spray dryer must be sufficiently robust
70 and flexible to produce the desired range of powders, with the required physical properties and
71 quality attributes (O’Connell and Flynn, 2007). The range of fluids being atomised within the
72 dairy sector have very different physicochemical properties (e.g., density, surface tension and
73 viscosity) and associated challenges depending on their formulations, where streams could be
74 relatively high in protein (e.g., milk protein concentrate), carbohydrate (e.g., lactose, whey
75 protein concentrate 35) or fat (e.g., whole milk powder, fat-filled milk powders) (Crowley et
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76 al., 2015; Fitzpatrick et al., 2007; Kim et al., 2002; O’Sullivan et al., 2018; O’Sullivan,
77 Schmidmeier et al., 2017; O’Sullivan & O’Mahony, 2016; Roos, 2002). Furthermore,
78 depending on the scale of operation and the commercial value of the final product, the atomiser
79 must be sufficiently robust to ensure continuous production with minimal downtime for
81 The aim of this review is to outline the principles of atomisation as an integral component
82 of the spray-drying process, and to critically compare the more commonly-used atomisation
83 technologies. A particular focus has been placed on the industrial relevance (e.g., CapEx,
84 operational cost or OpEx, capacity, etc.) of each of the discussed atomisation technologies
85 within the dairy sector for the efficient generation of droplets of a given size, and thus powders
86 with a desired microstructure (e.g., size, surface composition, etc.), physical properties (e.g.,
87 bulk density) and functionality in use (e.g., solubility, foaming and emulsion stability
88 considerations).
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90 2. Atomisation technology
91 The aim of atomisation is to increase substantially the surface area of the dairy
92 concentrate feed before it is dried (Filkova et al., 2014). The rate of evaporation is directly
93 proportional to droplet surface area; thus, it is highly desirable to achieve fine atomisation for
94 more efficient operation of the spray dryer, and it is also critical in determining physical
95 properties of the resultant powders, such as bulk density, wettability, dispersability, and
96 solubility (Forny et al., 2011; Hanley, Byrne, et al., 2011; Hanley, Cronin, et al., 2011; Patel
97 et al., 2009).
98 The principal properties of the spray of droplets resulting from atomisation are the mean
99 droplet size and droplet size distribution, which are reflected in the properties of the resultant
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100 powder (Fig. 2a). These properties depend upon a number of factors, including the atomisation
101 technology employed, operating conditions, and the compositional and physicochemical
102 properties of the atomised liquid (e.g., total solids content, rheological behaviour, and size of
103 particles in the feed stream); key parameters include concentrate viscosity, surface tension and
104 density (Pisecky, 2012). The feed stream to a spray dryer is typically a concentrated liquid feed,
105 which possesses an elevated solids content following evaporation, ranging from 26 to 60%
106 (w/w) depending on the specific product (Schuck et al., 2016), with the achievable solids
107 content of the feed normally determined by the viscosity of, and ability to pump, the
109 With greater energy density applied during the atomisation process, smaller droplets in
110 the spray are achievable, often with a narrow span (Filkova et al., 2014; Hall et al., 2011;
111 O’Sullivan et al., 2015). Broadly, the particle size distribution of the resultant powder is related
112 to the initial spray in terms of initial drop size. However, there is not necessarily a direct
113 relationship between these two parameters, for a variety of reasons such as particle deflation
114 or expansion and agglomeration, which are dependent on a combination of feed composition,
115 feed physicochemical properties and process conditions (Maa et al., 1997). Fig. 2b shows the
116 different powder morphologies that can be achieved from spray-drying operations, which are
118
120 Rotary wheel atomisers consist of a horizontal disc with or without radial vanes (or
121 grooves), which can be straight or curved (Fig. 3). This type of atomiser is driven by either
122 compressed air or an electrical motor. The liquid is fed into the atomiser centrally and then
123 flows radially outward towards the edge of the atomiser in the form of a thin film of liquid,
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124 which is dispersed into small individual droplets at the periphery of the wheel. The spray arises
125 from a centrifugal speed in the range 5,000 – 60,000 rpm (tip speeds from 100 to 200 m/s) and
126 forms a wide jet with an initially almost horizontal trajectory, which is referred to as a spray
127 cloud. To better control the dispersion properties, disc atomisers are often made with grooves
128 which allow the liquid feed to emerge with equal flow and pressure conditions in the form of
129 threads (Schröder and Walzel, 1998), leading to a more homogeneous spray, which elongate
130 on emerging from the periphery of the atomiser due to centrifugal acceleration and then
131 disintegrate into droplets. Moreover, this helps to optimise the drying of the droplets by
132 narrowing the droplet size distribution (Kamplade et al., 2014). The droplets produced are
133 spherical due to the influence of the imparted energy, the air turbulence effect, and the liquid
134 feed properties. Large rotary atomisers can handle flow rates of up to 200 ton/h.
135 The sprays resulting from rotary wheel atomisers are highly homogeneous. However,
136 several process factors will affect the spray characteristics and, thus, the quality of the spray-
137 dried product. Firstly, the design of the rotary wheel atomiser, in terms of the number of vanes
138 and their shapes (i.e., curved, circular, oval or rectangular), will influence the wheel capacity
139 and the droplet size and properties, respectively. For example, the use of curved vanes will give
140 rise to higher bulk density powders than those produced with straight vanes (Filkova et al.,
141 2014), due to the de-aeration of the feed liquid while travelling out through the curved vanes.
142 By controlling the flowrate of the liquid concentrate and the speed of the rotor, the
143 droplet size can be modulated. Indeed, use of a higher speed at constant wheel diameter and
144 feed flowrate can lead to smaller droplets, which are easier to dry due to increased rates of
145 evaporation (Baker, 1997). The tip speed of the atomiser is one of the most versatile processing
146 variables, from a practical point of view, as it is an established scale-up factor for a multitude
147 of processes (Hall et al., 2011). Overall, knowledge regarding the feed properties, as discussed
148 below (Section 4), is centrally important in predicting spray properties (Filkova et al., 2014).
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149
151 Pressure nozzle atomisers are composed of two internal features: (1) a device to create
152 turbulence within the nozzle head (swirl); and (2) an orifice (typically 0.4 to 4 mm in diameter)
153 through which the liquid feed is vertically discharged (Fig. 4). The liquid feed enters the nozzle
154 core tangentially with a decreasing diameter and leaves the orifice, under pressure, as a conical
156 As the spray cloud is much smaller than that for rotary wheel atomisers, it enables the
157 drying chamber to be taller and narrower, or alternatively, the use of more than one pressure
158 nozzle, with the latter allowing for increased drying capacity. The spray is created by the
159 conversion of the pressure energy applied to the liquid feed into kinetic energy as the liquid
160 passes through the nozzle aperture under pressure, usually in the range 180–220 bar
161 (Verdurmen et al., 2004). The size of the two components of the nozzle (i.e., the swirl chamber
162 and orifice), and the operating pressure, will determine the nozzle capacity and the droplet size
163 within the spray. The usual capacity of these nozzles is up to 400 L/h (Huang et al., 2006). If
164 higher feed flowrates are to be processed, several nozzles may be used in parallel in the drying
165 chamber.
166 The properties of the liquid feed and the imparted energy (i.e., pressure and kinetic
167 energies) will determine the properties of the spray and thus the droplets (size and span): the
168 higher the viscosity of the liquid feeds, the smaller the spray cone at the exit of the atomiser
169 (Chen et al., 1992), while the higher the pressure or the flowrate, the smaller the droplets
170 (Broniarz-Press et al., 2016) due to increased levels of energy density. Geometric parameters
171 also play an important role in determining the spray characteristics (Rizk and Lefebvre, 1987).
172 Rashad et al. (2016) showed that the spray angle and the Sauter mean diameter (𝐷3,2) of
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𝐷𝑠
173 droplets were influenced by the ratio of swirl chamber to discharge orifice diameters ( 𝐷0),
𝐿
174 the length to diameter ratio of the swirl chamber ( 𝑠 𝐷𝑠) and the length to diameter ratio of the
𝐿
175 discharge orifice ( 0 𝐷0) using water as the test liquid. Indeed, the spray cone angle decreased
𝐷𝑠
176 in a continuous manner when 𝐷0 increased, whereas an optimal value was determined in
𝐿0
177 the range of the studied conditions for 𝐷3,2. An increase of 𝐷0 led to an increase in 𝐷3,2
178 values, while the spray cone angle reached an optimum, associated with the size distribution
179 of the resultant spray of droplets (enhancement of the rate of heat and mass transfer). Finally,
𝐿𝑠
180 careful control of 𝐷𝑠 led to optima in the spray cone angle and 𝐷3,2 values, in both cases
182
184 Pneumatic nozzles, also known as two-fluid nozzles, consist of a tube with double entry
185 flows of air, vapour and/or liquid. The liquid feed can be mixed with the air inside or outside
186 the body of the nozzle (Fig. 5). With pneumatic nozzles, the liquid feed stream is broken into
187 droplets upon contact with a second fluid, which is usually compressed air or steam, and
188 normally gives rise to a spray pattern with an angle ranging from 20 to 60° (Filkova et al.,
189 2014). The spray arises from kinetic energy of air in the range of 1-3 kPa. The air flow brings
190 high frictional forces over liquid surfaces that create atomisation arising from the disintegration
191 of the liquid feed. Sarrate et al. (2015) showed that varying the liquid feed properties modified
192 the particle size and morphology after spray drying with a pneumatic nozzle; a low-viscosity
193 feed will result in low mean droplet size and a high homogeneity, whereas a high-viscosity
194 feed will give rise to a higher mean droplet size and lower homogeneity (Filkova et al., 2014).
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195 Indeed, viscosity and surface tension increase the amount of energy required to atomize the
196 spray, and an increase in either of these properties will typically increase the drop size.
197 These devices are highly flexible and enable manipulation of the drop diameter in the
198 spray by varying the gas:liquid ratio, and are consequently often employed within pilot-scale
199 spray drying systems. It is also possible to maintain the droplet size distribution when changing
200 the flow rate by adjusting the flow rate of the compressed air. The highest capacity of a
201 pneumatic nozzle is around 1,000 L/h. Three-fluid and four-fluid variants of these nozzles also
202 exist. The first is composed of two feeding atomising gases, each fed separately (Fig. 5), and
203 is able to atomise one kind of feed, while the second type of system allows the atomisation of
204 two distinct feeds. However, the latter two types are more likely to be used in the
205 pharmaceutical industry for both greater uniformity in droplet size and the capacity to
207
208 2.4. Critical assessment of rotary wheel, pressure nozzle and pneumatic nozzle atomisers
209 In order to precisely measure the droplet size and size distribution generated by a given
210 atomiser, a direct measuring technique should be used. Albrecht et al. (2013) proposed the use
211 of non-intrusive laser-based approaches, specifically laser Doppler and phase Doppler
212 measurement techniques for this purpose. The latter technique is based on the assumption that
213 droplets are spherical and allow the measurement of two parameters, i.e., the droplet size
214 distribution and the velocity at which the liquid feed is ejected from the atomiser. However,
215 this technique is not appropriate for rotary wheel atomisers due to the broad spray produced
216 using this type of atomiser. In this regard, several authors have developed alternative methods
217 based on imaging and allowing wide size distributions, with large and non-spherical droplets
218 to be measured in scattered spray systems (Glover et al., 1995; Zhou et al., 2015). Other
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219 mechanical or optical-based techniques can also be used (Dodge et al., 1987; Dodge, 1987;
220 Lee Black et al., 1996). Table 1 shows a comparison of the equations employed to determine
221 the D3,2 of the resultant spray, in addition to the principal advantages and disadvantages, for
223
225 There are numerous liquids which are challenging to atomise using the aforementioned
226 conventional atomiser configurations (i.e., rotary wheel, pressure nozzles and pneumatic
227 nozzles) and, to achieve atomisation of such liquids, novel approaches may be required. Such
228 liquids may be, for example, highly viscous, contain long-chain high molecular weight
229 macromolecules, which may yield a more cohesive fluid, or demonstrate highly non-
231 constant shear rate); such fluids may, rather than forming discrete droplets, form filaments.
232 Moreover, another desirable feature is the high degree of monodispersity achievable using
234 The most recent developments in this field of atomisation are focused upon ultrasonic
235 atomisation and high voltage-induced sprays, as well as single-drop drying studies (Chen,
236 2004; Fu et al., 2012; Sadek, Schuck, et al., 2015; Schutyser et al., 2012). However, it should
237 be noted that investigations of these atomisation approaches are limited predominately at this
238 time to fundamental research, rather than industrial implementation, owing primarily to issues
239 of scale, perceived complexity of the setup and the inherent complexity of liquid dairy systems,
241
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243 The effect of atomisation from ultrasonic waves was first reported by Wood and Loomis
244 in 1928, where the phenomenon was originally referred to as ultrasonic fogging, due to the
245 formation of mists and sprays of the liquids subjected to ultrasonic processors (Antonevich,
246 1959; Söllner, 1936; Wood and Loomis, 1928). Ultrasound involves generation of acoustic
247 longitudinal waves of higher frequency than the threshold of human auditory detection (≥ 16
248 kHz), which propagate through liquids in differing manners depending on the frequency (Soria
249 and Villamiel, 2010). Ultrasound can be categorised into two distinct types, based on the
251 (1) High-frequency (> 100 kHz), low-intensity (< 1 W/cm2) ultrasound, which is typically
252 used for the physicochemical evaluation of a range of microstructures, both food and
254 (2) Low-frequency (20 – 100 kHz), high-intensity (10 – 100 W/cm2) ultrasound, which is
255 often used for the alteration, development and generation of microstructures, again for
256 both food and non-food applications (O’Sullivan et al., 2017; O’Sullivan et al., 2018b).
258 electrically driven, with the latter being based on the piezoelectric effect within ultrasonic horns
259 (Rajan and Pandit, 2001). The generation of droplets by ultrasound is dependent upon both the
260 properties of the liquid and the operating conditions of the ultrasonic processor. The
261 physicochemical factors which primarily determine drop formation are the surface tension at
262 the gas-liquid boundary, bulk viscosity and liquid density (Bittner & Kissel, 1999; Briceño-
264 The processing variables which effect droplet size are feed rate of liquid to the nozzle
265 and acoustic intensity, which is dependent upon the specific probe (i.e., surface area) and both
266 the ultrasonic frequency and amplitude (Rajan and Pandit, 2001). In brief, smaller droplets can
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267 be achieved at lower flowrates to the nozzle, arising from increased residence times at the
268 atomiser surface, allowing for a greater exposure to acoustic energy. In addition, at higher
269 acoustic intensities, more energy is provided to the liquid, which manifests as production of
270 smaller droplets. Moreover, these effects can be combined to have a synergistic effect in
271 achieving small droplets with a narrow size distribution (O’Sullivan et al., 2017).
273 (Freitas et al., 2004; Rajan & Pandit, 2001). The key component of the setup is a device known
274 as a sonotrode, which has two main components, a transducer and a tip. The transducer converts
275 electrical energy into mechanical energy, which is achieved through use of piezoelectric
276 materials, such as quartz or lithium zirconate titanates, whereby these materials oscillate in
277 response to electrical energy, leading to mechanical vibrations. These mechanical vibrations
278 emanate from the tip of the sonotrode in the form of acoustic waves (Martini, 2013; O’Sullivan
279 et al., 2017). To achieve atomisation using this approach, the liquid is fed centrally to the tip
280 via a channel within the sonotrode itself, whereby it comes in direct contact with the tip, coating
281 it with a thin liquid film. The acoustic waves can then atomise the liquid into a spray of droplets
283 Practical applications of ultrasonic atomisation for spray drying within the food sector,
284 and more specifically within the dairy industry, have been limited, due to both the complex
285 makeup of liquid concentrates within the dairy sector and general equipment considerations
286 (i.e., comparatively high CapEx, energy utilisation, heat dissipation challenges, etc.).
287 Furthermore, this technology has been predominantly limited to laboratory-scale processing,
288 rather than pilot or industrial scales. Studies have been conducted investigating the
289 encapsulation efficiency of dried fish oil emulsions, stabilised by whey protein, prepared using
290 ultrasonic atomisation, and comparing this to other approaches; powders prepared utilising an
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292 comparison to pressure nozzles (either 1 or 2 channels), yet exhibited a narrower size
293 distribution in comparison to the other atomisation approaches investigated (Klaypradit and
295 One of the distinct advantages of ultrasonic nozzles in comparison to other atomisation
296 approaches is that a larger aperture can be used, which is invariably less prone to blockages
297 than the small orifices required for pressurised flow in nozzle atomisers. However, to the
298 authors’ knowledge, this approach is not used at an industrial scale within the dairy sector,
299 owing to the smaller size of powder particles from this approach, which adversely affect
300 rehydration properties, and general issues associated with processing, in terms of lower
301 throughput levels, heat generation and perceived complexity issues (Filkova et al., 2014; Rajan
303
306 atomisation, is a process which utilises electrical energy to disperse a liquid stream into a spray
307 of droplets. Droplets produced using this approach are highly charged, which enhances droplet
308 dispersion and prevents droplet coalescence (Jaworek, 2007). Furthermore, the spray of
309 droplets produced using this method demonstrates a high degree of monodispersity, and the
310 size of droplets can be precisely controlled through careful adjustment of the fluid flowrate
311 and/or the electrical conductivity of the liquid (Gañán-Calvo et al., 1997). Other factors which
312 affect drop formation through electronisation (i.e., high voltage-induction) are permittivity
313 (i.e., the measure of how an electric field affects a dielectric medium), density and rheological
314 properties of the liquid, tension at the gas-liquid surface, and charge density of the droplets
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316 In order to achieve an electrospray, high voltage is applied to the liquid using an
317 apparatus known as an emitter, whereby the liquid, upon reaching the emitter, will form a
318 Taylor cone (Fig. 7a), emitting a liquid jet through its apex (Meesters et al., 1992). A Taylor
319 cone is a cone of liquid from which liquid drops emanate above a given threshold voltage for
320 a given liquid, whereby the slightly rounded tip inverts and emits a spray of liquid. This is
321 referred to as a cone-jet, and is the beginning of the electrospray process, whereby a voltage
322 greater than the threshold voltage is necessary to achieve a stable cone-jet. The magnitude of
323 the threshold voltage is dependent predominately upon the properties (i.e., conductivity) of the
324 liquid, rather than the configuration of the nozzle (Yarin et al., 2001).
325 The configuration of an electrospray atomisation approach is depicted in Fig. 7b. The
326 setup consists of the liquid to be atomised, which is fed from a storage vessel to the emitter and
327 spray head using compressed air. The emitter is connected to a high voltage power supply,
328 which induces drop formation, and in many cases it is necessary to earth the resultant spray
330 Despite the capacity of these systems to convert a fluid stream into monodisperse liquid
331 droplets, to the best of the authors’ knowledge there are no examples of this technology being
332 employed for atomisation applications at laboratory, pilot or industrial scales within the dairy
333 sector. The reasons for this include (when compared to other atomisation approaches) the
334 limited throughput, the comparatively high complexity, and the limited number of fluids which
336 formulations incorporating several components (e.g., proteins, fats, carbohydrates, etc.), as
337 well as the challenging physical properties (e.g., non-Newtonian flow behaviour of fluids to be
338 atomised), which are commonly observed with dairy applications. Thus, the electrospray
339 atomisation approach is more commonly encountered in the production of ceramic powders,
340 aerosol standards and space thrusters (Gañán-Calvo et al., 1997; Jaworek, 2007). The few
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341 examples of electrospray technology employed for food applications are limited to that of
342 coating (e.g., aluminium coated with sunflower oil using 20 µm droplets to produce a
343 hydrophobic film), rather than for use in spray-drying systems, and, moreover, are quite limited
344 due to the aforementioned issues of scale and complexity of setup (Bhushani &
346
348 For the majority of industrial dairy spray-drying operations, the selection of a suitable
349 atomiser is typically a choice between rotary atomisers or pressure nozzles, as there is
350 comparatively limited use of the other nozzle systems presented earlier (i.e., pneumatic,
351 ultrasonic nozzles and electrospray) (Schuck et al., 2016). Pneumatic nozzles are typically used
352 in pilot-scale spray dryers or in some cases for lecithin-dosing systems in the manufacture of
353 instant powders and for coating or wet agglomeration of powders. Nevertheless, the criteria for
354 selecting a given atomisation technology is based on a variety of considerations, which include
355 CapEx, OpEx, availability, flexibility of application, and the target particle size distribution
356 (PSD) of the final powder product. Other key factor to consider in the selection of an atomiser
357 is the practical aspects of its use, such as the run times, capability for cleaning in place (CIP),
358 and safety considerations (e.g., fire and explosion regulations). These types of considerations
359 are critically important when determining the suitability of a given system, both in terms of the
360 initial investment and the associated payback times, and the inherent running costs, in terms of
361 both energy utilisation and maintenance. However, practical considerations around processing
362 must be considered to ensure a robust and flexible system, which is capable of atomising a
363 wide range of dairy liquid feed streams, and its overall plant usability.
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364 The predominant rationale for use of rotary wheel and pressure nozzle atomisers within
365 the dairy sector is that they are robust, reliable and well-established systems, and demonstrate
366 most of the aforementioned characteristics, in terms of capacity, ease of use, capability of CIP,
367 etc. On the other hand, for the alternative atomisation technologies, there is typically a higher
368 associated cost, and lack of familiarity, which in turn could potentially lead to capacity
369 constraints during powder manufacture. Thus, for these systems to be considered commercially
370 and industrially feasible by dairy processors, further research is required to assess their
372
374 Atomisation plays a critically important, integral role in the spray-drying process, and
375 thus its consistent operation is essential. Consequently, it is necessary to monitor the
376 atomisation operation through a variety of means to mitigate against production downtime and
377 also to facilitate optimal control of critical quality attributes of the finished product properties.
378 When considering methods that can be employed for monitoring the atomisation process, three
379 different approaches can broadly be employed: (1) characterisation of process properties (e.g.,
380 feed and air flowrate, air relative humidity, stream pressure, etc.) of streams entering and
381 exiting the spray dryer (Anderson, 2001), (2) control of parameters (e.g., air temperature)
382 within the spray dryer (Nath and Satpathy, 1998); and (3) use of computational fluid dynamics
383 (CFD) to gain a better understanding of material flow through the process (Fletcher et al.,
384 2006).
385
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387 Process variables of the inlet and outlet streams to a spray dryer can indicate whether
388 the process is performing as designed. One of the key processing parameters which is
390 of points in the system. This parameter should be maintained within specified ranges during
391 the drying process to ensure consistent product quality and maximise overall efficiency of the
392 drying process. Variations in pressure, either for inlet or outlet streams, give indications of
393 performance of a spray dryer system, in particular atomiser operation; for example, a spike in
394 pressure on the inlet to the dryer could indicate potential blockages within the system; pressure
395 sensors on the feed line could indicate a build-up in pressure due a blockage in the system (Fig.
396 1).
397 Inline viscosity measurement is another means of controlling the inlet liquid stream to
398 be atomised. The atomisation step requires droplets with high surface area:mass ratio (i.e.,
399 minimisation of droplet size), which can be achieved by variation of the pressure, which is
400 influenced by both the liquid feed viscosity and volumetric flowrate. Indeed, the droplet size
401 varies directly with the viscosity at a factor ranging between 0.17-0.25 (Masters, 2002). There
403 (1) Direct measurement through use of an inline viscometer, of which there are numerous
404 examples, such as the Couette type, whereby the main challenges associated with inline
405 viscometers are the response times for measurements for a given volume of fluid, and the ability
406 to measure viscosity within pressurised (150-250 bar) liquid feed lines to the spray-dryer.
407 (2) Indirect measurement of viscosity based on measurements of either the electrical current of
408 the concentrate pump or calculation of the theoretical viscosity from pressure drop data using
409 the Hagen-Poiseuille equation (O’Sullivan et al., 2017, 2018,). Schuck et al. (2005) proposed
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410 that the electrical current recorded from the feed pump could be used as a method to monitor
412 Electrical capacitance tomography (ECT) is a novel approach which demonstrates the
413 capacity for assessing the performance of drying processes in real-time, such as spray-drying,
414 fluidised beds and pneumatic conveying of powders (Jaworski & Dyakowski, 2001; Yang,
415 1996). The principles of ECT rely upon measurement of variations in the dielectric permittivity
416 distribution (i.e., a measure of resistance when forming an electric field in a given medium)
417 across a planar section of electrodes within a given process, whereby each electrode takes
418 measurements with respect to all other planar electrodes (Yang, 2010; Yang & Peng, 2003).
419 Variation in the dielectric permittivity from a given baseline (e.g., that of air) across a given
420 planar section indicate the presence of material passing through that section (Yang & Peng,
421 2003). Thus, for the case of spray drying, the measured material would be droplets produced
423 composite, proxy three-dimensional view within a given section of the process, which allows
424 for the tracking of a given droplet and provides a detailed understanding of both the mechanics
425 of motion (i.e., trajectory) and drying (i.e., change in dielectric permittivity as a function of
426 moisture loss on drying) for a given droplet. ECT has been successfully used to understand the
427 fluid mechanics with pneumatic conveying and circulating fluidised bed systems (Liu et al.,
429 One of the key considerations of these process control systems is their positioning in
430 the process with respect to the inlet to the spray dryer, and thus proximity to the atomiser nozzle
431 and the outlet. The further these sensors are from these points, the greater the response times
432 will be and, in addition, the more difficult it will be to assess the root cause of the problem.
433 Furthermore, in an ideal integrated system control, the inline sensors on the inlet feed would
434 work in parallel with some of the approaches discussed in the next section regarding monitoring
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435 systems within the dryer, whereby, if a fault were detected through use of a given sensor, the
436 specific reason could be corrected using integrated advanced process control (APC) systems.
437
439 There are generally two types of monitoring approaches which can be used for the
440 atomisation process within the spray-drier or chamber, i.e., (1) visual approaches, which are
441 relatively labour-intensive, and (2) automated approaches utilising data acquisition from within
443 Visual approaches that can be used to monitor the atomisation process within a spray
444 drying chamber include the use of sight glasses and/or closed circuit television (CCTV)
445 systems (Listiohadi et al., 2005). For best use, these are located near the top of the chamber in
446 view of the nozzles. However, both techniques are limited as sight glasses may foul during
447 drying operations and CCTV cannot trigger a corrective intervention (Fig. 1).
448 The infra-red (IR) camera adds an extra level of safety and process control through
449 temperature mapping within close proximity to the nozzle and electronic alarm points, and
450 actions can be triggered in advance of the development of processing challenges (e.g., a
451 blocked nozzle), thereby maintaining the quality of the product and reducing further the
452 possibility of overheating (Fig. 1). GEA Niro has developed a visual monitoring system for
453 spray dryers called the SprayEye. The SprayEye system links IR cameras to a pre-warning
454 system that detects high temperature increases in the powder within the spray dryer before one
455 would notice it using a normal camera. The SprayEye was first made of conventional digital
456 cameras to monitor the performance of spray nozzles. These cameras show a continuous picture
457 of the spray zone, allowing for the checking of leak occurrences or nozzle blockages.
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458 Therefore, the spray pattern of the nozzles into the drying chamber can be maintained at an
460 Automated approaches can be more accurate and user-friendly than visual systems;
461 however, they are normally associated with higher cost, in terms of CapEx, which play a key
462 role when determining procurement of a specific dryer configuration and associated control
464
467 information in terms of both material and energy flow through a given process, and over the
468 past decade has garnered particular interest as a means to transition to an in silico (i.e., studies
469 conducted solely through use of computers) methodology for process development. For the
470 specific application of spray drying, CFD can be used to understand the heat distribution within
471 a dryer, the material flow through the atomiser, and identify where potential issues could arise,
472 such as dead-zones in terms of both airflow and temperature (Fig. 8) (Fletcher et al., 2006).
473 Jaskulski et al., (2015) developed a three-dimensional (3D) CFD model of the agglomeration
474 of droplets and particles in a counter-current spray-drying process. Their model takes into
475 account droplet coalescence and shrinkage and the hydrodynamic segregation of particles in
476 order to accurately calculate the mass balance of the discrete phase. Two agglomeration areas
477 were observed in the chamber; the first comprised of wet particle agglomeration in the
478 atomization zone, while the second involved dry agglomeration above the air inlets, due to the
479 intensive mixing of particle streams. The elaborated model also allows prediction of the final
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481 Despite this technique providing significant information about the process, there are
482 several limitations, which include the high computer processing power required to run
483 simulations, the time-consuming nature of these runs, taking in some cases several weeks, and
484 the necessity for both highly experienced CFD modellers to develop representative simulations
485 and developed mathematical models that accurately reflect physicochemical and biochemical
486 processes. For the specific case of the monitoring of atomisation, CFD cannot be used as a
487 standalone technique, but rather provide information as to where issues could arise, and assist
489
491 Aside from the aforementioned process conditions, which can be varied, depending
492 upon the specific nozzle, other factors can affect atomisation. Broadly, these can be categorised
493 as (1) process parameters for the inlet stream to the dryer, and (2) the feed composition.
494 Variation in these will alter how the atomiser performs and, thus, the physical properties (e.g.,
496
498 As discussed in Section 3.1, there are several process parameters which affect
499 atomisation and can provide information regarding the process during a given production cycle.
500 The two main process parameters of interest are temperature in general terms and feed flow-
501 rate, as these will both alter the physical properties of the liquid stream to the atomiser to
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503 For the production of dairy powders, typical preheating temperatures for the feed are
504 ~75-85°C, which have the effect of reducing concentrate viscosity (Gharsallaoui et al., 2007).
505 The temperature of the inlet stream may also need to be maintained below a certain level,
506 depending on the product, as certain dairy solutions are prone to thermal aggregation (e.g.,
507 heat-induced whey protein aggregation), which could result in blockages. These include whey-
508 protein-dominant systems, whereby thermal denaturation of the protein occurs at temperatures
509 in excess of 68oC (Damodaran, 1997). However, denaturation in these systems is not an
510 instantaneous process (Moakes et al., 2015), allowing for sufficient time for evaporation
511 operations to increase the solids content of the inlet stream, to maximise efficiency of the
512 dryer, and the drying itself within the spray drying chamber, leading to minimal whey protein
514 The feed flow rate is considered to be the primary parameter to adjust in order to balance
515 the throughput and the optimal drying of a liquid concentrate considering the drying capacity
516 of the respective spray dryer set-up (Miller and Gil, 2012). The feed flowrate governs the
517 drying history of the feed by influencing the residence time of a particle according to the
518 relative humidity and the outlet air temperature (Paudel et al., 2013). In this regard, the feed
519 flow rate for a given solution is fixed to enable sufficient drying of the particles before they
520 make contact with the spray dryer wall, and is additionally related to other factors such as
521 atomiser type, dryer chamber geometry, etc (Vehring et al., 2007). It has also been shown that,
522 for the case of drying of mannitol solutions, the product was almost completely dried in the
523 upper part of the chamber at low feed flow rates, whereas the breaking strength (the greatest
524 stress that a material is capable of withstanding without rupture) was decreased at low rates
526
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529 The specific formulation of different components within a feed stream has a significant
530 effect on the performance of the atomiser. The four main components within dairy-based
531 products which play a role in drying are protein, fat, carbohydrate (i.e., lactose) and water. The
532 properties of the particles resulting from atomisation are strongly dependent on the respective
533 intrinsic material properties of each component. For example, Elversson & Millqvist-Fureby,
534 (2005) showed that atomisation of amorphous or crystalline carbohydrates leads to hollow or
535 porous particles, respectively. Furthermore, the presence of high concentrations of lactose
536 within an inlet stream to the dryer can potentially result in the blockage of nozzles due to large
537 lactose crystals. Surface activity and mechanical properties of components are also known to
538 affect particle geometry and morphology (Kawakami et al., 2010; Sadek et al., 2013).
539 Drying of a whey protein isolate (WPI) droplet leads to a smooth semi-spherical particle
540 shape, whereas drying of a native phosphocaseinate droplet results in a twisted and wrinkled
541 particle without fractures (Sadek et al., 2015a). Surface activity of the components of the feed
542 also influence their distribution into the particle during the drying process (i.e., migration of
543 certain components from the core to the surface of the droplet/powder particle), resulting in
544 differences between the particle surface and bulk concentrations (Briggs, 1994; Kim et al.,
545 2006). Both protein and fat accumulate at the particle surface during spraying and drying,
546 whereas lactose content is reported to be enriched in the core of the particle (Drapala et al.,
547 2017; Kelly et al., 2015; Nijdam and Langrish, 2006). As a further example, whole milk
548 powder (WMP) particles are mainly covered with fat followed by lactose and then protein,
549 whereas particles in SMP are mainly covered with proteins, with interstitial lactose crystals
550 (Murrieta-Pazos et al., 2012). Furthermore, the type of product being processed will strongly
551 influence the moisture content, and thus the efficiency of the dryer, as the ability of components
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552 to bind to water governs the drying kinetics and thus influences particle characteristics (Ameri
554
556 The concentration and viscosity of the feed are known to affect the geometric mean
557 diameter of spray-dried particles. Viscous concentrated solutions induce large droplets, that
558 form larger powder particles (Elversson and Millqvist-Fureby, 2005; Walton and Mumford,
559 1999) due to increasing breakup length of the liquid jets during atomisation. In addition, the
560 feed concentration may affect the solvent removal (Paudel et al., 2013), which is water in the
561 case of dairy products. The rate of evaporation from the droplet surface decreases with
562 increasing feed viscosity, due to higher fraction and/or molecular weight of polymers present
564
566 While several of the aforementioned atomisation technologies are well established and
567 have been in active industrial use for over a century, numerous advances have been made in
568 recent decades in understanding the fundamentals responsible for the generation of a spray of
569 discrete droplets from a bulk liquid stream and the factors associated with their formation, such
571 Many technological approaches are capable of achieving atomisation, such as rotary
572 wheel atomisers, pressure nozzles, pneumatic nozzles and ultrasonic nozzles, and there are
573 benefits and limitations associated with each, which will influence their selection in an
574 industrial setting, broadly categorised in terms of the functionality (i.e., efficient droplet
575 formation) and cost considerations (i.e., CapEx and OpEx) of a given atomiser.
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576 Given that atomisation plays a central role in spray drying, continual monitoring of the
577 system is of paramount importance. This monitoring may be achieved using a number of
578 different approaches, such as inline characterisation of the process streams, or direct
579 observation of the nozzle, where these approaches are, at times, used in conjunction with CFD
580 modelling of the process to highlight potential challenges during operation. In addition to
581 monitoring of the process, a detailed understanding of the properties of the material to be dried
582 is essential, as these will affect atomisation. Such properties include rheological flow
583 behaviour, and the potential for concentrated dairy streams at elevated temperatures to undergo
584 protein denaturation, or possess lactose crystals, depending on the specific formulation and
586 Although numerous advances have been made in understanding the droplet formation
587 and spray behaviour mechanisms of a variety of atomisation technologies, this understanding
588 is predominately at a laboratory scale. Although studies are being conducted at pilot-scale,
589 further work is required to fully understand the relationship between nozzle selection, design
590 criteria, process parameters and product formulation to allow for the effective utilisation of
591 atomisation technologies in a variety of product categories within the dairy sector.
592 Furthermore, greater investigation of novel atomiser designs could allow for unique powder
594
595
596
597 Acknowledgements
598 The authors would like to acknowledge the Dairy Processing Technology Centre
599 (DPTC), an Enterprise Ireland initiative, for financial support and permission to publish this
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600 work. This work was supported by the Irish State through funding from the Technology Centres
602 References
603 Albrecht, H.-E., Damaschke, N., Borys, M., Tropea, C., 2013. Laser Doppler and Phase
605 Ameri, M., Maa, Y.-F., 2006. Spray Drying of Biopharmaceuticals: Stability and Process
607 https://doi.org/10.1080/03602550600685275
608 Anderson, N.G., 2001. Practical Use of Continuous Processing in Developing and Scaling Up
610 https://doi.org/10.1021/op0100605
611 Antonevich, J.N., 1959. Ultrasonic Atomization of Liquids. Trans. IRE Prof. Gr. Ultrason.
613 Anu Bhushani, J., Anandharamakrishnan, C., 2014. Electrospinning and electrospraying
614 techniques: Potential food based applications. Trends Food Sci. Technol. 38, 21–33.
615 https://doi.org/10.1016/j.tifs.2014.03.004
616 Avvaru, B., Patil, M.N., Gogate, P.R., Pandit, A.B., 2006. Ultrasonic atomization: Effect of
618 https://doi.org/10.1016/j.ultras.2005.09.003
619 Baker, C.G.J., 1997. Industrial Drying of Foods. Springer Science & Business Media.
620 Bittner, B., Kissel, T., 1999. Ultrasonic atomization for spray drying: a versatile technique for
624 Zanelli-Iglesias, C., 2015. On the Ultrasonic Atomization of Liquids. Phys. Procedia 63,
27
ACCEPTED MANUSCRIPT
626 Broadhead, J., Edmond Rouan, S.K., Rhodes, C.T., 1992. The spray drying of
628 https://doi.org/10.3109/03639049209046327
629 Broniarz-Press, L., Włodarczak, S., Matuszak, M., Ochowiak, M., Idziak, R., Sobiech, Ł.,
630 Szulc, T., Skrzypczak, G., 2016. The effect of orifice shape and the injection pressure on
631 enhancement of the atomization process for pressure-swirl atomizers. Crop Prot. 82, 65–
633 Chen, S.K., Lefebvre, A.H., Rollbuhler, J., 1992. Factors Influencing the Effective Spray
634 Cone Angle of Pressure-Swirl Atomizers. J. Eng. Gas Turbines Power 114, 97–103.
635 https://doi.org/10.1115/1.2906313
636 Chen, X.D., 2004. Heat-Mass Transfer and Structure Formation During Drying of Single
638 Crowley, S. V., Desautel, B., Gazi, I., Kelly, A.L., Huppertz, T., O’Mahony, J.A., 2015.
639 Rehydration characteristics of milk protein concentrate powders. J. Food Eng. 149, 105–
641 Damodaran, S., 1997. Food proteins: an overview, in: Damodaran, S., Paraf, A. (Eds.), Food
642 Proteins and Their Applications. Marcel Dekker, New York, pp. 1–24.
643 Dodge, L.G., 1987. Comparison of performance of drop-sizing instruments. Appl. Opt. 26,
645 Dodge, L.G., Rhodes, D.J., Reitz, R.D., 1987. Drop-size measurement techniques for sprays:
646 comparison of Malvern laser-diffraction and Aerometrics phase/Doppler. Appl. Opt. 26,
647 2144–2154.
648 Drapala, K.P., Auty, M.A.E., Mulvihill, D.M., O’Mahony, J.A., 2017. Influence of emulsifier
649 type on the spray-drying properties of model infant formula emulsions. Food Hydrocoll.
28
ACCEPTED MANUSCRIPT
651 Elversson, J., Millqvist-Fureby, A., 2005. Particle size and density in spray drying-effects of
654 Filkova, I., Huang, L.X., Mujumdar, A.S., 2014. Industrial Spray Drying Systems, in:
656 Fitzpatrick, J.J., Barry, K., Cerqueira, P.S.M., Iqbal, T., O’Neill, J., Roos, Y.H., 2007. Effect
657 of composition and storage conditions on the flowability of dairy powders. Int. Dairy J.
659 Fletcher, D.F., Guo, B., Harvie, D.J.E., Langrish, T.A.G., Nijdam, J.J., Williams, J., 2006.
660 What is important in the simulation of spray dryer performance and how do current CFD
662 https://doi.org/10.1016/j.apm.2006.03.006
663 Forny, L., Marabi, A., Palzer, S., 2011. Wetting, disintegration and dissolution of
665 https://doi.org/10.1016/j.powtec.2010.07.022
666 Freitas, S., Merkle, H.P., Gander, B., 2004. Ultrasonic atomisation into reduced pressure
669 Fu, N., Woo, M.W., Chen, X.D., 2012. Single Droplet Drying Technique to Study Drying
670 Kinetics Measurement and Particle Functionality: A Review. Dry. Technol. 30, 1771–
671 1785.
672 Gañán-Calvo, A.M., Dávila, J., Barrero, A., 1997. Current and droplet size in the
674 https://doi.org/10.1016/S0021-8502(96)00433-8
29
ACCEPTED MANUSCRIPT
675 Gharsallaoui, A., Roudaut, G., Chambin, O., Voilley, A., Saurel, R., 2007. Applications of
676 spray-drying in microencapsulation of food ingredients: An overview. Food Res. Int. 40,
678 Gibbs, B., Kermasha, S., Alli, I., Mulligan, C., 2009. Encapsulation in the food industry: a
680 Glover, A.R., Skippon, S.M., Boyle, R.D., 1995. Interferometric laser imaging for droplet
681 sizing: a method for droplet-size measurement in sparse spray systems. Appl. Opt. 34,
683 Hall, S., Cooke, M., El-Hamouz, A., Kowalski, A.J., 2011. Droplet break-up by in-line
685 Hanley, K.J., Byrne, E.P., Cronin, K., Oliveira, J.C., O’Mahony, J.A., Fenelon, M.A., 2011a.
688 Hanley, K.J., Cronin, K., O’Sullivan, C., Fenelon, M.A., O’Mahony, J.A., Byrne, E.P.,
691 Haque, M., 2015. Study on denaturation of whey protein isolate and its control in convective
693 Huang, L.X., Kumar, K., Mujumdar, A.S., 2006. A comparative study of a spray dryer with
694 rotary disc atomizer and pressure nozzle using computational fluid dynamic simulations.
696 https://doi.org/10.1016/j.cep.2005.11.004
697 Jaskulski, M., Wawrzyniak, P., Zbiciński, I., 2015. CFD Model of Particle Agglomeration in
699 https://doi.org/10.1080/07373937.2015.1081605
30
ACCEPTED MANUSCRIPT
700 Jaworek, A., 2007. Micro- and nanoparticle production by electrospraying. Powder Technol.
702 Jaworski, A.J., Dyakowski, T., 2001. Application of electrical capacitance tomography for
705 Ju, J., Yamagata, Y., Ohmori, H., Higuchi, T., 2008. High-frequency surface acoustic wave
707 https://doi.org/10.1016/j.sna.2008.01.001
708 Kamplade, J., Mack, T., Küsters, A., Walzel, P., 2014. Break-Up of Threads From Laminar
710 https://doi.org/10.1115/FEDSM2014-21243
711 Kawakami, K., Sumitani, C., Yoshihashi, Y., Yonemochi, E., Terada, K., 2010. Investigation
714 https://doi.org/10.1016/j.ijpharm.2010.02.018
715 Kelly, G.M., O’Mahony, J.A., Kelly, A.L., Huppertz, T., Kennedy, D., O’Callaghan, D.J.,
717 properties of spray-dried milk protein concentrate powders. Int. Dairy J. 51, 34–40.
718 https://doi.org/10.1016/j.idairyj.2015.07.001
719 Khan, M.K.I., Schutyser, M.A.I., Schroën, K., Boom, R., 2012. The potential of
720 electrospraying for hydrophobic film coating on foods. J. Food Eng. 108, 410–416.
721 https://doi.org/10.1016/j.jfoodeng.2011.09.005
722 Kim, E.H.-J., Chen, X.D., Pearce, D., 2002. Surface characterization of four industrial spray-
723 dried dairy powders in relation to chemical composition, structure and wetting property.
31
ACCEPTED MANUSCRIPT
725 Klaypradit, W., Huang, Y.-W., 2008. Fish oil encapsulation with chitosan using ultrasonic
727 https://doi.org/10.1016/j.lwt.2007.06.014
728 Lee Black, D., McQuay, M.Q., Bonin, M.P., 1996. Laser-based techniques for particle-size
729 measurement: A review of sizing methods and their industrial applications. Prog. Energy
731 Legako, J., Dunford, N.T., 2010. Effect of Spray Nozzle Design on Fish Oil-Whey Protein
733 3841.2010.01708.x
734 Listiohadi, Y.D., Hourigan, J.A., Sleigh, R.W., Steele, R.J., 2005. An exploration of the
735 caking of lactose in whey and skim milk powders. Aust. J. Dairy Technol. 60, 207–213.
736 Littringer, E.M., Mescher, A., Eckhard, S., Schröttner, H., Langes, C., Fries, M., Griesser, U.,
737 Walzel, P., Urbanetz, N.A., 2012. Spray Drying of Mannitol as a Drug Carrier—The
738 Impact of Process Parameters on Product Properties. Dry. Technol. 30, 114–124.
739 https://doi.org/10.1080/07373937.2011.620726
740 Liu, S., Chen, Q., Wang, H.G., Jiang, F., Ismail, I., Yang, W.Q., 2005. Electrical capacitance
741 tomography for gas–solids flow measurement for circulating fluidized beds. Flow Meas.
743 Maa, Y.-F., Costantino, H.R., Nguyen, P.-A., Hsu, C.C., 1997. The Effect of Operating and
746 Marshall, W.R., 1954. Atomization and spray drying. American Institute of Chemical
747 Engineers.
748 Martini, S., 2013. Sonocrystallization of Fats, 1st ed. Springer US, New York.
749 McClements, D.J., 1995. Advances in the application of ultrasound in food analysis and
32
ACCEPTED MANUSCRIPT
751 2244(00)89139-6
752 Meesters, G.M.H., Vercoulen, P.H.W., Marijnissen, J.C.M., Scarlett, B., 1992. Generation of
753 micron-sized droplets from the Taylor cone. J. Aerosol Sci. 23, 37–49.
754 https://doi.org/10.1016/0021-8502(92)90316-N
755 Miller, D.A., Gil, M., 2012. Spray-Drying Technology, in: III, R.O.W., Watts, A.B., Miller,
756 D.A. (Eds.), Formulating Poorly Water Soluble Drugs, AAPS Advances in the
758 Moakes, R.J.A., Sullo, A., Norton, I.T., 2015. Preparation and characterisation of whey
759 protein fluid gels: The effects of shear and thermal history. Food Hydrocoll. 45, 227–
761 Muir, D.D., 1996. The shelf-life of dairy products: 1. Factors influencing raw milk and fresh
763 0307.1996.tb02616.x
764 Murrieta-Pazos, I., Gaiani, C., Galet, L., Scher, J., 2012. Composition gradient from surface
765 to core in dairy powders: Agglomeration effect. Food Hydrocoll. 26, 149–158.
766 https://doi.org/10.1016/j.foodhyd.2011.05.003
767 Nath, S., Satpathy, G.R., 1998. A systematic approach for investigation of spray drying
769 Nijdam, J.J., Langrish, T.A.G., 2006. The effect of surface composition on the functional
771 https://doi.org/10.1016/j.jfoodeng.2005.08.020
772 O’Callaghan, D., Cunningham, P., 2005. Modern process control techniques in the
774 https://doi.org/10.1051/lait:2005021
33
ACCEPTED MANUSCRIPT
775 O’Connell, J.E., Flynn, C., 2007. The manufacture and application of casein-derived
776 ingredients, in: Hui, Y.H. (Ed.), Handbook of Food Products Manufacturing. John Wiley
778 O’Sullivan, J., Murray, B., Flynn, C., Norton, I., 2015. Comparison of batch and continuous
780 O’Sullivan, J., Park, M., Beevers, J., Greenwood, R., Norton, I., 2017. Applications of
781 ultrasound for the functional modification of proteins and nanoemulsion formation: A
783 O’Sullivan, J.J., Drapala, K.P., Kelly, A.L., O’Mahony, J.A., 2018a. The use of inline high-
784 shear rotor-stator mixing for preparation of high-solids milk protein-stabilised oil-in-
785 water emulsions with different protein:fat ratios. J. Food Eng. 222, 218–225.
786 O’Sullivan, J.J., Espinoza, C.J.U., Mihailova, O., Alberini, F., 2018b. Characterisation of
787 flow behaviour and velocity induced by ultrasound using particle image velocimetry
788 (PIV): Effect of fluid rheology, acoustic intensity and transducer tip size. Ultrason.
790 O’Sullivan, J.J., O’Mahony, J.A., 2016. Food Ingredients, in: Reference Module in Food
792 O’Sullivan, J.J., Schmidmeier, C., Drapala, K.P., O’Mahony, J.A., Kelly, A.L., 2017.
793 Monitoring of pilot-scale induction processes for dairy powders using inline and offline
795 Palzar, S., Dubois, C., Gianfrancesco, A., 2012. Generation of Product Structures During
797 Patel, R.P., Patel, M.P., Suthar, A.M., 2009. Spray Drying Technology: an overview. Indian
799 Paudel, A., Worku, Z.A., Meeus, J., Guns, S., Van den Mooter, G., 2013. Manufacturing of
34
ACCEPTED MANUSCRIPT
800 solid dispersions of poorly water soluble drugs by spray drying: Formulation and
801 process considerations. Int. J. Pharm., Poorly Soluble Drugs 453, 253–284.
802 https://doi.org/10.1016/j.ijpharm.2012.07.015
803 Percy, S., 1872. Improvement in drying and concentrating liquid substances by atomizing.
804 US125406.
805 Pisecky, J., 2012. Handbook of Milk Powder Manufacture. GEA Niro, Copenhagen.
806 Rajan, R., Pandit, A.B., 2001. Correlations to predict droplet size in ultrasonic atomisation.
808 Rashad, M., Yong, H., Zekun, Z., 2016. Effect of geometric parameters on spray
809 characteristics of pressure swirl atomizers. Int. J. Hydrogen Energy, 4th International
812 https://doi.org/10.1016/j.ijhydene.2016.04.037
813 Rizk, N.K., Lefebvre, A.H., 1987. Prediction of Velocity Coefficient and Spray Cone Angle
814 for Simplex Swirl Atomizers. Int. J. Turbo Jet Engines 4, 65–74.
815 https://doi.org/10.1515/TJJ.1987.4.1-2.65
816 Roos, Y.H., 2002. Importance of glass transition and water activity to spray drying and
818 Sadek, C., Pauchard, L., Schuck, P., Fallourd, Y., Pradeau, N., Le Floch-Fouéré, C., Jeantet,
819 R., 2015a. Mechanical properties of milk protein skin layers after drying: Understanding
820 the mechanisms of particle formation from whey protein isolate and native
822 https://doi.org/10.1016/j.foodhyd.2015.01.014
823 Sadek, C., Schuck, P., Fallourd, Y., Pradeau, N., Le Floch-Fouéré, C., Jeantet, R., 2015b.
35
ACCEPTED MANUSCRIPT
826 Sadek, C., Tabuteau, H., Schuck, P., Fallourd, Y., Pradeau, N., Le Floch-Fouéré, C., Jeantet,
827 R., 2013. Shape, Shell, and Vacuole Formation during the Drying of a Single
829 https://doi.org/10.1021/la404108v
830 Sarrate, R., Ticó, J.R., Miñarro, M., Carrillo, C., Fàbregas, A., García-Montoya, E., Pérez-
831 Lozano, P., Suñé-Negre, J.M., 2015. Modification of the morphology and particle size of
832 pharmaceutical excipients by spray drying technique. Powder Technol. 270, Part, 244–
834 Schröder, T., Walzel, P., 1998. Design of Laminar Operating Rotary Atomizers under
835 Consideration of the Detachment Geometry. Chem. Eng. Technol. 21, 349–354.
836 https://doi.org/10.1002/(SICI)1521-4125(199804)21:4<349::AID-CEAT349>3.0.CO;2-
837 9
838 Schuck, P., Jeantet, R., Bhandari, B., Chen, X.D., Perrone, Í.T., de Carvalho, A.F., Fenelon,
839 M., Kelly, P., 2016. Recent advances in spray drying relevant to the dairy industry: A
841 https://doi.org/10.1080/07373937.2016.1233114
842 Schuck, P., Méjean, S., Dolivet, A., Beaucher, E., Famelart, M.-H., 2005. Pump amperage: a
843 new method for monitoring viscosity of dairy concentrates before spray drying. Lait 85,
845 Schutyser, M.A.I., Perdana, J., Boom, R.M., 2012. Single droplet drying for optimal spray
846 drying of enzymes and probiotics. Trends Food Sci. Technol. 27, 73–82.
847 Söllner, K., 1936. The mechanism of the formation of fogs by ultrasonic waves. Trans.
849 Soria, A.C., Villamiel, M., 2010. Effect of ultrasound on the technological properties and
36
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850 bioactivity of food: a review. Trends Food Sci. Technol. 21, 323–331.
851 https://doi.org/http://dx.doi.org/10.1016/j.tifs.2010.04.003
852 Tang, K., Gomez, A., 1996. Monodisperse Electrosprays of Low Electric Conductivity
853 Liquids in the Cone-Jet Mode. J. Colloid Interface Sci. 184, 500–511.
854 https://doi.org/10.1006/jcis.1996.0645
855 Vehring, R., Foss, W.R., Lechuga-Ballesteros, D., 2007. Particle formation in spray drying. J.
857 Verdurmen, R.E.M., Menn, P., Ritzert, J., Blei, S., Nhumaio, G.C.S., Sonne Sørensen, T.,
858 Gunsing, M., Straatsma, J., Verschueren, M., Sibeijn, M., Schulte, G., Fritsching, U.,
859 Bauckhage, K., Tropea, C., Sommerfeld, M., Watkins, A.P., Yule, A.J., Schønfeldt, H.,
862 Walton, D.E., Mumford, C.J., 1999. The Morphology of Spray-Dried Particles: The Effect of
863 Process Variables upon the Morphology of Spray-Dried Particles. Chem. Eng. Res. Des.
865 Wood, W.R., Loomis, A.L., 1928. The physical and biological effects of high-frequency
867 https://doi.org/10.1016/S0016-0032(28)92379-0
868 Wu, J.X., Yang, M., Berg, F. van den, Pajander, J., Rades, T., Rantanen, J., 2011. Influence
869 of solvent evaporation rate and formulation factors on solid dispersion physical stability.
871 Yang, W., 2010. Design of electrical capacitance tomography sensors. Meas. Sci. Technol.
873 Yang, W.Q., 1996. Hardware design of electrical capacitance tomography systems. Meas.
37
ACCEPTED MANUSCRIPT
875 Yang, W.Q., Peng, L., 2003. Image reconstruction algorithms for electrical capacitance
877 0233/14/1/201
878 Yarin, A.L., Koombhongse, S., Reneker, D.H., 2001. Taylor cone and jetting from liquid
880 https://doi.org/10.1063/1.1408260
881 Zhou, W., Hu, J., Feng, M., Yang, B., Cai, X., 2015. Study on imaging method for measuring
883 https://doi.org/10.1016/j.partic.2014.12.003
884 Zhu, K., Madhusudana Rao, S., Wang, C.-H., Sundaresan, S., 2003. Electrical capacitance
887
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1 Figure captions
2 Fig. 1. Overview of the spray-drying unit operation and its associated process control systems
4 Fig. 2. (a) Factors effecting powder manufacture for spray drying applications, including
5 properties of the inlet stream, atomisation conditions, and process parameters associated with
6 the drying air, and (b) potential powder morphologies yielded from spray-drying.
7 Fig. 3. Rotary atomizing wheels with (A) straight radial vanes, (B) curved vanes and (C)
9 Fig. 4. Design of a pressure nozzle with (A) a grooved core and (B) a swirl chamber (Pisecky,
11 Fig. 5. Pneumatic nozzle with (a) internal air / liquid mixing and (b) external mixing (Pisecky,
13 Fig. 6. A detailed schematic of an ultrasonic atomiser (Freitas et al. (2004), reproduced with
15 Fig. 7. (a) Photograph of a liquid cone and (b) depiction of setup for electrospray atomisation.
16 Images taken from (Meesters et al., 1992) and (Gañán-Calvo et al., 1997), reproduced with
18 Fig. 8. Computational fluid dynamics (CFD) simulations of (a) trajectory of flow from the
19 atomiser, and (b) swirling flow within the spray dryer main chamber. Images taken from
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21 Figures
22 Fig. 1.
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25 Fig. 2.
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28 Fig. 3.
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31 Fig. 4.
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34 Fig. 5.
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37 Fig. 6.
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Highlights
2 Table 1. Comparison of the equations used for the determination of Sauter mean diameter, and advantages, and disadvantages for use of rotary,
- variation of the liquid flow rate without - production of wall deposits arising
having consequences on the droplet size from broad spray (Huang et al., 2006),
𝑚1 0.6 𝑏.𝜇.𝑁 0.2 𝜎.𝜌.𝑏3.𝑁 3 0.1
𝑣 𝑣 thus requiring wider body drying
0.4.( ) .( ) .( ) .𝑟 - simple droplet size control (wheel
2 𝑚1 2 chambers
𝑏.𝜌.𝑁.𝑟 .𝑁𝑣 𝑚1 revolution speed)
- not recommended for the drying of high
- can operate at high liquid feed viscosity
added value products such as protein
where 𝑚 (kg/s) is mass feed rate; 𝑁 (rps) is - can handle a high capacity isolate powders (too much waste)
rotational speed; 𝑟 (m) is wheel diameter; 𝑏 (m) is
- suitable for liquids that contain - the diameter of the chamber is a
Rotary vane height; 𝑁𝑣 is number of vanes; 𝜌 (kg/m3) is limiting factor when different powder
abrasive solids
atomisers fluid density; 𝜎 (N/m) is fluid surface tension and 𝜇 particle sizes are needed
(P.s) is fluid viscosity - the use of curved vanes can help to
reduce air incorporation (Hui, 2008) - incorporation of air into the droplets
due to air aspiration by the rotating
- reduction of wall deposit using wheel, resulting in high levels of
suitable system composed of a short occluded air in the final powder particles
chamber with a large diameter (i.e.,
newer generation wide-body spray- - air incorporation leads to modified
dryer configurations); this allows the properties of the final powder, such as a
particles to dry in a horizontal direction lower powder density and higher powder
before making contact with the walls volume
- amount of occluded air depending on
the feed properties (high protein contents
will lead to a stronger effect due to the
well-established good surface activity of
dairy protein)
- suitable for the drying of viscous, thick - highest energy consumption of all three
1.5
and/or abrasive liquid feed products devices due to the cost of compressed
𝜎 𝜇 0.45 𝑉𝑓
air/steam
585000· + 597[ ] ·[1000· ] - two-fluid nozzles are mainly used in
𝑣𝑟𝑒𝑙· 𝜌 𝜎·𝜌 𝑉𝑎𝑖𝑟
pilot-scale spray-dryers due to - production of fine particles
Pneumatic limitations of pressure nozzle or wheel
- may need extra air supply
atomisers atomizers at this scale
where 𝜎 (N/m) is fluid surface tension; 𝜌 (kg/m3) is
density; 𝜇 (Pa.s) is viscosity; 𝑣𝑟𝑒𝑙 (m/s) is relative
velocity; and 𝑉𝑓 and 𝑉𝑎𝑖𝑟 (m3/s) are volumetric flow
rate of the fluid and air, respectively