Journal of Cleaner Production 370 (2022) 133602

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Journal of Cleaner Production

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Ultrahigh water-retention cellulose hydrogels as soil amendments for early

seed germination under harsh conditions
Cong-Cong Qin a, Somia Yassin Hussain Abdalkarim a, *, Ying Zhou a, Hou-Yong Yu a, **, Xia He b
a
The Key Laboratory of Advanced Textile Materials and Manufacturing Technology of Ministry of Education, Zhejiang Sci-Tech University, Hangzhou, 310018, China
b
School of Art and Design, Zhejiang Sci-Tech University, Hangzhou, 310018, China

A R T I C L E I N F O A B S T R A C T

Handling Editor: M.T. Moreira Agricultural lands are greatly affected by climate change, harsh soils, and desertification, which negatively
impact the future sustainability of crop production. This work proposes a new strategy based on cellulose-
Keywords: inspired hydrogel (Gel-glycerol) as soil modulates to transform harsh soil into arable soil to promote seed
Wood pulps germination and growth. Gel-glycerol with a 3D network structure exhibited good rheological properties, high
Zinc chlorides
thermal stability, thermal reversibility (− 81.3 ◦ C), and ultrahigh water-retention capacity (160%) for enhancing
Hydrogels
seeds germination. Compared with the control sample, the germination percentage and the average leaves
Soils
Water retentions number of wheat plants increased by 21.88% and 100% after 21, days with Gel-glycerol. Associated with the
Seedings growth most common water-retaining agents (potassium polyacrylate, KPAM), the germination percentage of lettuce
seeds for 16 days increased by 38% and 22% with Gel-glycerol treatment under harsh soils. Moreover, the water
uptake value of wheat plants with Gel-glycerol improved by 94.7%. This result confirmed that adding Gel-
Glycerol as an amendment can significantly tailor soil salt content. This finding offers excellent applicability
in the agriculture ecosystem, displaying the potential value in soil amendments and an alternate solution for
solving the continuing challenge of harsh environmental conditions.

1. Introduction polymers are not biodegradable and can cause severe soil contamination
by generating microparticles during their degradation (Liao and Chen,
A large part of the earth’s surface contains desert lands found on each 2021).
continent. They estimated that 33% of the world’s land area impacts Natural biopolymers have been explored as a safe alternative to
over 1 billion people by desertification (Zvinavashe et al., 2021). Due to replace synthetic polymers to yield biodegradable and eco-friendly
increasing life activities, the land use in these regions is greatly affected hydrogels (Zainal et al., 2021). Cellulose, the most abundant polymer
by harsh environmental conditions of soil erosion and salinity, which on earth, has been applied to prepare hydrogels for environmental ap­
negatively impact the future sustainability of crop productivity and plications such as agriculture and wastewater treatment (Guan et al.,
plant survival (Borrelli et al., 2017; Lu et al., 2021). New technologies 2020; Jia et al., 2018). Cellulose with hydroxyl groups enables hydrogel
have investigated harsh remediation soils to overcome these environ­ formation by physically crosslinking cellulose solution (Baghbadorani
mental impacts (Panagos et al., 2018; D.-C. Wang et al., 2021). Super­ et al., 2020; Z. Wang et al., 2021). Furthermore, cellulose hydrogels in
absorbent hydrogels (SHs) have received significant attention due to agriculture applications have various forms, such as seed additives, seed
their low-cost, stability in the swollen state, and highly stimulating soil coatings, root dips, growth regulators, protecting agents, and controlled
remediation (Bauli et al., 2021). In agriculture, SHs can increase plant release (Fahsi et al., 2021). In this context, cellulose anionic hydrogel
water availability (Petroudy et al., 2018). Also, serve as nutrient carriers was successfully prepared by dissolving TEMPO-oxidized cellulose
and soil conditioners, increasing crop yield (Heise et al., 2019). More­ nanofibers in NaOH/urea aqueous solution and crosslinked with
over, most commercial SHs are synthetic polymers based on poly­ epichlorohydrin (Zhang et al., 2017). The resultant hydrogel showed
acrylamide and acrylate commercially identified as solid rain (Supare excellent water absorption properties and has applied as soilless culture
and Mahanwar, 2021). Despite their advantages to the soil, these mediums for sesame seeds’ growth, and the germination rate increased

* Corresponding author. Xiasha Higher Education Zone, Zhejiang Sci-Tech University, No.928 Second Avenue, Hangzhou, Zhejiang, 310018, China.
** Corresponding author. Xiasha Higher Education Zone, Zhejiang Sci-Tech University, No.928 Second Avenue, Hangzhou, Zhejiang, 310018, China.
E-mail addresses: [email protected] (S.Y.H. Abdalkarim), [email protected] (H.-Y. Yu).

https://doi.org/10.1016/j.jclepro.2022.133602
Received 3 November 2021; Received in revised form 5 August 2022; Accepted 9 August 2022
Available online 13 August 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
C.-C. Qin et al. Journal of Cleaner Production 370 (2022) 133602

to 100% within four days. Also, cellulose nanofiber-based-hydrogels pulp in an aqueous ZnCl2/glycerol solvent system. First, 71 wt% was
were prepared via TEMPO oxidation, followed by high-pressure ho­ dissolved in deionized water at 90 ◦ C for 5 min, then 2% (w/w) of waste
mogenization, and applied as hydro-retentor materials for radish and wood pulp was added to an aqueous ZnCl2 solution and vigorously
cress germination (Barajas-Ledesma et al., 2020). Their result found that stirred at 90 ◦ C for 30 min (Chen et al., 2020). Then about 0.8 g glycerol
radish seeds treated with hydrogel increased the germination index by as a “plasticizer” was added to the mixture and stirred at 90 ◦ C for
30–40%. In previous studies, our research group reported an effective another 30 min (Fig. 1). The resulting homogeneous solution was son­
dissolution mechanism of cellulose in different chloride salts, such as icated to remove the air bubbles and transferred into a polytetra­
LiCl, ZnCl2, CaCl2, and FeCl3, with different water amounts that had fluoroethylene (PTFE) plate at room temperature. The as-prepared
compared to other non-derivatizing cellulose solvents (Chen et al., cellulose-hydrogels were denoted as Gel-0 (without glycerol) and
2020). Hence, cellulose dissolution using green solvent systems is Gel-glycerol (with the addition of glycerol). The resultant cellulose
essential to confirm homogenous cellulose throughout the solution hydrogels with hydrophilic properties were applied to Wheat and Let­
preparation. To the best of our knowledge, there have been no relevant tuce seeds germination, as shown in Fig. 1. In ancient Chinese mythol­
reports on the effect of cellulose-derived hydrogels based on an inor­ ogy, the magic weapon of Guanyin was a bottle with poplar and willow
ganic salt system (zinc chloride/glycerol) on harsh soil conditions. branches. This bottle is called the “Guanyin bottle” it contains manna
The main purpose of this work is to functionalize cellulose hydrogels water, believed to bring death back to life. This study takes inspiration
by physically crosslinking waste wood pulp in an aqueous (zinc chlo­ from Guanyin Bodhisattva’s incarnation by holding “bottle manna”
ride/glycerol) solvent system with a facile and eco-friendly method. The downward pour out the water has the strength to transform the barren
effect of these cellulose hydrogels as soil amendments on natural soil for soil into healthy soil for seeds germination.
facilitating wheat germinations was evaluated. The effect of cellulose
hydrogels and KPAM on the germination of lettuce seeds under harsh
2.3. Hydrogel characterization
saline-alkali and sandy soils were studied and compared.
2.3.1. Light microscopy
2. Materials and methods The optical microscope (Nikon ECLIPSE TS100, Shanghai Photo­
electric Technology Co., Ltd.) was used for cellulose observation with a
2.1. Materials magnification of 400× (40 × 10).

Wood pulp was purchased from Hangzhou Gaojing Fine Chemical 2.3.2. Rheological analysis
Co., Ltd. Glycerol (≥99.0%), anhydrous zinc chloride (ZnCl2), sodium Viscoelasticity test of cellulose gel. The hydrogel was evaluated in
hydrogen carbonate (NaHCO3), and sodium chloride (NaCl, GR, 99.8%) Discovery Hybrid Rheometer at 80 ◦ C (TA Instruments) Equipped with
were supplied by Aladdin Reagent (Shanghai) Co., Ltd. Gongyi Xinqi 20 mm parallel plate geometry. The test methods employed were
Chemical Plant supplied potassium polyacrylate (KPAM). Hydrochloric oscillatory amplitude sweeps at a constant frequency of 1 Hz. A fre­
acid (HCl, AR, 36–38%) and nitric acid (HNO3, 65%–68%) were from quency sweep test was conducted on each sample to determine their
was obtained from Hangzhou Shuanglin Chemical Reagent Co., Ltd. Zinc viscoelastic behaviors at a constant oscillation strain of 0.1% and over a
(Zn) standard solution (GSB 04-1761-2004, 1000 mg/L) and sodium frequency range of 0.1–100 Hz. The storage (G′ ) and the loss (G′′ ) moduli
(Na) standard solution (GSB 04-1738-2004, 1000 mg/L) provided by were recorded while the strain increased from 0.01% to 100%.
National Research Center for Certified Reference Materials (NRCCRM).
The loamy soil, lettuce, and wheat seeds were purchased from the local 2.3.3. Fourier transform infrared (FTIR)
supermarket (Hangzhou, China). The sand comes from the stadium of FTIR spectrometer (Nlcolet iS50, Thermo Electron Corp., USA) was
Zhejiang Sci-Tech University. used to record infrared spectra and analyzed over a spectral width of
4000-400 cm− 1.
2.2. Dissolution and regeneration of cellulose
2.3.4. Differential scanning calorimetry (DSC)
The cellulose-hydrogel was prepared by the dissolved waste wood DSC measurements were performed on a DSC Q20 from TA

Fig. 1. The schematic diagram illustrates the preparation of cellulose hydrogels and their application in wheat and lettuce seeds germination, inspired by Guanyin
bottle manna in the mythology of ancient China.

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C.-C. Qin et al. Journal of Cleaner Production 370 (2022) 133602

instruments. Each sample was first cooled to − 90 ◦ C at a rate of 5 ◦ C weight of dry soil and wheat seeds. The mixture was placed into plastic
min− 1 and then heated to 40 ◦ C at a rate of 5 ◦ C min− 1. cups, and a soil sample without gel was taken as a control. Then 100 mL
of water was added in each case, and initial weights were taken (W0).
2.3.5. Thermogravimetric analysis (TGA) The weights of samples (Wt) were taken at regular time 7 days intervals
The thermal stability of the samples was measured using Thermog­ until a constant weight was achieved. The water uptake (%) of the gel in
ravimetric analysis (Netzsch TG209 F1) at 30–600 ◦ C (nitrogen atmo­ the soil can be determined using the following equation (1):
sphere) at a heating rate of 10 ◦ C min− 1.
Wt − W0
Water Uptake = × 100% (1)
W0
2.4. Characterization of hydrogel-applied soils and plants
W0 and Wt are the soil weight before exposure to treatment and after t
2.4.1. Wheat seeds germination days of treatment with water, gel-0, and Gel-glycerol for 7 days.
The germination experiments were conducted indoors at room
temperature. The soil was collected from Zhejiang Sci-Tech University 2.4.6. Water retention capacity
cypress trees, and plant residue was carefully removed; this soil was About 0.5 ± 0.05 g of both hydrogel and KPAM were placed in a petri
named natural soil, and elemental analysis is presented in Table S1 dish at room temperature is (26 ◦ C), and relative humidity is (65%); the
(Supplementary Information). About 100 g of air-dried soil was experiments were randomly designed with groups, and each group with
randomly designed with three replications in plastic cups, and eight three replications and repeated three data for each group of tests. The
wheat seeds were sowed for each replicate approximately 4 cm deep. simulation was carried out in an oven under high-temperature condi­
The seeds were grown in the winter (from December 2020 to February tions (60 ◦ C); the data were recorded every day until equilibrium. The
2021). Experiments followed a completely randomized design of three high-temperature condition is to record data every 1 h until the end of
treatments: control with only water, Gel-0, and Gel-glycerol treatments the 9 h. KPAM has fully absorbed water, and the data was recorded every
with a concentration of 5 ppm. Finally, 50-mL Gel-0, Gel-glycerol, and day until it reached equilibrium. The weight loss was calculated as fol­
water solutions were applied every 7 days to each cup seeding. The lows the equation (2):
whole growth parameters of the wheat plants in the plastic cups were
sampled after 21 days. Ratio of mass =
W0 − Wt
× 100% (2)
W0
2.4.2. Lettuce seed germination under saline-alkali stress
where W0 is the average value of the starting sample weight, and Wt is
The experiment was conducted indoors at Zhejiang Sci-Tech Uni­
the average sample weight at the t-day.
versity in August 2021. About 100 lettuce seeds were evenly sowed in
2–3 cm deep of mixed saline-alkali soil into the flowerpot; the experi­
2.4.7. Micronutrient determination of soil-plant samples
ments followed a randomized design of three treatments in each group
Simultaneous measurement of energy dispersive x-ray spectroscopy
with three replications: control (water), KPAM, and Gel-glycerol. The
(EDS) is analysis connected with a field-emission scanning electron
Alkaline and saline stress conditions were formed by adding 45 mM
microscopy (FE-SEM, JSM-5610; JEOL, Japan) at an acceleration
NaCl and 55 mM NaHCO3 to deionized water. The pH and electric
voltage of 1.0 kV at room temperature elemental analyses of the soils.
conductivity (E.C) of irrigation solutions were maintained at pH 8.5 and
Soil samples were dried in a 60 ◦ C oven for 24 h and then ground to a
22 mS/cm; then, the soil was treated with mixed saline-alkali soil and
fine powder in a mortar with a sterile pestle. Digestion with 10 mL of
elemental analysis of saline-alkali soil as in Table S2 (Supplementary
aqua regia mixture consisting of HCl: HNO3 (3:1) in a 100 mL test tube at
Information). Finally, 300-mL solutions of water, KPAM, and Gel-
150 ◦ C for 2 h. The resulting digest was diluted to 100 ml. The super­
glycerol were applied every 4 days to each flowerpot. After 8 and 16
natant was filtered through a microporous filter membrane (0.45 μm)
days, lettuce seeds germinations were observed by taking images of a
(Jinteng Microporous Membrane, China), and the Zn and Na concen­
flowerpot using a mobile camera to investigate the seeding growth.
trations in the digested solution were determined using inductively
coupled plasma mass spectrometry (ICP-MS, Agilent 7800, USA). The
2.4.3. Lettuce seed germination under sandy soils stress
mass concentrations of the Na and Zn standard series were (0, 2.0, 5.0,
The experiment was conducted indoors at Zhejiang Sci-Tech Uni­
10.0, 20.0, 50.0 mg/L), and (0, 0.1, 0.5, 1.0, 5.0, 10.0 mg/L),
versity in August 2021. The collected soils were sifted through a 2 mm
respectively.
sieve and air-dried. After that, mix 1.2 kg of sand and loamy soils in a
Before sample digestion, wheat roots and lettuce leaves were freeze-
flowerpot, which was sandy soils (80% sand and 20% loamy), and the
dried at − 50 ◦ C and 100 Pa for 24 h. Then grind to a fine powder in a
elemental analyses of sandy soils (sand and loamy soil) were presented
mortar using a sterile pestle and sieve (particle size <100 μm) at room
in Table S3 (Supplementary Information). Then, soils were treated with
temperature. The dry sample was mixed with 10 mL HNO3 (10 mL) in a
three treatments, each with three replications: control (water), KPAM,
100 mL test tube and left overnight at room temperature. Other diges­
and Gel-glycerol treated sand. Afterward, 100 lettuce seeds were sown
tion and concentration testing methods are the same as soil.
evenly in the soil at 2–3 cm depth. Finally, 300-mL solutions of water,
KPAM, and Gel-glycerol were applied every 4 days to each flowerpot.
2.5. Statistical analysis
After 8 and 16 days, lettuce seeds germinations were observed by taking
images of flowerpots using a mobile camera to investigate the seeding
The measured germination percentage, height, width, leaves num­
growth.
ber, plant weight, and water uptakes in the wheat collected from the
cups (n = 3) were averaged to calculate the mean value and standard
2.4.4. Observations and measurements of seeds germination assay
error. Significant differences in these indexes of wheat growth param­
Plastic cup wheat plants were sampled after 21 days, and their visual
eters were assessed by one-way analyses of variance (ANOVA), and p <
observations were photographed with a Mobile Camera. Wheat growth
0.05 was considered statistically significant.
parameters were also calculated, including average plant height,
germination percentage, average leaf number, average leaf width, fresh
biomass weight, and dry biomass weight.

2.4.5. Water-uptake behavior of gel in soil

Two hydrogels with 0.5 g were appropriately mixed with the known

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3. Results and discussion affected by a high aspect ratio and a higher degree of fibrillation. The
viscosity of Gel-glycerol was higher than that of Gel-0. This behavior
3.1. Characterization hydrogels signifies that glycerol further makes the cellulose molecular chains more
densely packed, and the viscosity remains higher when the network is
3.1.1. Solubility of wood pulp in Zncl2 salts tangled (Culebras et al., 2021).
The effect of temperature on cellulose’s swelling and dissolution The addition of glycerol to gel has a specific effect on viscosity,
behavior is shown in Fig. 2. The wood pulp fibers start to swell in melt storage modulus (G′ ), and loss modulus (G′′ ) under low-frequency con­
ZnCl2⋅3H2O, which results in a homogenous and transparent solution ditions. The elastic and loss modulus of viscous fluids have characteristic
(Fig. 2A and B). Both Gel-0 and Gel-glycerol possessed similar dissolu­ frequency dependence (Fig. 2F). The G′ and G′′ of Gel-0 and Gel-glycerol
tion states with transparency, and no fibers were found in the have changed significantly upon increasing frequency. The G′ of all gel
ZnCl2⋅3H2O solution at 90 ◦ C for 30 min, confirming the effective samples was more significant than the loss G′′ , and the high-frequency
dissolution of cellulose fibrils. Gel-0 (Fig. 2C) and Gel-glycerol (Fig. 2D) region’s rheological curve was relatively straightforward: a character­
show the thermal reversibility of the gel. The sol-gel transition can be istic sol-gel rheology curve. The Gel-glycerol showed higher G′ and G′′
detected during the heating-cooling cycle of the gels. When the gels were values than Gel-0, suggesting that the rheological properties of the gels
heated at 90 ◦ C, the gels could be changed easily to a sol state. The gels were affected by glycerol gelling structure (Peng et al., 2020). An
were transformed into a solid state after cooling to room temperature at enhancement of rheological properties of the Gel-glycerol was caused by
26 ◦ C. From the above, it can be concluded that the temperature changes the plasticity induced by glycerol on the network, which is consistent
also affect the sol-gel transition of the hydrogel. with the viscosity change rheology (Zoratto et al., 2020).

3.1.2. The rheological properties 3.1.3. Microstructure and thermal properties

The viscosity of Gel-0 and Gel-glycerol was explored at 90 ◦ C. Both DSC experiments were studied to investigate the boundaries of the
cellulose gels show a typical shear-thinning behavior (Fig. 2E). It was phase regions in cellulose dissolution (Fig. 3A). Based on DSC results, the
evident that the two gels’ viscosity decreased with the shear rate (Li aqueous ZnCl2⋅3H2O solvent has − 77.9 ◦ C. In contrast, Gel-0 and Gel-
et al., 2019). The increase in shear rate can explain this observation, glycerol ice points were shifted to − 79.3 ◦ C and − 81.3 ◦ C, respec­
which might cause the cellulose network to break easily, and individual tively. This reduction in ice points was due to the interaction between
elements to begin to flow. Besides, the viscosity of the solution can be ZnCl2⋅3H2O with the cellulose chain (Chen et al., 2020). Besides,

Fig. 2. Microscopic images of (A) Gel-0 and (B) Gel-glycerol, (C and D) corresponding photos of the cellulose in the solution, (E) the viscosity test of the two gels at a
shear rate (0.1–100s), and (F) the storage d modulus G′ and loss modulus G’’.

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C.-C. Qin et al. Journal of Cleaner Production 370 (2022) 133602

Fig. 3. (A) DSC curves, (B) FTIR spectra, (C) TGA, and (D) DTG curves of wood pulp, Gel-0, and Gel-glycerol.

glycerol might be used as a cryoprotectant to hinder protein crystals molecules began at onset temperatures (T0) of about 281.9 ◦ C and
from freezing below 0 ◦ C (Zhang et al., 2019), and the above result 272 ◦ C, respectively. Besides, the T0 of Gel-glycerol was about 69 ◦ C less
suggests that glycerol can enhance the anti-freezing performance of than the original wood pulp (Xu et al., 2010). Furthermore, the
hydrogels. maximum degradation temperatures (Tmax) were 370 ◦ C for wood pulp,
The FTIR spectra in Fig. 3B depict that the crystal structure of the 300.4 ◦ C for Gel-0, and 308.2 ◦ C for Gel-glycerol. In addition, the re­
wood pulp fiber is affected by the ZnCl2⋅3H2O treatment, and the sidual weight of Gel-0 and Gel-glycerol (28.2–31.8%) was higher than
characteristic bands of cellulose structure are emphasized. All Gel wood pulp (12.5%) at 600 ◦ C. This study suggested that a higher con­
samples showed similar characteristic bands to wood pulp, demon­ centration of ZnCl2 caused more severe damage to cellulose intermo­
strating no noticeable chemical reaction during cellulose dissolution. In lecular hydrogen bonds, leading to decreased thermal stability (Burger
contrast, the shifted peak and the changed peak intensity indicated et al., 2020). The residual components are mainly zinc oxide and zinc
changes in structural details, such as the reconstruction of hydrogen chloride, higher than 12.5% residual ash of lignocellulose (Jones et al.,
bonds between cellulose molecules. For example, the strong band that 2013).
appeared at 3430 cm− 1 in wood pulp was attributed to the stretching
vibration of O–H groups in cellulose, which shifted to a higher wave­
3.2. Assessment of hydrogels for soils
number in Gel-0 (3443 cm− 1) and Gel-glycerol (3450 cm− 1). This shift
could be attributed to the dissolution of wood pulp with ZnCl2⋅3H2O
3.2.1. Wheat seeds germinations
caused by parity vibration of intramolecular hydrogen-bonded OH-
The influences of Gel-0 and Gel-glycerol in wheat germination and
groups and Zn⋅⋅⋅OH stretching (Li et al., 2019; Zhang et al., 2019).
growth after 7, 14, and 21, days are depicted in Fig. 4A. The wheat plant
Moreover, the bands at 2920 and 1430 cm− 1 for all samples were
showed the relatively highest growth rate with treatment in the soil.
assigned to C–H’s stretching vibration, H–C–H’s bending vibration, and
There are significant differences between applying Gel-glycerol, Gel-0,
O–C–H for the aliphatic moieties in cellulose (Liang et al., 2017; Song
and water at the exact dosage (p < 0.05), which recommends that Gel-
et al., 2019). Both bands at 1430 and 552 cm− 1 were seen in the spectra
glycerol and Gel-0 efficiently improve wheat growth. After 21 days,
of wood pulp while band intensities significantly weakened in Gel-0, and
the wheat plant with Gel-glycerol produced more roots than Gel-0 and
Gel-glycerol indicated that the regenerated cellulose had structural
water treatments (Fig. 4B). The maximum root length was about 2.7 cm,
changes. In addition, the characteristic band at 895 cm− 1 was associated
3.8 cm, and 5.5 cm for water, Gel-0, and gel-glycerol.
with the cellulose Iβ structure and the disordered form in cellulose found
Furthermore, the effects of Gel-0 and Gel-glycerol treatments on
on Gel-0 and Gel-glycerol (Cheng et al., 2017; Zhang et al., 2019).
wheat germination in outdoor soil with a large area are shown
Fig. 3C shows thermal stabilities of wood pulp, Gel-0, and Gel-
(Fig. 4C–E). Fig. 4E showed a significant increase in wheat germination
glycerol samples.The weight is almost unchanged in the temperature
with Gel-glycerol treatment within 8 days but a decrease in wheat ger­
range between 150 ◦ C and 342 ◦ C. More weight loss (68.3%) from
minations as in the other treatments (Fig. 4C and D). The increase in
341 ◦ C to 370 ◦ C was comparatively fast, attributable to dehydration and
wheat germination was most significant in Gel-glycerol because Gel-
decomposition of the molecules of wood pulp (Fig. 3D). When the
glycerol with hydrophilic properties could swell in humid environ­
temperature increased from 371 ◦ C to 600 ◦ C, the weight losses were
ments and endow the plant roots with extra moisturization. This result
slower and regular. Nevertheless, the TG curves of Gel-0 and Gel-
indicates that the hydroxyl groups in the cellulose chains coordinated
glycerol illustrated that the dehydration and decomposition of the
with Zn2+ ions. In addition, water molecules can be retained in cellulose

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Fig. 4. (A) Photograph of wheat plant growth in soil treated with water, Gel-0, and Gel-glycerol on day 1 to day 21, (B) the photograph represents the roots of the
wheat plant after 21 days of soil with various treatments, the photograph of wheat germination and growth on outdoor soil (0.5*0.5 m) between 1 and 8 days after
treatment with water (C), Gel-0 (D), Gel-glycerol (E), and (F) Schematic diagram of functional cellulose hydrogel and their possible enhancing mechanism of seeding
growth with various treatments.

sheets, which could act as a plant root coating to increase water diffusion between (7–21 days) under soil conditions; are displayed in Fig. 5G and
and increase the Zn2+ nutrients in the soil (Fig. 4F). H. It is clear that the weight values for all samples slightly increased as
germination time increased. This result strongly correlates with an in­
3.2.2. Wheat seedings growth parameters crease in germination time, seeding shoot, dosage rate of hydrogels or
The growth parameters of wheat and results relating to plant growth, water, and root length, which finally increases plant weight. Compared
such as spike length, width, and germination percentage, are repre­ with water treatment, a maximum increase in the average weight by 7.6
sented in Fig. 5. The addition of Gel-glycerol and Gel-0 had significant g after 21 days with Gel-glycerol treatment(Fig. 5G). Nevertheless, the
effects on the plant height (p < 0.05). The increasing tendency was average weight of the wheat plant increased by only 5.5 g after 21 days
highest with Gel-glycerol than with other treatments. With Gel-glycerol with Gel-0 treatment.
treatment, the plant height increased to 7.6 cm, 15.0 cm, and 19.7 cm Under hydrogel treatments, wheat plants exhibited more remarkable
after 7, 14, and 21 days, respectively (Fig. 5A). While for Gel-0 treat­ water uptake improvements than water treatment (Fig. 5H). Gel-
ment, the average plant height increased to 4.0 cm, 12.4 cm, and 18.4 glycerol shows the best water uptake among other treatments. Water
cm after 7 and 21 days, respectively. Meanwhile, the germination per­ uptake values were improved by 94.7% and 75.9% after 21 days, with
centage of wheat plants with Gel-glycerol and Gel-0 increased by 21.9% Gel-glycerol and Gel-0, respectively. When the cellulose has dissolved in
and 15.6% over water treatment, respectively (Fig. 5B). The above re­ the chloride salt solution, the separated cellulose chains partially poly­
sults indicate that Gel-glycerol and Gel-0 positively affect the early stage merize during the solvent exchange process at the water molecules that
of plant growth, increasing the seedings’ growth parameters. As seen in intersect the hydrogen-bond networks (Chen et al., 2020), which results
Fig. 5C, the average leaf number increased as time increased, and the in network passageways and allows water vapor molecules to penetrate
plants with water were weak. Compared with water treatment, the the wheat roots (Cuomo et al., 2019). Therefore, under the same envi­
average number of leaves with Gel-glycerol and Gel-0 increased by ronment, the addition of Gel-glycerol has a significant effect on water
100% and 50%, respectively. Besides, the average leaf width increased retention performance and an inhibitory effect on soil moisture evapo­
by 0.13 cm and 0.09 cm with Gel-glycerol and Gel-0 treatments, ration (Zhang et al., 2017). Besides these, Gel-glycerol was also bene­
respectively (Fig. 5D). Also, the fresh biomass weight of wheat increased ficial by reducing the Cd concentration in the natural soil, as shown in
by 350% and 500% with Gel-0 and Gel-glycerol, respectively (Fig. 5E), Fig. S1, which makes the roots grow faster and more robust than water
associated with water. In comparison, the dry biomass weight of wheat treatment (Fahsi et al., 2021). It can be concluded that the obtained
increased by 329% and 445% for Gel-0 and Gel-glycerol, respectively Gel-glycerol had a positive effect on soil, which was also helpful in
(Fig. 5F). Therefore, gel treatments in this work as soil amendments retaining water for plant roots and increasing the Zn2+ nutrients in the
significantly increased the germination percentage and plant growth. soil. This explanation was further confirmed by EDS and ICP-MS results
Moreover, grain weight by plants and water uptake of wheat seeds which show that Gel-glycerol can significantly increase the

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C.-C. Qin et al. Journal of Cleaner Production 370 (2022) 133602

Fig. 5. The effect of water, Gel-0, and Gel-glycerol treatments on wheat growth parameters after 21 days, including (A) average plant height, (B) germination
percentage, (C) average leaf number, (D) average leaf width, (E) fresh biomass weight of wheat, (F) dry biomass weight of wheat, (G) average sample weight, and (H)
water uptake.

concentration of trace element Zn and decrease salt content in natural more water molecules.
soil, thereby regulating the absorption of micronutrients by plant roots Nevertheless, the shape and size of KPAM shrank significantly in the
(Tables S4–S5 and Fig. S2, Supplementary Information). 9 h, and the KPAM weight loss has reached a maximum ratio of 92%.
This phenomenon indicated that KPAM could degrade under high tem­
3.2.3. Water retention capacity peratures (60 ◦ C) depending on its environment. Besides, its average
Gel-glycerol hydrogel has a better water retention capacity than molecular weights can be effectively decreased via radical chain deg­
KPAM at room temperature, as illustrated in Fig. 6A. The mass ratio of radations to cause chain scissions (Zhang et al., 2017).
the Gel-glycerol increased when exposed to the open air for 8 days. This
improvement is because Gel-glycerol begins to absorb moisture in the 3.2.4. Lettuce seeds germination under harsh soils
air, and the highest absorption exceeds 160% of its own and then loses The effects of Gel-glycerol and KPAM on the germination of lettuce
water slightly to reach equilibrium (Fig. 6B). However, the mass ratio of seeds under harsh soil between 1, 8, and 16 days were provided in
KPAM decreased after three days (Fig. 6A); thus, its shape and size were (Fig. 7). Photographs of lettuce seeds germination were evaluated to
significantly changed within 8 days (Fig. 6B), and the water evaporation confirm whether these Gel-glycerol could provide micronutrients to the
quickly reached 85%. Fig. 6C represents the evaluation of water loss plant under different soils (saline-alkali and sandy soils). It was evident
with a time of the Gel-glycerol and KPAM at an extreme environmental that Gel-glycerol treatment showed the highest lettuce germination
temperature of 60 ◦ C for 9 h. It was clear that Gel-glycerol still maintains percentage of 38%, compared with other treatments of 20% for KPAM
good water retention capacity after a slight water loss; only weight and 7% for water (Fig. 7A). Indicating that the effects of Gel-glycerol
decreased by 8% within 9 h. Meanwhile, its shape and size practically with the presence of active groups could act as a regulator for seed
did not change (Fig. 6D). This observation can be attributed to high germination and growth by reducing the salt content in the soil
hydrophilicity and the network structure of Gel-glycerol for absorbing (Tables S5–S6, Supplementary Information). Indeed, through Gel-

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C.-C. Qin et al. Journal of Cleaner Production 370 (2022) 133602

Fig. 6. (A) Evolution of water loss with a time of the Gel-glycerol hydrogel and KPAM kept in a chamber at 26 ◦ C and 65% relative humidity, (B) photographs of the
Gel-glycerol hydrogel and KPAM after 1 and 8 days (26 ◦ C), (C) evolution of water loss with a time of the Gel-glycerol hydrogel at 60 ◦ C, and (D) photographs of the
Gel-glycerol hydrogel and KPAM after heated for 1 and 9 h (60 ◦ C).

Glycerol treatment, micronutrients can be adjusted to improve the soil increasing crop yield in recent years. However, the mechanism of these
and increase the lettuce germination percentage. When sandy soils were superabsorbent hydrogels for increasing plant water availability and
treated with Gel-glycerol, it resulted in the highest germination per­ enhanced seed germinations is still unclear. More importantly, most of
centage of 22%, compared with 12% for KPAM and 3% for water these superabsorbent hydrogels are non-degradable and have serve ef­
(Fig. 7B). These results confirmed that the KPAM as a superabsorbent fects on soils. To explore the sustainable increase of agricultural pro­
polymer could absorb hundreds of times its original weight in purified duction; with positive effects on soil amendments, Gel-glycerol with
water. However, water retention can quickly evaporate at high tem­ ultrahigh water retention capacity was used in the present study. Adding
peratures. Indeed, the specific retention of KPAM was weaker than the Gel-glycerol as a soil conditioner positively evaluates wheat and lettuce
roots of most plants. Generally, the lettuce seeds have mainly produced seed germinations and growths. The lettuce growth in saline-alkali and
in arid and semiarid conditions. sandy soils further supports that Gel-glycerol possessed high germina­
Nonetheless, waterlogging is the main stress factor that affects seed tion percentages due to a positive effect of Gel-glycerol additions on
yield and quality at early flourishing, thus influencing lettuce growth soils-plants by tailoring plant nutritional needs of Zn and Na. The Na
and germination. The prepared Gel-glycerol can decrease the stress of concentration in soils, wheat root, and lettuce leaves decreased with Gel-
waterlogging duration for lettuce seeds by enhancing the water reten­ glycerol treatment. This work will promote the advancement of cellulose
tion capacity, which could slowly release into the root system (Fahsi hydrogel in the agriculture ecosystem, displaying the excellent value in
et al., 2021; Vivas et al., 2006). By combining the results of EDS and soil modulating, seed germination, and an alternate solution for solving
ICP-MS, Gel-Glycerol can regulate the changes of micronutrients in the the continuing challenge of harsh environmental conditions to meet the
soil to affect lettuce growth and germination in soils (Tables S6–S9, sustainable development of crop production.
Supplementary Information). Compared to water treatment, the Na While this study opens a new outlook on the dissolution of cellulose
concentration in saline-alkali soils decreased over the initial value by waste with energy-saving and low-cost methods, it gives further
33.2%, and Zn concentration improved by 105.3% with Gel-Glycerol importance to cellulose hydrogel with ultrahigh water retention ca­
treatment (Fig. 7C). This work further showed a positive effect of pacity in the agriculture ecosystem. Consequently, future studies might
Gel-glycerol additions on lettuce leaves is sufficient to meet the plant’s extend this approach to other waste cellulose to produce regenerated
nutritional needs of Zn and Na. cellulose for a more comprehensive range of applications. Future studies
have to answer how nutrients such as (Zn and Cl) can affect plant
4. Conclusion toxicity and should provide a basis for understanding the mechanistic
role of Zn and Cl in response to resistance and tolerance of plants to
Desertification caused by harsh soil conditions, especially soil diseases.
erosion and salinity, has received more public concern. To mitigate
harsh soils, a large variety of superabsorbent hydrogels have been used
to assess their efficiency as nutrient carriers and soil conditioners,

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C.-C. Qin et al. Journal of Cleaner Production 370 (2022) 133602

Fig. 7. Photographs of lettuce seeds germinated after 1,8 and 16 days of sowing lettuce seeds on saline-alkali soil (A), sandy soils (B), treated with water, KPAM, and
Gel-glycerol, and (C) represent Na and Zn concentrations in saline-alkali soil, and lettuce leaves with water and Gel-Glycerol treatments.

CRediT authorship contribution statement Appendix A. Supplementary data

Cong-Cong Qin: Conceptualization, Methodology, Formal analysis, Supplementary data to this article can be found online at https://doi.
Writing – original draft. Somia Yassin Hussain Abdalkarim: Re­ org/10.1016/j.jclepro.2022.133602.
sources, Supervision, Writing – review & editing. Ying Zhou: Performed
the experiments, Funding acquisition. Hou-Yong Yu: Writing – review References
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