ACS Nano
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2024
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IF 15.8
Guoqiang Zhao,Xiaoyu Tao,Tongsen Guo,Liangjie Fu,Huaming Yang
Solution-phase epitaxy is a versatile method to synthesize functional nanomaterials with customized properties, where supports play a central role as they not only serve as nucleation templates but also greatly affect the local electronic structures. However, developing functional supports remains a great challenge. Herein, inspired by the commonly observed epitaxy of minerals in the natural environment, we report using calcination-modified kaolinite as the support for the epitaxial growth of hexagonal CoO nanoparticles (h-CoO NPs), which enables over 40 times higher mass-specific activity toward H2O2 electrochemical activation than the counterpart without the support. High-resolution electron microscopy, magic-angle spinning nuclear magnetic resonance, and X-ray absorption fine structure results prove that the Al sites in kaolinite play a crucial role in the formation of h-CoO NPs. Moreover, the five-coordinate Al (AlV) sites produced by the dehydration of kaolinite are indispensable for forming the epitaxial interface. Theoretical calculations reveal that the local electron densities around AlV sites are lower than those of general six-coordinate Al sites, which render AlV sites with strong adsorption capability that facilitates the nucleation of h-CoO NPs. Also, the AlV sites induce the electron transfer from h-CoO to the kaolinite support that results in the upshift of the Co 3d band center and hence improve the H2O2 activation kinetics. Our results demonstrate the superiority of nanoclay as functional supports and could offer a more benign strategy to the solution-phase epitaxy production of functional nanomaterials for diverse applications.
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WATER RESEARCH
·
2024
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IF 11.4
Yunxuan Chen,Jun Nan
Abandoning the costly development of new membrane materials and instead directly remodeling the naturally occurring cake layer constitutes a dynamic, low-cost, long-lasting, and proactive strategy to "fight fouling with fouling". Several optimization strategies, including coagulation/modified magnetic seed loading and applying a weak magnetic force (0.01T) at the ultrafiltration end, improved the anti-fouling, retention, and sieving performances of conventional ultrafiltration process during the treatment of source water having complex natural organic matter (NOMs) and small molecule micropollutants. Two modified magnetic seeds we prepared were composite nano-seed particles (Fe 3 O 4 @SiO 2 -NH 2 (FS) and Fe 3 O 4 @SiO 2 @PAMAM-NH 2 (FSP)). Aim of the study was to regulate the formation of cake layer via comprehensive testing of the antifouling properties of optimized processes and related mechanistic studies. It was found to be essential to enhance the interception of xanthate and tryptophan proteins in the cake layer for improving the anti-fouling performance based on the correlation and redundancy analyses, while the use of modified magnetic seeds and magnetic field showed a significant positive impact on water production. Blockage modeling demonstrated the ability to form a mature cake layer during the initial filtration stage swiftly. This mitigated the risk of irreversible fouling caused by pore blockage during the early stage of coagulation-ultrafiltration. Morphologically, the reconstructed cake layer exhibited elevated surface porosity, an internal cavity channel structure, and enhanced roughness that can promote increased water flux and retention of water impurities. These optimized the maturity of the cake layer in both time and space. Density Functional Theory (DFT), Extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory, and Modified Extended Derjaguin-Landau-Verwey-Overbeek (MDLVO) calculations indicated aggregation behavior of matter on the cake layer to be enhanced effectively due to magnetic seed loading. This is mainly due to the strengthening of polar interactions, including hydrogen bonding, π-π* conjugation, etc., which can happen between the cake layer loaded with FSP and the organic matter. Under the influence of a magnetic field, magnetic force energy (VMF) significantly impacts the system by eliminating energy barriers. This research will provide innovative strategies for effectively purifying intricate source water through ultrafiltration while controlling membrane fouling.
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ELECTROCHIMICA ACTA
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2024
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IF 5.5
Huiyao Li,Zhuoran Ao,Yu Wan,Yaru Liang,Peiguang Li,Youlan Zou
The improvement of ionic conductivity and Li dendrite inhibition capability of poly(ethylene oxide)(PEO)-based solid polymer electrolytes(SPEs) is urgent for the development of all-solid-state lithium metal batteries (ASSLMBs). Here, intercalated composite consisted with PEO polymer chains inserted into the clay gallery of the formamide intercalated kaolinite (KM) is formed. Due to this alternating organic-inorganic layered structure, the crystallinity of PEO decreases to 26.2% and the ion conductivity of SPE with 3% KM of PEO mass added(PEO+KM-3) increased to 1.43 × 10 −3 S cm −1 at 60 °C. Besides, bis (trifluoromethane) sulfonimide lithium salt (LiTFSI) interacts with formamide to form a complex, making the local solvated Li + transports close to a quasi-solid model. PEO+KM-3 SPE exhibits a good inhibition effect on lithium dendrites due to the formation of organic silicon at lithium anode side, and Li/ PEO+KM-3/Li cell works steadily for more than 1600 h at 60 °C with 0.1 mA cm −2 . The assembled Li//LiFePO 4 cell provides a capacity of 118 mAh g −1 after 500 cycles at 0.5 C at 60 °C.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Yunxuan Chen,Jun Nan,Mingqi Guo,Yibo Zhang,Jinghui Wang,Qi Wang,Rui Fang
Finding alternative solutions of water source containing short-term relative high turbidity and large organic content is a pressing need in view of the inherent limitations of traditional inorganic coagulants. Requirement of significant dosage increase for conventional iron and aluminum salt coagulants can create several challenges including dose adjustment, suboptimal performance and high concentration of residual metal ions. In this study, acrylamide monomer (AM) and methacryloyloxyethyltrimethylammonium chloride (DMC) were grafted onto starch and carboxymethyl starch to obtain novel cationic and amphoteric starch-modified coagulants. Concurrently, the obtained coagulants were comprehensively evaluated under varying simulated water quality conditions to analyze their turbidity and organic matter removal efficiencies. Polymerized aluminium chloride (PACl) was used as the reference coagulant to evaluate the roles of polymer charge density, total charge, and molecular chain length in the coagulation mechanism for further illustration of their efficacy. In comparison to the traditional coagulant PACl, the modified coagulant was found to be more effective in enhancing flocculation and aggregation behavior, lowering of energy barriers, and enhancing adsorption energy by using the Density Functional Theory (DFT) calculations and Extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory based investigation of the mechanism. Moreover, these behaviors were mainly attributed to significant exchange of charge density between coagulant and the pollutants. Additionally, in order to facilitate accurate and efficient treatment of water having diverse qualities, quadratic polynomial equation based mathematical model was constructed for quantitative analysis and model prediction. Findings of this study point towards an effective and precise approach to coagulation technology and thereby enabling sustainable and efficient purification of turbid source water containing large organic matter.
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Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Na Li,Yuping Fan,Xianshu Dong,Xiaomin Ma,Ruxia Chen,Ming Chang,Guang Xu
To mitigate the negative environmental impact of flocculants while improving their efficiency, developing eco-friendly and effective flocculants is essential. In this study, a cationic hydrophobic flocculant (GgB) was synthesized using natural organic polymer guar gum and the surface-active monomer N-benzyl-2-(methacryloyloxy)-N, N-dimethylethan-1-aminium chloride via ultraviolet-initiated polymerization. The synthesis conditions were optimized through response surface methodology to maximize the flocculant's performance. The monomer was found to be most likely grafted onto the 3rd hydroxyl group of the guar gum galactose branched chain using Raman spectroscopy, elemental analysis, nuclear magnetic resonance X-ray photoelectron spectroscopy, scanning electron microscopy, and density functional theory simulation. This flocculant was subsequently applied to the flocculation-filtration processes of montmorillonite and kaolin particles in wastewater, which revealed the flocculation efficiency of GgB on montmorillonite suspension was higher than kaolinite at the same dose, but more effective for kaolinite dewatering. Mechanistic studies and molecular dynamics simulations indicated that the cooperation between charge neutralization, hydrophobic association, and adsorption bridging synergistically contributed to clay particle flocculation, and hydration of clay minerals has a significant effect on GgB, with electrostatic interactions dominating in montmorillonite systems and van der Waals forces prevailing in kaolinite systems. Overall, this research highlights the synthesis of eco-friendly flocculant and elucidates its mechanisms in clay particles, offering critical insights for the design and application of environmentally sustainable flocculants in wastewater treatment processes.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Chongming Wang,Sujie Shan,Zhengyu Yang,Xinpeng Xu,Xingning Huang,Xi Li,Songqi Liu,Boling Li,Yao Xu,Dapeng Li
Mounting evidence indicates that eliminating phosphate (P i ) alone is not enough to lower outbreak risks of undesirable algae, and synchronously sequestrating organic phosphorus species (OPs) dissolved in overlying water and residing in sediments cannot be ignored. However, more efforts were focused on the immobilization of P i than OPs because of insufficient understanding and analytical challenges. Herein, CaO 2 -loaded halloysite nanotubes/lanthanum-crosslinked sodium alginate (La-CaO 2 @HNTs/SA) hydrogel beads were newly developed and employed as a capping material for efficiently sequestrating P i and OPs from eutrophic water and sediment. Batch sorption results showed that the La-CaO 2 @HNTs/SA has a high uptake capacity towards P i (i.e., 44.05 mg-P/g) and Myo -inositol hexakisphosphate (IHP, a representative pollutant of OPs, 36.28 mg-P/g), and good selectivity for P in the presence of NO 3 – , Cl − , and HCO 3 – , profited by synergy of electrostatic attraction, inner-sphere complexation, surface precipitation, and partial degradation. After applying La-CaO 2 @HNTs/SA, P levels in overlying water could rapidly reduce from 0.95 to 0.01 mg-P/L within 120 min. Further thin-layer capping experiments (60 days) indicated that La-CaO 2 @HNTs/SA performed very well in immobilizing P i and OPs in overlying and pore waters and enhancing reductant-soluble P transformation (BD-P; ∼19 % to 11 %) to more stable HCl-extracted P (HCl-P; ∼33 % to 43 %) in sediments under continuous P input, with minor effect on benthic microorganisms. These findings advance the use of eco-friendly La-CaO 2 @HNTs/SA in eutrophication alleviation via simultaneous sequestration of P i and OPs.
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CARBOHYDRATE POLYMERS
·
2025
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IF 12.5
Shijia Gu,Wenzhi Zhang,Xiaoxiao Tan,Peng Wang,Zhichun Shi,Jun Lv,Ming Zhao,Guohua Dong
The extensive utilization of natural starch (NS) in preparation of slow-release fertilizer (SRF) remains a crucial challenge owing to its undesirable defects such as poor solubility and mechanical properties. Herein, based on the preparation of di-esterified starch derivatives (PCDS) from NS with phosphoric acid and carbamate and synthesis of PCDS cross-linked chitosan (CS) hydrogels (PCDS-CSH), a dual-layer coated urea SRF (EC/PCDS-CSH/urea-SRF) was successfully developed utilizing ethyl cellulose (EC) and PCDS-CSH as the inner/outer coating. Due to the ameliorated properties of PCDS (viscosity and gelation temperature) compared to NS, the PCDS-CSH shows significantly improved swelling performance and water retention capacity. Importantly, the corresponding EC/PCDS-CSH/urea-SRF demonstrates superior nitrogen (N) nutrient slow-release behaviors, achieving cumulative release rates of 48.5 % (12 h ) and 61.3 % (48 h) in water together with 22.9 % (10 d) and 52.9 % (29 d) in soil, respectively. Kinetics fitting analysis reveals that N release in EC/PCDS-CSH/urea-SRF follows the Higuchi model (in water) and First-order kinetics (in soil), respectively, both of which belong to non-Fickian diffusion process. Furthermore, tomato seedling pot experiments demonstrate that the EC/PCDS-CSH/urea-SRF shows a significant promotion role toward the plant growth. Consequently, this study provides a novel route for developing biomass based SRFs utilizing modified NS derivatives.
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JOURNAL OF RARE EARTHS
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2025
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IF 7.2
Jiaxin Pan,Xiaowei Huang,Longsheng Zhao,Depeng Liu,Ting'an Zhang,Zongyu Feng
The investigation of the leaching mechanisms of ion adsorption rare earth ores (IAREO) using MgSO 4 is significantly hindered by the complex mineral composition. In this study, the direct analogue of the natural IAREO sample, Y-kaolinite, was prepared and used to investigate the leaching mechanisms of rare earths from kaolinite under varying initial MgSO 4 concentrations and pH. The results of X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray absorption fine structure (XAFS) data indicate that the Y-kaolinite prepared exhibits a similar composition, micromorphology and coordination structure with nature IAREO sample. The coordination number and bond length of Y–O are 9.2±1.4 and 0.23±0.010 nm, respectively. The results of batch desorption experiments and sequential chemical extractions show that lowering the initial pH from 5.00 to 2.00 significantly enhances the desorption of rare earths from Y-kaolinite. Specifically, the additional desorption amounts are 0.52 mmol/kg for inorganic hydroxy Y (Hy-Y) and 0.40 mmol/kg for ion-exchangeable Y (Ex-Y). The enhancement mechanism was revealed by density functional theory (DFT) and Visual MINTEQ. The desorption of Hy-Y and Ex-Y is directly and indirectly enhanced by hydrogen ions, respectively. The desorption of Hy-Y is consistent with the dissolution behavior of the Y hydroxyl compound at lower pH. The desorption of Ex-Y is promoted by [Al(H 2 O) 6 ] 3+ released from Hy-Al by hydrogen ions. Additionally, when the concentration of MgSO 4 is 100 mmol/L and initial pH is 2.00, the desorption rate of rare earths is 87.1%, while the adsorption rate of magnesium is 63.1% and the stoichiometry ratio of Y 3+ to Mg 2+ is 1.04, which indicates that adequate hydrogen ions reduce the consumption of MgSO 4 and enhance the leaching of rare earth. These finding provide valuable insights into optimizing the selective leaching of rare earths from IAREO.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
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2025
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IF 5
Nusrullah Mehtab,Lu Bin,Miao Guilan,Bibi Amna,Wang Yanmei
Acrylamide-based non-ionic polymers have gained significant attention for wastewater treatment due to their high flocculation efficiency. However, optimizing the polymer dosage and knowing the role of hydrogen bonding in flocculation remain challenging. In this study, acrylamide/(N-hydroxyethyl)acrylamide (AM/HEA) copolymers at different molar ratios were synthesized via solution polymerization. The polymers were characterized using FTIR, 1 H NMR, DSC, and TGA. The kaolin suspension was employed to evaluate the flocculation performance of copolymers by the jar test method. The AM/HEA copolymers showed superior flocculation efficiency, achieving 98% turbidity removal at an optimal polymer flocculant dose of 0.2 mg/L, with a stirring speed of 400 rpm and a stirring time of 180 s. Zeta potential and TEM imaging results showed that flocculation primarily occurred through polymer adsorption on the kaolin surface, with its coiled conformation may enhance particle bridging. These results emphasize the critical role of polymer molecular structure in optimizing flocculation performance and suggest AM/HEA copolymers as efficient flocculants for water treatment exercises.
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WATER RESEARCH
·
2025
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IF 12.4
Peng Wang,Pei An,Chenlong Wang,Zhaoyu Chen,Chenglong Yu,Wen Zhang,Shengyan Pu
Nontarget reactions (NTRs) have long been considered a major barrier to the efficiency and sustainability of in situ chemical oxidation (ISCO) in contaminated aquifers. Here, we report a paradigm-shifting discovery on the dual role of ubiquitous subsurface components, clay minerals and humic acid (HA), in H 2 O 2 -based remediation. We demonstrate through controlled experiments that HA adsorbed onto montmorillonite (MT) enhances dimethyl phthalate (DMP) removal by 18.3–125.6 % compared to systems containing only clay or HA. Contrary to the conventional view of NTRs as parasitic scavengers of reactive oxygen species, they also promote the generation of target hydroxyl radicals (∙OH), as directly verified by quenching experiments and EPR spectroscopy. Electrochemical analyses confirm that HA mediates direct electron transfer (DET) between MT and H 2 O 2 , leading to interfacial ∙OH formation. The electron-shuttling efficiency of HA is governed by its molecular structure, with electron-donating groups (e.g., para-OH, enediols) maximizing DET efficacy, as quantified by Hammett correlations ( R 2 >0.90). The improved interfacial reaction diffusion model further reveals that ∙OH-mediated reactions are free from diffusion limitations ( η =0.999) and confined to the solid-liquid interface (<200 nm), where non-radical pathways dominate. Our findings redefine NTRs as tunable interfacial processes and establish a mechanistic basis for leveraging their beneficial role in next-generation sustainable aquifer remediation.
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ENERGY
·
2025
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IF 9.4
Zhangzhou Wang,Yurong He,Tianqi Tang,Gong Cheng
Lithium-ion batteries, integral to electric vehicles and energy storage systems, encounter significant thermal management and safety challenges. In light of these issues, this study developed a multifunctional phase change material (PCM) with enhanced flame-retardant properties for application in battery thermal management systems (BTMS). The PCM demonstrated good cyclic stability, retaining a high phase change enthalpy value of 93.68 J/g after 50 cycles. Cone calorimeter tests revealed that the peak heat release rate of the PCM was 64.3 % lower than that of pure polyethylene glycol, with a total heat release reduction of 32.7 %, and the PCM exhibited self-extinguishing behavior, achieving the UL-94 V-0 flame retardancy rating. Its thermal conductivity and thermal diffusivity were 2.73 W/(m·K) and 1.00 mm 2 /s, respectively, effectively enhancing heat dissipation efficiency. In battery thermal management experiments, the PCM effectively kept the maximum battery temperature below 45 °C across a range of ambient temperatures from 25 °C to 35 °C and discharge rates from 1C to 2C, maintaining battery safety. This study offers novel perspectives on the design of flame-retardant materials for BTMS and an effective approach to enhancing battery thermal management and safety.
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BIOMACROMOLECULES
·
2025
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IF 5.4
Chuchu Tang,Xianda Liu,Shuxiang Zhang,Shengjun Cheng,Wenjie Wang,Xiran Zhou,Junhan Tang,Ran Wei,Weifeng Zhao,Changsheng Zhao
Severe intestinal bleeding poses life-threatening risks, including hemorrhagic shock, organ damage, infection, and death. Current hemostatic materials struggle to adhere to wet, dynamic intestinal tissues, hindering effective hemostasis. Inspired by the hookworm’s rigid mouthpart and flexible body, which enable robust anchoring in the intestine, we developed a hydrogel microneedle patch (40K@P/G MNs) integrating multianchoring and hemostatic mechanisms. The patch leverages microneedle topology and gallic acid-grafted chitosan for enhanced mucosal adhesion, coupled with an extensible backing layer of optimized elasticity, achieving robust tissue adhesion (86.17 ± 26.19 mm Hg) in porcine intestinal models. The patch enhances clotting through a synergistic mechanism involving both chitosan and kaolin, which collectively promote platelet adhesion and activate the coagulation cascade, yielding a low blood coagulation index (4.92 ± 0.68%). It demonstrated excellent hemostatic performance in a rat liver hemorrhage model, achieving hemostasis within 35 s and preventing rebleeding. Its backing layer matches the intestine’s mechanical stress, providing elasticity to withstand peristaltic forces. This multianchoring microneedle patch offers a carbohydrate-based solution for rapid, localized hemostasis in challenging intestinal environments.
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