ACS Sustainable Chemistry & Engineering最新文献

Coordinated Metabolic Strategies for Green and Efficient Orotic Acid Biomanufacturing in Escherichia coli 大肠杆菌绿色高效生物制造的协调代谢策略

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-21 DOI: 10.1021/acssuschemeng.6c08632

Changgeng Li,Runze Zhao,Ruihong Liu,Wenjing Fan,Tang'en Shi,Siyu Zhao,Ling Ma,Zichen Yu,Zhichao Chen,Haibo Xiong,Xin Liang,Qingyang Xu

{"title":"Coordinated Metabolic Strategies for Green and Efficient Orotic Acid Biomanufacturing in Escherichia coli","authors":"Changgeng Li,Runze Zhao,Ruihong Liu,Wenjing Fan,Tang'en Shi,Siyu Zhao,Ling Ma,Zichen Yu,Zhichao Chen,Haibo Xiong,Xin Liang,Qingyang Xu","doi":"10.1021/acssuschemeng.6c08632","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c08632","url":null,"abstract":"Orotic acid (OA) is an intermediate in de novo pyrimidine biosynthesis and a bio-based chemical of interest for nutraceutical, animal nutrition, and biomedical applications. Efficient fermentative OA production, however, remains constrained by carbon loss, insufficient nitrogen assimilation, product-associated stress, and energy-redox imbalance during high-titer production. This study constructed a high-performance Escherichia coli cell factory by coordinating product transport, carbon-nitrogen flux, and energy-redox metabolism. Deletion of the inward OA transporter dctA improved extracellular OA accumulation, while the introduction of a nonoxidative glycolysis (NOG) module, acetyl-phosphate recycling, and byproduct-pathway attenuation reduced overflow carbon loss. Nitrogen assimilation was strengthened by tuning heterologous ammonium transport and balancing NADPH supply. Adenylate metabolism reconstruction and microaerobically responsive expression of vgb and cyoABCDE increased intracellular ATP levels and promoted the NADH/NAD+ redox balance, supporting OA biosynthesis during mid-to-late-stage fed-batch fermentation. OA24 produced 214.2 g/L OA in 42 h in a 5-L bioreactor, with an apparent glucose-based yield of 0.70 g/g glucose and productivity of 5.10 g/L/h; relative to the initial strain Ora21, the yield and productivity increased by 20.7% and 34.2%, respectively. This work provides a carbon-efficient and high-intensity biomanufacturing strategy for OA and related pyrimidine chemicals.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"3 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineering Fe Species on USY Zeolite Support for the Oxidative Cleavage of Lignin to Bio-Based Diethyl Maleate 工程铁在USY沸石上支持木质素氧化裂解生成生物基马来酸二乙酯

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-21 DOI: 10.1021/acssuschemeng.6c08496

Rujia Chen,Kejia Wu,Xiudan Zhao,Yun Tian,Zhenping Cai,Jinrong Liang,Weilu Ding,Wentao Mu,Xuehui Li

{"title":"Engineering Fe Species on USY Zeolite Support for the Oxidative Cleavage of Lignin to Bio-Based Diethyl Maleate","authors":"Rujia Chen,Kejia Wu,Xiudan Zhao,Yun Tian,Zhenping Cai,Jinrong Liang,Weilu Ding,Wentao Mu,Xuehui Li","doi":"10.1021/acssuschemeng.6c08496","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c08496","url":null,"abstract":"The development of sustainable routes for polymer monomers is crucial for the chemical industry. Herein, we report a highly efficient and selective oxidative depolymerization strategy for converting lignin into diethyl maleate (DEM), a valuable precursor for polyaspartic polyurea resins. A series of iron oxide catalysts supported on commercial USY zeolites via a simple impregnation-calcination method were developed. Notably, the catalyst prepared using iron sulfate (Fe2(SO4)3) as the precursor exhibited superior performance, achieving a maximum DEM yield of 53.0 wt % and a selectivity of 72.4% from organosolv bagasse lignin, outperforming the iron nitrate- and chloride-derived catalysts by 29.2 and 31.9 wt % in yield, respectively. Comprehensive characterizations revealed that the unique highly dispersed Fe(SO4)x phases significantly increased the proportion of Fe3+ species and facilitated electron transfer across the support-iron interface. The synergistic interplay between sulfur-induced Brønsted acid sites and isolated octahedral iron sites was identified as the key factor driving the efficient cleavage of lignin linkages and subsequent oxidative ring-opening. By combining commercially available supports and earth-abundant metals, this work offers an environmentally viable pathway for lignin depolymerization into polymer monomers, demonstrating significant potential for industrial scalability.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"73 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

One-Pot Green Synthesis of Low-Viscosity Acetal Epoxy Resins for Diluent-Free Industrial Processing and Closed-Loop Recycling of Carbon Fiber Composites 一锅绿色合成低粘度缩醛环氧树脂，用于碳纤维复合材料的无稀释工业加工和闭环回收

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-21 DOI: 10.1021/acssuschemeng.6c09509

Dehang Yang,Shuai Du,Shanshan Dai,Fengyuan Zhang,Songqi Ma

{"title":"One-Pot Green Synthesis of Low-Viscosity Acetal Epoxy Resins for Diluent-Free Industrial Processing and Closed-Loop Recycling of Carbon Fiber Composites","authors":"Dehang Yang,Shuai Du,Shanshan Dai,Fengyuan Zhang,Songqi Ma","doi":"10.1021/acssuschemeng.6c09509","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c09509","url":null,"abstract":"Recyclable epoxy thermosets and their carbon fiber-reinforced polymer composites (CFRPs) have faced three long-standing bottlenecks: complex synthesis and purification processes, inherently high viscosity incompatible with the industrial vacuum-assisted resin infusion (VARI) process—the dominant technology for manufacturing large wind turbine blades and aerospace composites—and incomplete recovery of individual composite constituents. While dynamic covalent bonds offer a promising route to epoxy recyclability, most existing recyclable epoxy systems fail to simultaneously overcome these hurdles. Herein, we report a green, scalable one-pot synthesis of a novel low-viscosity acetal epoxy resin (BCAE) that simultaneously addresses the synthesis, processing, and end-of-life recycling challenges of epoxy thermosets. This telescoped protocol eliminates intermediate purification steps, delivering BCAE with an ultra-low viscosity of 1.9 Pa·s at 25 °C—6.7-fold lower than commercial bisphenol A diglycidyl ether (DGEBA)—enabling diluent-free VARI fabrication of high-performance CFRPs. The cured BCAE networks exhibit dual recyclability: catalyst-free thermal reprocessability and mild acid-triggered degradation under ambient conditions. Most notably, we demonstrate a closed-loop monomer recycling combined with an open-loop upcycling system with key quantitative breakthroughs: carbon fibers are recovered with 96.7% strength retention in the regenerated composite, the benzaldehyde monomer is recycled to resynthesize BCAE with identical performance, and the tertiary amine polyol degradation product is upcycled as a high-value curing agent for commercial epoxies. Life cycle assessment confirms that closed‑loop recycling reduces CO2‑equivalent emissions by approximately 79% compared with incineration. This work provides a general and industrially viable strategy for sustainable thermoset composites, aligning perfectly with global carbon neutrality goals.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"63 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221781","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Engineering Self-Woven Hierarchical Bimetallic Nitride Electrode with Built-In Interfacial Electric Field for Enhanced Alkaline Hydrogen Evolution 内置界面电场的工程自编织分层氮化双金属电极增强碱性析氢

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-20 DOI: 10.1021/acssuschemeng.6c04554

Wubin Wan,Xuejing Yang,Tianguo Wang,Cheng Luo,Chuitao Zeng,Xingxing Zhu,Xingyou Lang

{"title":"Engineering Self-Woven Hierarchical Bimetallic Nitride Electrode with Built-In Interfacial Electric Field for Enhanced Alkaline Hydrogen Evolution","authors":"Wubin Wan,Xuejing Yang,Tianguo Wang,Cheng Luo,Chuitao Zeng,Xingxing Zhu,Xingyou Lang","doi":"10.1021/acssuschemeng.6c04554","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c04554","url":null,"abstract":"Single-phase transition metal nitrides (TMNs) for alkaline hydrogen evolution reaction (HER) are limited by sluggish charge transfer kinetics, suboptimal adsorption, and restricted accessibility of active sites—intrinsic drawbacks of their electronic structure and conventional electrode architecture. Herein, we circumvent these obstacles by constructing a Ni4N/CoN heterostructure on nickel foam (Ni4N/CoN/NF) with two synergistic features: a built-in interfacial electric field (BIEF) and a hierarchical porous morphology. The work function difference between Ni4N and CoN generates a robust BIEF that drives directional electron transfer from Ni to Co, precisely tailoring the electronic configuration of Ni sites to optimize adsorption energy. Moreover, this hierarchical architecture, assembled from interconnected nanochains and nanosheets, simultaneously enhances active-site exposure, facilitates electron transport, and promotes efficient gas release. Benefiting from these synergistic advantages, the Ni4N/CoN electrode delivers an industrial-level current density of 1000 mA cm–2 at an overpotential of only 213 mV in alkaline media. Moreover, the combination of its robust interwoven nanochain architecture and strong interfacial electronic coupling endows the electrode with outstanding operational stability, sustaining continuous hydrogen evolution for over 500 h at the current density of 500 mA cm–2. This work presents a viable strategy for designing efficient and durable heterostructure electrocatalysts toward practical water electrolysis.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"15 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218813","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Breaking Solvent Constraints Enables Sustainable Nanoscale Chemical Synthesis by Acoustic Droplet Ejection 突破溶剂限制，通过声滴喷射实现可持续的纳米级化学合成

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-20 DOI: 10.1021/acssuschemeng.6c07249

Emis Ingenito,Alexander Dömling

{"title":"Breaking Solvent Constraints Enables Sustainable Nanoscale Chemical Synthesis by Acoustic Droplet Ejection","authors":"Emis Ingenito,Alexander Dömling","doi":"10.1021/acssuschemeng.6c07249","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c07249","url":null,"abstract":"Miniaturized chemical synthesis through acoustic droplet ejection (ADE) is transforming reaction discovery by reducing material consumption and enabling highly parallelized, autonomous workflows. However, its application in organic synthesis has remained largely confined to DMSO and aqueous media, restricting solvent exploration and limiting broader process innovation. Often attributed to the intrinsic physics of acoustic transfer, these constraints may instead reflect historical calibration practices. Here, we establish a data-driven framework for expanding ADE-compatible solvent space toward a more applicable nanoscale reaction chemistry. Through systematic gravimetric analysis of 19 high-boiling organic solvents, including water and DMSO as reference fluids, we identify a broad operating window that supports accurate (deviation < 10%) and reproducible (RSD < 8%) dispensing using existing instrumentation. We further validate this framework via automated assembly of a 384-member Suzuki–Miyaura reaction library, where testing of N,N-dimethylformamide and a bio-based alternative solvent dimethyl isosorbide resulted in broad product formation across diverse substrates. This work decouples solvent choice from historical conventions and opens the route to a reaction-agnostic, solvent-flexible, and sustainable approach for high-throughput reaction discovery, enabling ADE workflows to transition from condition-constrained screening tools to general engines for sustainable, data-driven chemical exploration.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"56 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Fast Preparation of Ultratough Cellulose Aerogel Fibers via One-Step Composite Solvent Exchange under Ambient Pressure Drying 常压干燥下一步复合溶剂交换快速制备超韧纤维素气凝胶纤维

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-20 DOI: 10.1021/acssuschemeng.6c10206

Shasha Liu,Jingjing Yuan,Ling Nie,Zishan Xiong,Zhihao Zhao,Xinrui Hao,Xiong Qian,Jinfeng Wang,Weilin Xu,Kunkun Zhu

{"title":"Fast Preparation of Ultratough Cellulose Aerogel Fibers via One-Step Composite Solvent Exchange under Ambient Pressure Drying","authors":"Shasha Liu,Jingjing Yuan,Ling Nie,Zishan Xiong,Zhihao Zhao,Xinrui Hao,Xiong Qian,Jinfeng Wang,Weilin Xu,Kunkun Zhu","doi":"10.1021/acssuschemeng.6c10206","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c10206","url":null,"abstract":"Traditional ambient-pressure drying of aerogels relies on minimizing capillary shrinkage to preserve nanoporous structures, yet this strategy inevitably compromises either processing efficiency or mechanical robustness. Here, we show that capillary shrinkage can instead be exploited as a controllable structural reconstruction process. Through a rapid composite solvent exchange strategy, effective solvent exchange is achieved within only 10 min, enabling regulated capillary stress to drive network rearrangement and pore-wall reinforcement during ambient-pressure drying while preserving an interconnected nanoporous architecture. The resulting cellulose aerogel fibers exhibit a density of 0.10 g·cm–3, an areal porosity of 82.15%, and a specific surface area of 90.67 m2·g–1, together with a tensile strength of 29.46 MPa and a toughness of 10.05 MJ·m–3, representing strength improvements of 135.1% and 280.6% over freeze-dried and supercritical-dried counterparts, respectively. Despite moderate network densification, the aerogel fabric maintains excellent thermal insulation, with a room-temperature thermal conductivity of 0.037 W·m–1·K–1, producing a temperature difference of 27.7 °C on a 100 °C hot plate. Our results establish controlled capillary reconstruction as a scalable structural engineering strategy for manufacturing mechanically robust nanoporous materials through ambient-pressure drying.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"13 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221759","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Melt-Spun FeCrNiMoC0.3 High-Entropy Alloy Ribbons: Microstructure Refinement for Enhanced Bifunctional Alkaline Overall Water Splitting 熔体纺丝fecrnimo0.3高熵合金带：增强双功能碱性整体水分解的微观结构改进

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-20 DOI: 10.1021/acssuschemeng.6c07043

Tong Zhang,Guanglong Li,Zhen Wen,Wei Zhang,Shulin Dong,Siruo Zhang,Yingdong Qu

{"title":"Melt-Spun FeCrNiMoC0.3 High-Entropy Alloy Ribbons: Microstructure Refinement for Enhanced Bifunctional Alkaline Overall Water Splitting","authors":"Tong Zhang,Guanglong Li,Zhen Wen,Wei Zhang,Shulin Dong,Siruo Zhang,Yingdong Qu","doi":"10.1021/acssuschemeng.6c07043","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c07043","url":null,"abstract":"Alkaline water electrolysis urgently requires scalable, binder-free integrated bulk electrodes with high activity and robust stability at high current densities. High-entropy alloys (HEAs) are promising candidates for such electrodes, but conventional as-cast HEAs generally suffer from coarse grains, which limits their electrocatalytic performance. Herein, FeCrNiMoC0.3 HEA ribbons were fabricated as integrated electrocatalysts via melt-spinning rapid solidification. This metallurgical treatment refines matrix grains to an average size of 135.7 nm, uniformly disperses nanoscale carbides, induces FCC lattice expansion, and drives directional charge transfer from Fe/Cr/Ni to Mo without altering the phase composition. In 1.0 M KOH, the melt-spun ribbons (MSRs) exhibit enhanced bifunctional electrocatalytic performance. At 10 mA cm–2, the MSR electrode delivers overpotentials of 218 mV for the oxygen evolution reaction (OER) and 81 mV for the hydrogen evolution reaction (HER), with Tafel slopes of 30.8 and 55.4 mV dec–1, respectively. The two-electrode overall water splitting achieves 500 mA cm–2 at 2.03 V and runs stably for over 500 h. Grain and carbide refinement, accompanied by electronic modulation, an enlarged electrochemically active surface area, and reduced charge transfer resistance, collectively accounts for the enhanced performance. This work provides a facile and scalable metallurgical strategy to optimize carbide-containing binder-free bulk HEAs and offers a reference for understanding the microstructure–activity relationship of bulk alloy electrodes for alkaline water electrolysis.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"14 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Macroscopic-to-Atomic Mechanism of Zinc Effects on CaO Carbonation 锌对CaO碳酸化的宏观-原子机理研究

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-20 DOI: 10.1021/acssuschemeng.6c09525

Mingqian Yang,Bo Xu,Yue Wang,Yaolin Yi

{"title":"Macroscopic-to-Atomic Mechanism of Zinc Effects on CaO Carbonation","authors":"Mingqian Yang,Bo Xu,Yue Wang,Yaolin Yi","doi":"10.1021/acssuschemeng.6c09525","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c09525","url":null,"abstract":"CaO-based materials are promising sorbents for CO2 capture and represent the dominant reactive phase in Ca-rich alkaline industrial residues. Zinc is one of the most common metal impurities in CaO-based sorbents, yet its influence on the carbonation behavior of CaO remains less understood. Thus, this study investigates the effect of Zn (0–50,000 mg·kg–1) on CaO carbonation, combining phase evolution, structure–property relationships, surface chemistry, carbonate distribution, and density functional theory calculations, to establish a mechanistic framework linking atomic-scale CO2 activation to macroscopic carbonation behavior. Results showed that increasing Zn concentration progressively suppressed the carbonation reactivity of CaO. The CO2 uptake decreased from 0.528 to 0.478 gCO2·gsorbent–1 at 120 min, corresponding to a 9.4% reduction, while the initial carbonation during the chemically controlled stage was inhibited by approximately 30%. At a high Zn concentration (50,000 mg·kg–1), calcium zincate hydrate and zinc hydroxycarbonate formed, and carbonate crystallization shifted from continuous surface precipitation to discontinuous crystal growth, producing fewer but coarser carbonate crystallites. Zn delayed the hydroxyl-to-carbonate interfacial transformation and produced spatially heterogeneous carbonation domains. The weakened interaction between surface O 2p states and CO2-derived C 2p states reduced the electronic coupling at the adsorption interface and lowered the thermodynamic stability of adsorbed CO2. Thus, Zn-affected CaO carbonation through Zn-bearing secondary-phase formation, pore-network reconstruction, spatially heterogeneous interfacial conversion, and local electronic perturbation. This study provides mechanistic insights into Zn-affected gas–solid reactions and a theoretical basis for evaluating Zn-contaminated Ca-rich industrial residues for CO2 capture.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"73 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149221758","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dual Metal-Active Phase for Significantly Enhanced Nitrate-to-Ammonia Electrocatalysis from Dynamic Reconstruction of a CuCo-Based Catalyst cu基催化剂动态重构显著增强硝酸盐制氨电催化的双金属活性相

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-20 DOI: 10.1021/acssuschemeng.6c08592

Li Deng,Jinfeng Li,Dongming Wang,Ruikai Qi,Siqi Zhang,Mingbin Gao,Xiaofeng Lu

{"title":"Dual Metal-Active Phase for Significantly Enhanced Nitrate-to-Ammonia Electrocatalysis from Dynamic Reconstruction of a CuCo-Based Catalyst","authors":"Li Deng,Jinfeng Li,Dongming Wang,Ruikai Qi,Siqi Zhang,Mingbin Gao,Xiaofeng Lu","doi":"10.1021/acssuschemeng.6c08592","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c08592","url":null,"abstract":"Electrochemical transformation of nitrate (NO3–) into ammonia (NH3) offers an environmentally sustainable pathway to complete the nitrogen cycle, enabling both green NH3 synthesis and NO3– pollution remediation. Herein, we propose an in situ synergistic reconstruction strategy for fabricating a Cu2O@Co-carbon nanofibers (CNFs) pre-electrocatalyst, integrated with the glycerol oxidation reaction (GOR) to replace the energy-intensive oxygen evolution reaction (OER), thereby significantly reducing energy consumption toward electrocatalytic NO3–-to-NH3 conversion. The potential-dependent reconstruction gives rise to coexisting Co0 and Co(OH)2 species together with active Cu sites. Electrochemical measurements and density functional theory (DFT) calculations support their complementary roles in *H generation and NO3– activation, respectively, thereby promoting the NO3RR while suppressing competing reactions. The resulting catalyst delivers an exceptional NH3 yield rate of 61.0 mg cm–2 h–1 at industrial-level current density, manifesting outstanding catalytic performance. This study offers a novel design principle and a reliable strategy for developing high-efficiency non-noble-metal-based bifunctional electrocatalysts and advanced coupled electrochemical systems.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"413 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218814","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Regulation of Lattice Oxygen and Phase Transition in O3-Type High-Entropy Layered Sodium-Ion Cathodes o3型高熵层状钠离子阴极中晶格氧和相变的调控

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-20 DOI: 10.1021/acssuschemeng.6c05438

Ruyi Liu,Ziyao Zhao,Xinwang Niu,Xuyang Zhao,Shuhan Zhu,Fan Bu,Zongyu Guan,Guoyao Pang,Feixiang Ding,Xin Xia,Feng Ye,Biwei Xiao,Chao Xu

{"title":"Regulation of Lattice Oxygen and Phase Transition in O3-Type High-Entropy Layered Sodium-Ion Cathodes","authors":"Ruyi Liu,Ziyao Zhao,Xinwang Niu,Xuyang Zhao,Shuhan Zhu,Fan Bu,Zongyu Guan,Guoyao Pang,Feixiang Ding,Xin Xia,Feng Ye,Biwei Xiao,Chao Xu","doi":"10.1021/acssuschemeng.6c05438","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c05438","url":null,"abstract":"Irreversible phase transition and lattice-oxygen loss above 4.0 V cause rapid capacity decay in high-capacity O3-type layered cathodes for sodium-ion batteries (SIBs). Herein, a novel high-entropy layered cathode of Na0.95Li0.05Ni0.3Fe0.1Mn0.3Zn0.05Ti0.2O2 (LNFMZT) with regulated lattice oxygen through a high-entropy configuration and multi-element compositional regulation is successfully synthesized by a high-temperature solid-state method. We show that high-entropy modification stabilizes the single-phase structure, expands Na+ diffusion pathways, and optimizes the transition-metal (TM)–O coordination environment. The LNFMZT delivers a high initial capacity (163.7 mAh g–1 at 0.1 C) and good cycling stability (64.0% retention over 250 cycles at 1 C) at a high-voltage window of 2.0–4.2 V. Combining in situ and ex situ experimental characterizations, we find that a high-entropy layered cathode exhibits reduced charge-transfer resistance, enhanced Na+ diffusion dynamics, good reversibility of lattice oxygen redox, and smoother O3-P3-OP2 evolution, which greatly improve the structural integrity and electrochemical durability. This work underscores the critical role of high-entropy modification in coupling lattice oxygen stability with phase transition reversibility for advanced SIB cathodes.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"42 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149218812","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0