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2025 Vol. 10, No. 5

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Review articles
Antibiotics-heavy metals combined pollution in agricultural soils: Sources, fate, risks, and countermeasures
Yuanxiang Shu, Donghao Li, Tong Xie, Ke Zhao, Lu Zhou, Fengxiang Li
2025, 10(5): 869-897. doi: 10.1016/j.gee.2024.07.007
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Agricultural soil is related to food security and human health, antibiotics and heavy metals (HMs), as two typical pollutants, possess a high coexistence rate in the environmental medium, which is extremely prone to inducing antibiotic-HMs combined pollution. Recently, frequent human activities have led to more prominent antibiotics-HMs combined contamination in agricultural soils, especially the production and spread of antibiotic resistance genes (ARGs), heavy metal resistance genes (MRGs), antibiotic resistant bacteria (ARB), and antibiotics-HMs complexes (AMCs), which seriously threaten soil ecology and human health. This review describes the main sources (Intrinsic and manmade sources), composite mechanisms (co-selective resistance, oxidative stress, and Joint toxicity mechanism), environmental fate and the potential risks (soil ecological and human health risks) of antibiotics and HMs in agricultural soils. Finally, the current effective source blocking, transmission control, and attenuation strategies are classified for discussion, such as the application of additives and barrier materials, as well as plant and animal remediation and bioremediation, etc., pointing out that future research should focus on the whole chain process of “source-process-terminal”, intending to provide a theoretical basis and decision-making reference for future research.
Recent advances on the electrocatalytic oxidation of biomass-derived aldehydes
Zhikeng Zheng, Ke Li, Lu Lin, Zhiwei Jiang, Yuchen Wang, Kai Yan
2025, 10(5): 898-916. doi: 10.1016/j.gee.2024.09.004
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The escalating demand for sustainable and environmentally benign chemical processes has driven the exploration of biomass as an alternative to non-renewable resources. Electrocatalytic upgrading of biomass-derived aldehydes plays a crucial role in biomass refining, and has become a frontier of mainstream research. This paper reviews the recent advances on the electrocatalytic oxidation of typical biomass-derived aldehydes (5-hydroxymethylfurfural, furfural, glucose, xylose, vanillin and benzaldehyde, etc.). The research presented in this review covers a wide range of oxidation mechanisms for each aldehyde. It is evident from the current literature that challenges related to the comprehensiveness of mechanistic studies, catalyst stability, and reaction scalability remain, but the rapid progress offers hope for future advancements. Finally, we elucidate the challenges in this domain and provide the perspectives on future developments. This review corroborates the significance of investigating the electrocatalytic oxidation of biomass-derived aldehydes and emphasizes the need for continued research to refine these processes for industrial applications.
Electronic structure modulation of high entropy materials for advanced electrocatalysis
Luoluo Qi, Jingqi Guan
2025, 10(5): 917-936. doi: 10.1016/j.gee.2024.07.009
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High-entropy materials (HEMs) have managed to make their mark in the field of electrocatalysis. The flexibly adjustable component, unique configuration and proprietary core effect endow HEMs with excellent functional feature, superior stability and fast reaction kinetics. Recently, the relationship between the compositions and structures of high-entropy catalysts and their electrocatalytic performances has been extensively investigated. Based on this motivation, we comprehensively and systematically summarize HEMs, outline their intrinsic properties and electrochemical advantages, generalize current state-of-the-art synthetic methods, analyze electrochemical active centers in conjunction with characterization techniques, utilize theoretical research to conduct a high-throughput screening of the targeted high-entropy catalyst and the exploration of the reaction mechanisms, and importantly, focus specially on the electrochemical applications of high-entropy catalysts and propose strategies for regulating electronic structure to accelerate electrochemical reaction kinetics, including morphological control, defect engineering, element regulation, strain engineering and so forth. Finally, we provide our personal views on the challenges and further technical improvements of high-entropy catalysts. This work can provide valuable guidance for future research on high-entropy electrocatalysts.
Mechano-driven chemical reactions
Shaoxin Li, Jiajin Liu, Zhong Lin Wang, Di Wei
2025, 10(5): 937-966. doi: 10.1016/j.gee.2024.08.001
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Traditional chemical processes often generate substantial waste, leading to significant pollution of water, air, and soil. Developing eco-friendly chemical methods is crucial for economic and environmental sustainability. Mechano-driven chemistry, with its potential for material recyclability and minimal byproducts, is well-aligned with green chemistry principles. Despite its origins over 2000 years ago and nearly 200 years of scientific investigation, mechano-driven chemistry has not been widely implemented in practice. This is likely due to a lack of comprehensive understanding and the complex physical effects of mechanical forces, which challenge reaction efficiency and scalability. This review summarizes the historical development of mechano-driven chemistry and discusses its progress across various physical mechanisms, including mechanochemistry, tribochemistry, piezochemistry, and contact electrification (CE) chemistry. CE-induced chemical reactions, involving ion transfer, electron transfer, and radical generation, are detailed, emphasizing the dominant role of radicals initiated by electron transfer and the influence of ion transfer through electrical double layer (EDL) formation. Advancing efficient, eco-friendly, and controllable green chemical technologies can reduce reliance on traditional energy sources (such as electricity and heat) and toxic chemical reagents, fostering innovation in material synthesis, catalytic technologies, and establishing a new paradigm for broader chemical applications.
Research papers
Copper silicate nanoneedle arrays on reduced graphene oxide like “shelter forest” guiding Zn gradient deposition
Na Gao, Yang Wang, Zhanming Gao, Tianming Lv, Mengyu Rong, Xueying Dong, Dongzhi Chen, Changgong Meng, Yifu Zhang
2025, 10(5): 967-981. doi: 10.1016/j.gee.2024.07.004
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With the sustainable and efficient development of aqueous zinc ion batteries (AZIBs), the research on addressing the issues of the adaptability and durability of zinc anodes has been hot-topic and is still of great challenge. In this work, inspired by the sand treatment and afforestation of the Gobi Beach in Northwest China to ameliorate the problem of wind and sand encroachment, we propose a material with a morphology similar to that of a “shelter forest”, CuSiO3 nanoneedles arrays grown on both sides of reduced graphene oxide (rGO@CuSi), as a coating layer on the zinc metal surface to guide Zn gradient deposition. The presence of rGO improves the electrical conductivity of CuSiO3, and the finite element simulation of the electric field and Zn2+ concentration proves that the electric field distribution can be effectively homogenized and the local current density can be reduced for the rGO@CuSi-Zn electrode with the surface presenting the shape of a protective forest. This is due to the abundant pores between the nano-needle array structures on the surface of the electrode, which provide high electron and ion transport paths, and are conducive to achieving uniform Zn deposition, like the principle of wind-sand stabilization by protective forest. Both electrochemical experiments and density functional theory calculations show that the negatively charged surface of rGO@CuSi with good Zn affinity is more capable of guiding Zn2+ transport. Thanks to its inherent material and structural characteristics, the rGO@CuSi-Zn anode has a high specific capacity and good cycling stability. This study provides insight for interface engineering like protective forest to accelerate the commercialization of high-performance Zn-based batteries.
Lamellar COF solid-state electrolytes for robust ambient-temperature lithium-ion transfer enhanced by PEI-driven channel alignment
Yafang Zhang, Xinji Zhang, Jiajia Huang, Zhirong Yang, Shiyue Zhou, Chenye Wang, Wenjia Wu, Jingtao Wang
2025, 10(5): 982-993. doi: 10.1016/j.gee.2024.09.009
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Ionic covalent organic framework (COF) lamellar membranes are the alternative materials as promising Li+ conductors for all-solid-state lithium batteries. However, COF lamellar membrane suffers from poor structural stability and inevitable cross-layer transfer resistance due to the weak interaction at interface of adjacent nanosheets. Herein, a lamellar polymer-threaded ionic COF (PEI@TpPa-SO3Li) composite electrolyte with single Li+ conduction was prepared by assembling lithium sulfonated COF (TpPa-SO3Li) nanosheets and then threading them with polyethyleneimine (PEI) chains. It reveals that the threaded PEI chains induce the oriented permutation of pore channel of PEI@TpPa-SO3Li electrolyte through electrostatic interaction between -NH2/-NH- and -SO3Li groups. This enables the construction of continuous and aligned -SO3- … Li+ … -NH2/-NH- pairs along pore channels, which act as efficient Li+ conducting sites and afford high Li+ hopping conduction (1.4 × 10-4 S cm-1 at 30 °C) with a high Young's modulus of 408.7 MP and wide electrochemical stability window of 0~4.7 V. The assembled LiFePO4||Li and LiNi0.8Mn0.1Co0.1O2||Li half-cells achieve high discharge capacities of 155.0 mAh g-1 and 167.2 mAh g-1 at 30 °C under 0.2 C, respectively, with high capacity retention of 98% after 300 cycles. This study provides an alternative route to highly ion-conductive lamellar porous electrolytes for high-performance energy devices.
Solvent-free synthesis of highly dispersed zinc-doped porous carbons as efficient dibenzothiophene adsorbents
Ping Lu, Zhenhua Sun, Xinrong Ke, Changshen Ye, Zhixian Huang, Ting Qiu
2025, 10(5): 994-1001. doi: 10.1016/j.gee.2024.09.010
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Designing efficient adsorbents for the deep removal of refractory dibenzothiophene (DBT) from fuel oil is vital for addressing environmental issues such as acid rain. Herein, zinc gluconate and urea-derived porous carbons SF-ZnNC-T (T represents the carbonization temperature) were synthesized without solvents. Through a temperature-controlled process of “melting the zinc gluconate and urea mixture, forming H-bonded polymers, and carbonizing the polymers,” the optimal carbon, SF-ZnNC-900, was obtained with a large surface area (2280 m2 g-1), highly dispersed Zn sites, and hierarchical pore structures. Consequently, SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of 43.2 mg S g-1, compared to just 4.3 mg S g-1 for the precursor. It also demonstrated good reusability, fast adsorption rate, and the ability for ultra-deep desulfurization. The superior DBT adsorption performance resulted from the evaporation of residual zinc species, which generated abundant mesopores that facilitated DBT transformation, as well as the formation of Zn-N sites that strengthened the host-guest interaction (ΔE = -1.466 eV). The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents.
Study on the effect of controlled disproportionation pore-forming and relative vacuum mechanism on the reduction rate of continuous magnesium smelting process
Jing-zhong Xu, Ting-an Zhang, Yan Liu, Zhihe Dou, Yishan Liu, Baiao Feng, Hongxuan Liu
2025, 10(5): 1002-1014. doi: 10.1016/j.gee.2024.09.006
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Compared with the vacuum continuous magnesium smelting process (RVCMS), its excellent energy saving and emission reduction performance provides a feasible method for green magnesium smelting. In the process of industrialization, the reduction rate of prefabricated pellets affects the yield of metal magnesium and the utilization of reducing slag. In this paper, the reduction mechanism under different carbonate structures is analyzed by controlled disproportionation of prefabricated pellets and micro-nano simulation. The results show that the low temperature decomposition of NH4·HCO3 pore-forming, improve the reduction rate (99.72%) effect is remarkable. Combined with thermodynamics and relative vacuum mechanism, a theoretical model of the relationship between disproportionation pore-forming and reduction rate was established. It was concluded that the energy consumption required to produce per ton of magnesium by adding NH4·HCO3 to the prefabricated pellets was reduced by 0.29-0.34 tce, and the carbon emission was reduced by 1.069-1.263 t. The reduction slag had good compressive strength (Side 101.19 N cm-2, Bottom 466.4 N cm-2). Compared with the 20 MPa reduction slag sample without pore-forming agent, the side compressive strength increased by 51.66%, and the bottom compressive strength increased by 119.10%. The amount of single furnace filler is increased by more than 50%.
Coupling adsorption and in-situ Fenton-like oxidation by iron-containing low-grade attapulgite clay towards organic pollutant removal: From batch experiment to continuous operation
Chao Jiang, Xiaoli Liu, Xingpeng Wang, Qihui Wang, Huiyu Li, Weiliang Tian, Saeed Ahmed, Yongjun Feng
2025, 10(5): 1015-1026. doi: 10.1016/j.gee.2024.10.004
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Coupling adsorption and in-situ Fenton-like oxidation process was developed for Methylene blue (MB) using refined iron-containing low-grade attapulgite (ATP) clay, and the removal mechanism was investigated. The MB was initially adsorbed on the porous ATPs, and then the enriched MB was removed by the H2O2-assisted Fenton-like oxidation with the iron-containing ATP catalyst. Under optimal conditions, the ATP powder exhibits the maximum removal efficiency of 100% with negligible iron leaching (1.5 mg L-1) and no sludge formation. Furthermore, polysulfone/ATP (PSF/ATP) pellets were fabricated through a water-induced phase separation process to construct a fixed-bed reactor (FBR) for continuous contaminant removal. For the first cycle, the maximum adsorption capacity was 15.5 L with an outlet MB concentration of 1.973 mg L-1 (< 2 mg L-1, GB4287-2012) using the PSF/ATP pellets containing 50.0 g of ATP powders, and the maximum Fenton-like oxidation capacity was 35.5 L with the outlet concentration of 0.831 mg L-1. After five cycles, the total treated volume of the MB solution was ca. 255 L, and the efficiency remained above 99%. After 10 h of continuous treatment towards practical resin industrial wastewater, the chemical oxygen demand (COD) removal efficiency was still measured at 83.05%, costing 0.398 $ m-3. These results demonstrate the practical applicability of iron-containing low-grade ATP clay for textile water treatment.
Eco-friendly and facile nanomanufacturing of amorphous Co-Ce-Fe trimetallic molybdates composites for accelerated anodic oxygen evolution in alkaline water electrolysis: Evaluation of active sites performance
Jiejie Feng, Liling Wei, Huayi Li, Jianquan Shen
2025, 10(5): 1027-1038. doi: 10.1016/j.gee.2024.09.012
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Currently, endeavors to scale up the production of amorphous catalysts are still impeded by intricate synthesis conditions. Here, we have prepared a series of metal-based molybdate via one-step coprecipitation method. After ingredient optimization, amorphous Co2CeFe2-MoO4 was identified as exhibiting the highest intrinsic activity among its counterparts. Modulation of electron structure enables Co2CeFe2-MoO4 to balance the adsorption behavior towards reactive intermediates. Ultimately, the obtained Co2CeFe2-MoO4 molybdate demonstrated a captivating OER performance, showcasing a low overpotential of 230 mV at 10 mA cm-2. Moreover, the alkaline electrolyzer employing the Co2CeFe2-MoO4 anode exhibited a low cell voltage of 1.50 V for water splitting and underwent an acceptable attenuation of 4.99% after 165 h of continuous operation, demonstrating its favorable catalytic activity and durability. This work provides a facile and eco-friendly synthesis pathway for crafting cost-effective and durable earth-abundant OER electrocatalysts tailored for water splitting to produce clean hydrogen.
Dual-bonded polyethyleneimine network with electron-withdrawing groups at α, β-sites for ultra-stable and low-energy CO2 capture in harsh environments
Tong Zhou, Yunxia Wen, Zhinan Wu, Shuailong Song, Bohong Wu, Hongwei Guo, Huanhao Chen, Xin Feng, Liwen Mu, Xiaohua Lu, Tuo Ji, Jiahua Zhu
2025, 10(5): 1039-1049. doi: 10.1016/j.gee.2024.10.005
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As an innovative approach to addressing climate change, significant efforts have been dedicated to the development of amine sorbents for CO2 capture. However, the high energy requirements and limited lifespan of these sorbents, such as oxidative and water stability, pose significant challenges to their widespread commercial adoption. Moreover, the understanding of the relationship between adsorption energy and adsorption sites is not known. In this work, a dual-bond strategy was used to create novel secondary amine structures by a polyethyleneimine (PEI) network with electron-extracted (EE) amine sites at adjacent sites, thereby weakening the CO2 binding energy while maintaining the binding ability. In-situ FT-IR and DFT demonstrated the oxygen-containing functional groups adjacent to the amino group withdraw electrons from the N atom, thereby reducing the CO2 adsorption capacity of the secondary amine, resulting in lower regeneration energy consumption of 1.39 GJ t-1-CO2. In addition, the EE sorbents demonstrated remarkable performance with retention of over 90% of their working capacity after 100 cycles, even under harsh conditions containing 10% O2 and 20% H2O. DFT calculations were employed to clarify for the first time the mechanism that the oxygen functional group at the α-site hinders the formation of the urea structure, thereby being an antioxidant. These findings highlight the promising potential of such sorbents for deployment in various CO2 emission scenarios, irrespective of environmental conditions.
Cooperative α-C-H activation enabled quantitative and partial photooxidation of biomass-derived 5-hydroxymethylfurfural
Jie Li, Ye Meng, Yu Wen, Yinyin He, Putla Sudarsanam, Song Yang, Hu Li
2025, 10(5): 1050-1063. doi: 10.1016/j.gee.2024.11.004
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Photocatalytic activation of C-H bonds is versatile but challenging for undergoing oriented conversion processes. Herein, a spatially site-isolated heterojunction (ZS-Vs/ZIS) of ZnIn2S4 with strong Lewis acidity (ZIS) and ZnS with S-vacancy (ZS-Vs) is constructed for activating α-C-H bond and forming ·O2- to cleave the C-H bond, respectively. ZS-Vs/ZIS displays outstanding performance in visible-light partial photooxidation of bio-based 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) in an unprecedented yield of 95.7% at 25 °C. In-situ experiments and calculations reveal that Zn sites of ZIS serve as hole enrichment to adsorb HMF for α-C-H activation via ligand-to-metal charge transfer. Shallow trap states introduced by S-vacancy in ZS-Vs act as an electron pool to realize directed O2 activation into ·O2- for breaking pre-activated α-C-H bond in HMF to exclusively give DFF. Moreover, ZS-Vs/ZIS has good recyclability and universality in the photooxidation of various alcohols to carbonyls (86.4-95.6% yields). The synergistic C-H activation/breaking strategy exhibits high potential in targeted photocatalytic transformations.
Biomass-derived single atom catalysts with phosphorus-coordinated Fe-N3P configuration for efficient oxygen reduction reaction
Peng-Peng Guo, Abrar Qadir, Chao Xu, Kun-Zu Yang, Yong-Zhi Su, Xin Liu, Ping-Jie Wei, Qinggang He, Jin-Gang Liu
2025, 10(5): 1064-1072. doi: 10.1016/j.gee.2024.11.002
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Exploiting non-precious metal catalysts with excellent oxygen reduction reaction (ORR) performance for energy devices is paramount essential for the green and sustainable society development. Herein, low-cost, high-performance biomass-derived ORR catalysts with an asymmetric Fe-N3P configuration was prepared by a simple pyrolysis-etching technique, where carboxymethyl cellulose (CMC) was used as the carbon source, urea and 1,10-phenanthroline iron complex (FePhen) as additives, and Na3PO4 as the phosphorus dopant and a pore-forming agent. The CMC-derived FeNPC catalyst displayed a large specific area (BET: 1235 m2 g-1) with atomically dispersed Fe-N3P active sites, which exhibited superior ORR activity and stability in alkaline solution (E1/2 = 0.90 V vs. RHE) and Zn-air batteries (Pmax = 149 mW cm-2) to commercial Pt/C catalyst (E1/2 = 0.87 V, Pmax = 118 mW cm-2) under similar experimental conditions. This work provides a feasible and cost-effective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
Boosting charge transfer of BiOBr/AgBr S-scheme heterojunctions via interface Br atom co-sharing for enhanced visible-light photocatalytic activity
Junhao Ma, Liang Xu, Zhaoyi Yin, Zhifeng Li, Zhiguo Song, Jianbei Qiu, Yongjin Li
2025, 10(5): 1073-1084. doi: 10.1016/j.gee.2024.11.003
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Efficient interfacial charge transfer and robust interfacial interactions are crucial for achieving the superior spatial separation of carriers and developing efficient heterojunction photocatalysts. Herein, BiOBr/AgBr S-scheme heterojunctions are synthesized via the co-sharing of Br atoms using an ion-exchange approach, which involves the in-situ growth of AgBr nanoparticles on the surfaces of BiOBr nanosheets. It is revealed that successful construction of a high-quality interface with strong interactions via Br atom bridge between BiOBr and AgBr, which provided a rapid migration channel for charge carriers. In addition, in-situ XPS, Kelvin probe force microscopy, and electron spin resonance evaluations confirmed the establishment of an S-scheme charge-transfer pathway in this tightly contacted heterojunction, which could efficiently prevent the recombination of photogenerated carriers while retaining carriers with a high redox capacity. Finally, the photocatalytic test confirmed that the BiOBr/AgBr heterojunction showed excellent photocatalytic performance and wide applicability thanks to the construction of high quality heterojunction. Overall, this work highlights the importance of rational designing of heterogeneous interfaces at the atomic level in photocatalysis, and contributes to rationally design BiOBr-based S-scheme heterojunctions photocatalytic materials with high quality atomic co-sharing interfaces.
Regulating WOx coordination environment improves proton transfer for catalytic amine regeneration in CO2 capture
Zanbu Geng, Yang Yang, Wenqing Xu, Yixi Wang, Yiren Li, Chaoqun Li, Juan Liu, Tingyu Zhu
2025, 10(5): 1085-1095. doi: 10.1016/j.gee.2024.12.002
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Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO2 capture technologies. However, the intrinsic relationship between the properties of the acidic sites and their catalytic activity is controversial. In this study, a series of W-based catalysts supported by ZrTiOx were synthesised, and the effects of the intensity, distribution, and type of acid sites were systematically investigated by quantitatively regulating the acidic site properties. The results indicate stronger acidic sites play a more important role in the catalytic reaction. Moreover, the catalysts showed excellent performance only if the Brønsted acid sites (BASs) and Lewis acid sites (LASs) coexisted. During the catalytic reaction, the BASs facilitated deprotonation, and the LASs promoted the decomposition of carbamates. The ratio of BASs to LASs (B/L) was a critical factor for catalytic activity, wherein optimal performance was achieved when the B/L ratio was close to 1. The 10% HPW/ZrTiOx composite performed better than WO3/ZrTiOx and HSiW/ZrTiOx because it had a stronger acid intensity and a suitable B/L ratio. As a result, the relative heat duty was reduced by 47% compared to 30% aqueous MEA, and the maximum CO2 desorption rate was increased by 83%. The Bader charge indicated that the W atoms of HPW/ZrTiOx lost more electrons (0.18) than those of WO3/ZrTiOx, which can weaken the O-H bond energy. Consequently, the calculated deprotonation energy is as low as 257 kJ mol-1 for HPW/ZrTiOx.

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