ACS Sustainable Chemistry & Engineering最新文献_第9页

Chemoselective Synthesis of Hydrocinnamaldehyde Enabled by a Self-Sufficient Heterogeneous Redox Biocatalyst 非均相氧化还原生物催化剂催化氢肉桂醛的化学选择性合成

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c05935

Agostina Colacicco,Idania L. López,Martina Bigliardi,Ainhoa Oliden-Sánchez,Fernando López-Gallego,Martina L. Contente

{"title":"Chemoselective Synthesis of Hydrocinnamaldehyde Enabled by a Self-Sufficient Heterogeneous Redox Biocatalyst","authors":"Agostina Colacicco,Idania L. López,Martina Bigliardi,Ainhoa Oliden-Sánchez,Fernando López-Gallego,Martina L. Contente","doi":"10.1021/acssuschemeng.6c05935","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c05935","url":null,"abstract":"Abstract The selective C═C bioreduction of cinnamaldehyde to hydrocinnamaldehyde is a key transformation for the fragrance, pharmaceutical, and polymer industries, but remains challenging with conventional metal catalysts. Here, we report a self-sufficient heterogeneous biocatalyst (ssHB) combining an extremophilic ene-reductase from Halomonas elongata (HeNRed) with a thermostable glucose dehydrogenase from Bacillus subtilis (BsGDH) for in situ nicotinamide adenine dinucleotide (NADH) regeneration. A consensus coimmobilization protocol was identified by microtiter plate screening, where both enzymes were reversibly coimmobilized on macroporous agarose supports activated with positively charged diethylaminoethyl (DEAE) groups. The same support also enabled NADH coimmobilization, allowing cinnamaldehyde bioreduction without exogenous cofactor supply. The resulting ssHB was thoroughly characterized and implemented in a plug-flow packed-bed reactor (PBR), enabling &gt;90% conversion of cinnamaldehyde to hydrocinnamaldehyde under continuous flow with a 30 min residence time in the presence of 50% toluene as a cosolvent. The PBR operated continuously for 12 reactor cycles without exogenous supply of NADH before exhaustion. Translating this self-sufficient system from batch to continuous flow increased volumetric productivity 55-fold, reaching a space-time yield of 12.1 g L–1 h–1. The system also enabled full recovery of enzyme activity through streamlined reloading with fresh NADH. This work demonstrates how enzyme immobilization, cofactor recycling, and reaction intensification can be integrated into a scalable and sustainable platform for valorizing renewable feedstocks in green chemical manufacturing.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"19 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209545","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

Interfacial Microenvironment Engineering of Carbon-Doped Carbon Nitride-Wrapped SnO2 Nanofibers for Efficient Overall Photocatalytic H2O2 Production 碳掺杂氮化碳包覆SnO2纳米纤维的界面微环境工程研究

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c07470

Yuan Lin,Pengjia Li,Ziying Feng,Huanhuan Li,Yunyun Gui,Linghao Yu,Shao-Chuan Li,Junhua Zou,Lijun Liu

{"title":"Interfacial Microenvironment Engineering of Carbon-Doped Carbon Nitride-Wrapped SnO2 Nanofibers for Efficient Overall Photocatalytic H2O2 Production","authors":"Yuan Lin,Pengjia Li,Ziying Feng,Huanhuan Li,Yunyun Gui,Linghao Yu,Shao-Chuan Li,Junhua Zou,Lijun Liu","doi":"10.1021/acssuschemeng.6c07470","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c07470","url":null,"abstract":"Abstract Photocatalytic H2O2 production offers a sustainable alternative to the energy-intensive anthraquinone process, yet its efficiency is limited by rapid charge recombination, sluggish oxygen activation, and mismatched interfacial environments. Herein, a hierarchical heterostructure of carbon-doped carbon nitride nanosheets tightly wrapped on SnO2 nanofibers (C-PCN/SnO2) is constructed via one-step calcination of electrospun Sn2+-containing polyvinylpyrrolidone (PVP) nanofibers mixed with bulk carbon nitride precursor, during which Sn-PVP converts to SnO2 nanofibers while PVP decomposition simultaneously induces in situ exfoliation of bulk carbon nitride and carbon self-doping, forming a closely contacted heterojunction. Experimental and theoretical results reveal that the built-in electric field at the heterointerface drives S-scheme charge separation, preserving highly reductive electrons and oxidative holes. Notably, C-PCN serves as an efficient oxygen adsorption and activation domain, whereas hydrophilic SnO2 facilitates water-involved oxidation, jointly optimizing the interfacial reaction microenvironment. Benefiting from this synergy, the optimized heterojunction achieves a H2O2 production rate of 31.09 μM h–1 under visible light without sacrificial agents or cocatalysts, 7.6 and 12.5 times higher than C-PCN and SnO2, respectively. This work provides a new insight into reaction microenvironment engineering for efficient solar-driven H2O2 production.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"135 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209547","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

Engineered Antiperovsksite Nitride for Boosting Electrocatalytic Green Hydrogen Production 促进电催化绿色制氢的工程反钙钛矿氮化物

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c05997

Yufeng Qian,Lanli Chen,Jinglei Wang,Muhammad Humayun,Lu Zhang,Huaming Zhang,Yuxiao Liu,Junhong Duan,Quanshui Zhu,Mohamed Bououdina,Mohammad Reza Naimi Jamal,Yanwei Wang,Chundong Wang

{"title":"Engineered Antiperovsksite Nitride for Boosting Electrocatalytic Green Hydrogen Production","authors":"Yufeng Qian,Lanli Chen,Jinglei Wang,Muhammad Humayun,Lu Zhang,Huaming Zhang,Yuxiao Liu,Junhong Duan,Quanshui Zhu,Mohamed Bououdina,Mohammad Reza Naimi Jamal,Yanwei Wang,Chundong Wang","doi":"10.1021/acssuschemeng.6c05997","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c05997","url":null,"abstract":"Abstract Developing efficient and robust electrocatalysts for overall water splitting is vital for sustainable green hydrogen production, yet it remains a formidable challenge. In this work, a robust Mo-doped FeNNi3 antiperovskite catalyst (Mo-FeNNi3) is fabricated via a facile two-step strategy involving hydrothermal reaction and subsequent nitrogen treatment. The designed hydrangea-like structure not only endows the electrocatalyst with a robust framework but also exposes abundant available active sites, thereby facilitating efficient mass transport and accelerating reaction kinetics. The as-prepared Mo-FeNNi3 electrocatalyst delivers exceptional catalytic performance, requiring very low overpotentials of 17, 36, and 77 mV to achieve a current density of 10 mA cm–2 for the hydrogen evolution reaction in alkaline, acidic, and neutral media, respectively, alongside an outstanding oxygen evolution reaction overpotential of 223 mV in alkaline solution. Remarkably, when employed in an alkaline electrolyzer (Mo-FeNNi3||Mo-FeNNi3), it delivers a current density of 10 mA cm–2 at a remarkably low cell voltage of 1.472 V, significantly outperforming the commercial RuO2||Pt/C benchmark (1.536 V). The theoretical studies provide evidence that the electronic structure regulation in Mo-FeNNi3 accelerates water dissociation kinetics and optimizes the adsorption/desorption energies of reaction intermediates, thereby dramatically enhancing the hydrogen production efficiency.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"15 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209542","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

Ammonia Plasma Engineering Enables Efficient Regeneration of Spent Graphite Anodes 氨等离子体工程使废石墨阳极高效再生

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c05993

Xiao Li,Huiyuan Lin,Dong-Jie Xu,Liang Chen,Liming Yang

{"title":"Ammonia Plasma Engineering Enables Efficient Regeneration of Spent Graphite Anodes","authors":"Xiao Li,Huiyuan Lin,Dong-Jie Xu,Liang Chen,Liming Yang","doi":"10.1021/acssuschemeng.6c05993","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c05993","url":null,"abstract":"Abstract Recycling spent graphite anodes is essential for the sustainable development of the lithium-ion battery (LIB) industry. Conventional recycling technologies are often constrained by inherent drawbacks, including high energy consumption, severe secondary pollution, and inadequate structural restoration. Herein, we report a simple room-temperature NH3 plasma treatment strategy for regenerating spent graphite into high-performance anodes. Through precise control of the plasma treatment conditions, three key functions are achieved simultaneously: effective removal of residual passivating solid electrolyte interphase (SEI) species, restoration of the graphitic structural ordering and in situ nitrogen doping. The optimal regenerated anode (denoted N-Gr-20), obtained by 20 min plasma treatment, delivers a high reversible specific capacity of 412 mAh g–1 at 0.5 C. It also exhibits excellent rate capability (296 mAh g–1 at 3.0 C) and exceptional long-cycle stability, retaining a capacity of 286 mAh g–1 after 350 cycles at 2.0 C. Electrochemical kinetic analyses indicate that the restored graphitic framework promotes solid-state Li+ diffusion, while nitrogen-induced surface defects provide additional active sites for surface-controlled lithium storage. Overall, this work establishes a green and sustainable closed-loop strategy for spent LIB recycling and verifies the promising application potential of plasma engineering in the regeneration of spent battery anodes.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"22 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209544","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

Toward Sustainable Sodium-Ion Storage via Local Structural Engineering of Nonstoichiometric Iron-Based Mixed Phosphate–Pyrophosphate Cathodes 通过非化学计量铁基混合磷酸盐-焦磷酸盐阴极的局部结构工程实现可持续的钠离子存储

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c08881

Tinghang Xu,Zhaolu Liu,Xingbo Zhao,Yao Liu,Xingyue Xu,Hui Yang,Shi Chen,Jie Xu,Baofeng Wang,Junxi Zhang,Yang Yu,Jianhang Huang,Yongjie Cao

{"title":"Toward Sustainable Sodium-Ion Storage via Local Structural Engineering of Nonstoichiometric Iron-Based Mixed Phosphate–Pyrophosphate Cathodes","authors":"Tinghang Xu,Zhaolu Liu,Xingbo Zhao,Yao Liu,Xingyue Xu,Hui Yang,Shi Chen,Jie Xu,Baofeng Wang,Junxi Zhang,Yang Yu,Jianhang Huang,Yongjie Cao","doi":"10.1021/acssuschemeng.6c08881","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c08881","url":null,"abstract":"Abstract The nonstoichiometric iron-based mixed phosphate (Na5.12Fe4.44(PO4)2(P2O7)2, N5.12FPP) has emerged as a promising cathode material for sodium-ion batteries (SIBs), benefiting from its low cost, intrinsic safety, and robust structural framework. However, its practical application remains limited by intrinsically low electronic conductivity, sluggish Na-ion transport kinetics, and insufficient long-term cycling stability. In this work, an aliovalent Ti-doping strategy is proposed to modulate the local crystal structure and electronic-state distribution of nonstoichiometric N5.12FPP materials via spray drying following by solid-state calcination method. After optimizing the Ti-doping level, the Na4.72Fe4.24Ti0.2(PO4)2(P2O7)2 (N5.12FPP-0.2Ti) cathode delivers a reversible capacity of 128.5 mAh g–1 at 0.1 C, retains 104.2 mAh g–1 even at 20 C, and maintains 90.05% of its initial capacity after 3000 cycles at 20 C in SIBs. Moreover, a full sodium-ion cell assembling with N5.12FPP-0.2Ti as the positive electrode and commercial hard carbon as the negative electrode achieves a maximum gravimetric energy density of 302.9 Wh kg–1 and power density of 30.4 W kg–1. Therefore, these results demonstrate that Ti-doping can reinforce the host framework, facilitate Na-ion transport, and improve the electrochemical performance of Fe-based mixed-phosphate cathode materials, highlighting its potential for advanced SIBs.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"63 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209538","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

Pt-Modified CoFe Alloy Electrode Enables Ampere-Level Coproduction of Acetate and Hydrogen pt修饰的CoFe合金电极使乙酸和氢的安培级协同生产

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c08560

Cheng Lai,Khalfan Abrahman Khamis,Pengzuo Chen

{"title":"Pt-Modified CoFe Alloy Electrode Enables Ampere-Level Coproduction of Acetate and Hydrogen","authors":"Cheng Lai,Khalfan Abrahman Khamis,Pengzuo Chen","doi":"10.1021/acssuschemeng.6c08560","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c08560","url":null,"abstract":"Abstract Paired electrolysis integrating the ethanol oxidation reaction (EOR) with the hydrogen evolution reaction (HER) provides an energy-efficient strategy for the simultaneous production of value-added chemicals and green hydrogen. Herein, we report a Pt-modified CoFe alloy electrode directly grown on nickel foam (Pt-CoFe/NF) through a facile two-step strategy. The conductive CoFe alloy maximizes Pt utilization, while the electronically coupled Pt-CoFe interface regulates the electronic structure, accelerates charge transfer, and generates abundant catalytic active sites. Operando spectroscopic investigations, together with density functional theory calculations reveal that the Pt-CoFe heterointerface promotes water activation and *OH generation for ethanol oxidation, while simultaneously optimizing *H adsorption for hydrogen evolution, thereby synergistically accelerating both half-reactions. As a result, the Pt-CoFe/NF electrode requires only 1.48 V and 95.8 mV to achieve 1000 mA cm–2 for the EOR and HER, respectively, and also delivers a high acetate Faradaic efficiency (90.6%) with a yield rate of 4.30 mmol h–1 cm–2 at 1.9 V. In addition, the assembled EOR‖HER electrolyzer delivers a low cell voltage of 2.25 V to reach 1 A cm–2, high yields of H2/acetate and realizes long-term stability for 100 h.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"26 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209541","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

Efficient Catechol Production from 2-Acetylfuran in Subcritical Water with ZnCl2 as a Lewis-Acid Catalyst ZnCl2为路易斯酸催化剂亚临界水中2-乙酰呋喃高效产儿茶酚

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c08123

Stef Ghysels,Hero Jan Heeres,Peter J. Deuss

{"title":"Efficient Catechol Production from 2-Acetylfuran in Subcritical Water with ZnCl2 as a Lewis-Acid Catalyst","authors":"Stef Ghysels,Hero Jan Heeres,Peter J. Deuss","doi":"10.1021/acssuschemeng.6c08123","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c08123","url":null,"abstract":"Abstract Catechol (1,2-benzenediol) is a critical platform chemical with a growing global market, currently produced primarily through the fossil-based Hock process to produce phenol from benzene, followed by its hydroxylation to catechol. As the transition toward a bio-based economy intensifies, identifying sustainable production routes from renewable resources like lignocellulosic biomass is essential. To that end, different biomass-to-catechol strategies have been developed, such as (i) lignin depolymerization, followed by catalytic conversion of their alkylated/methoxylated phenol monomers, or (ii) glucose fermentation to catechol. Yet both approaches face specific challenges that hamper strong market integration. As an alternative, this present study reports an interesting, yet long-neglected alternative, catechol synthesis in subcritical water from 2-acetylfuran, a biomass-derived furan obtained from, e.g., sorbitol dehydration or acylation of furan. Since the subcritical reaction of 2-acetylfuran to catechol essentially entails a rearrangement, a higher atom economy can be persued, compared to lignin and fermentation-based routes. After initial exploration, a systematic optimization of the reaction temperature, time, and Lewis catalyst concentration (ZnCl2) through response surface modeling, a catechol yield of 52% was achieved (i.e., a 10-fold increase over what was previously achieved) at a conversion of 82% and a selectivity of 61% (applying catalyst concentration of 2.4 mol % ZnCl2, 310 °C reaction temperature and 366 min reaction time). Mass balance closures reached 92–93%, identifying acetic acid as the primary side product formed through competing α-dicarbonyl cleavage, with virtually no catechol degradation under these reaction conditions. These findings establish 2-acetylfuran as a high-potential feedstock for sustainable aromatic production, offering a robust pathway for integrating green catechol into industrial biorefinery schemes.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"11 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209588","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

Ampere-Level Pulsed Electrosynthesis of Glycolic Acid over Pd-Modified Low-Coordination Cobalt Nanosheets 在pd修饰低配位钴纳米片上的安培级脉冲电合成乙醇酸

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c08608

Wentao Wang,Ma Jiamin,Zhouhong Yu,Nan Zhang,Yun Tong

{"title":"Ampere-Level Pulsed Electrosynthesis of Glycolic Acid over Pd-Modified Low-Coordination Cobalt Nanosheets","authors":"Wentao Wang,Ma Jiamin,Zhouhong Yu,Nan Zhang,Yun Tong","doi":"10.1021/acssuschemeng.6c08608","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c08608","url":null,"abstract":"Abstract Selective electrosynthesis of glycolic acid (GA) from ethylene glycol (EG) offers an attractive route for producing value-added chemicals, yet achieving high performance at ampere-level current densities remains challenging because of the oxidative deactivation of noble-metal active sites. Herein, we report a Pd nanoparticle-decorated low-coordination Co nanosheet catalyst (Pd@L-Co) for efficient pulsed electrosynthesis of GA. Benefiting from the strong electronic interaction between Pd nanoparticles and defect-rich Co nanosheets, the optimal Pd@L-Co catalyst delivers ampere-level EG oxidation with a maximum GA Faradaic efficiency of 96.96% at 0.9 V vs RHE and a GA yield of 2.42 mmol h–1 cm–2 at 1.3 V vs RHE. More importantly, pulse electrolysis effectively suppresses the continuous oxidation of Pd sites, maintaining highly active metallic Pd species and enabling sustained catalytic performance. Operando measurements reveal that alternating anodic/cathodic potentials dynamically regenerate Pd active centers while simultaneously preventing the accumulation of surface-poisoning intermediates. Density functional theory calculations further demonstrate that defect-rich Co optimizes the electronic structure of Pd, promotes OH* activation, and lowers the energy barrier to the rate-determining step of intermediate formation.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"63 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209587","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

Modulating Phase-Selective Dealloying and Structural Stability of a Self-Supporting Nanoporous CuZrAl MG Electrode via Trace Pd Decoration 微量Pd修饰自支撑型纳米孔CuZrAl MG电极的调制相选择脱合金及其结构稳定性

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c07591

Ling Li,Wence Xu,Yue Zhao,Kexin Yan,Zhonghui Gao,Yanqin Liang,Hui Jiang,Zhaoyang Li,Dan Luo,Enzuo Liu,Zhenduo Cui,Wei Li,Meng Zhang,Zhongwei Chen,Shengli Zhu

{"title":"Modulating Phase-Selective Dealloying and Structural Stability of a Self-Supporting Nanoporous CuZrAl MG Electrode via Trace Pd Decoration","authors":"Ling Li,Wence Xu,Yue Zhao,Kexin Yan,Zhonghui Gao,Yanqin Liang,Hui Jiang,Zhaoyang Li,Dan Luo,Enzuo Liu,Zhenduo Cui,Wei Li,Meng Zhang,Zhongwei Chen,Shengli Zhu","doi":"10.1021/acssuschemeng.6c07591","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c07591","url":null,"abstract":"Abstract Combining high mechanical integrity with optimized catalytic kinetics remains a critical bottleneck for exploiting Cu-based nanoporous materials in the hydrogen evolution reaction (HER). In this work, a self-supporting nanoporous Cu-based metallic glass modified with trace Pd (np-Pd-CuZrAl) was fabricated via sequential phase-selective chemical dealloying and galvanic replacement. In 1.0 M KOH, the np-Pd-CuZrAl catalyst exhibits superior performance, requiring an overpotential of only 89.0 mV at 10 mA cm−2 with a low Tafel slope of 34.38 mV dec−1, maintaining exceptional activity after 100 h of continuous operation. Notably, nanoindentation and tensile testing demonstrate the exceptional deformation tolerance of the np-Pd-CuZrAl electrode, which successfully retains its structural and electrochemical functionality under severe tensile and bending deformations. In situ Raman spectroscopy and DFT calculations demonstrate that Pd incorporation effectively tunes the d-band center, enhances interfacial water adsorption, and inhibits surface oxidation. Furthermore, a water-splitting cell using this cathode achieves 10 mA cm−2 at 1.54 V. This work establishes a compelling strategy to modulate atomic configuration and mechanical stability in freestanding metallic glass electrodes, providing deep metallurgical insights.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"86 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209536","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

Monodentate Acetate-Coordinated Electrolyte for Accelerated Zn2+ Desolvation and Stable Zinc Anodes 加速Zn2+脱溶和稳定锌阳极的单齿酸盐配位电解质

IF 8.4 1区化学

ACS Sustainable Chemistry & Engineering Pub Date : 2026-10-15 DOI: 10.1021/acssuschemeng.6c09143

Yaping Song,Yang Song,Liwen Hu,Xiangyu Luo,Shuqiang Jiao

{"title":"Monodentate Acetate-Coordinated Electrolyte for Accelerated Zn2+ Desolvation and Stable Zinc Anodes","authors":"Yaping Song,Yang Song,Liwen Hu,Xiangyu Luo,Shuqiang Jiao","doi":"10.1021/acssuschemeng.6c09143","DOIUrl":"https://doi.org/10.1021/acssuschemeng.6c09143","url":null,"abstract":"Abstract Aqueous zinc-ion batteries (AZIBs) are promising candidates for large-scale energy storage, but their practical deployment is hindered by dendrite growth and water-induced side reactions. These challenges mainly arise from the high desolvation barrier of [Zn(H2O)6]2+, which slows interfacial kinetics and promotes irregular Zn deposition. Here, we propose a monodentate acetate-coordinated electrolyte (MACE) based on non-flammable trimethyl phosphate (TMP) as a co-solvent and KAc as a coordination regulator. Both theoretical and experimental analyses reveal that the acetate coordination mode critically governs Zn2+ desolvation behavior: compared with bidentate coordination, the monodentate configuration weakens the Ac–-Zn2+ interaction, lowers the desolvation energy barrier, and enables uniform, compact Zn deposition. Meanwhile, excess Ac– constructs a H-bonding network with water molecules, effectively suppressing water activity and related parasitic reactions. As a result, the MACE enables highly stable Zn anodes, delivering a Zn symmetric cell lifespan of over 4800 h at 0.5 mA cm–2 and 0.5 mAh cm–2. Moreover, Zn||NH4V4O10 full cells exhibit high capacity and excellent cycling stability. This work highlights the pivotal role of the anion coordination mode in Zn2+ desolvation and offers a new solvation-regulation strategy for advanced AZIBs.","PeriodicalId":25,"journal":{"name":"ACS Sustainable Chemistry & Engineering","volume":"4 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209549","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