ChemSusChem最新文献_第8页

Failure Mechanism Analysis and Emerging Strategies for Enhancing the Photoelectrochemical Stability of Photoanodes. 失效机理分析和增强光阳极光电化学稳定性的新策略。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-25 DOI: 10.1002/cssc.202401420

Yingjuan Zhang, Boyan Liu, Liangcheng Xu, Zeran Ding, Rui Yang, Songcan Wang

{"title":"Failure Mechanism Analysis and Emerging Strategies for Enhancing the Photoelectrochemical Stability of Photoanodes.","authors":"Yingjuan Zhang, Boyan Liu, Liangcheng Xu, Zeran Ding, Rui Yang, Songcan Wang","doi":"10.1002/cssc.202401420","DOIUrl":"10.1002/cssc.202401420","url":null,"abstract":"The development of efficient and stable photoanode materials is essential for driving the possible practical application of photoelectrochemical water splitting. This article begins with a basic understanding of the fundamentals of photoelectrochemical devices and photoanodes. State-of-the-art strategies for designing photoanodes with long-term stability are highlighted, including insertion of hole transport layers, construction of protective/passivation layers, loading of co-catalysts, construction of heterojunctions, and modification of the electrolyte. Based on the insights gained from these effective strategies, we present an outlook for addressing key aspects of the challenges of stabilizing photoanodes development in the future work. Widespread adoption of stability assessment criteria will facilitate reliable comparisons of results from different laboratories. In addition, deactivation of photoanode is defined as a 50 % reduction in productivity. An in-depth understanding of the deactivation mechanism is essential for the design and development of efficient and stable photoanodes. This work will provide insights into the stability assessment of photoanode and facilitate the production of practical solar fuels.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401420"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142015768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Main-Group Elements Enhance Electrochemical Nitrogen Reduction Reaction of Vanadium-Based Single Atom Catalysts Through d-p Orbital Hybridization. 主族金属元素通过 d-p 轨道杂化增强钒基单原子催化剂的电化学氮还原反应。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-22 DOI: 10.1002/cssc.202400808

Haoyu Wang, Riming Hu, Ruochen Zhu, Liang Xue, Shuaijun Yang, Yong Nie, Jiayuan Yu, Xuchuan Jiang

{"title":"Main-Group Elements Enhance Electrochemical Nitrogen Reduction Reaction of Vanadium-Based Single Atom Catalysts Through d-p Orbital Hybridization.","authors":"Haoyu Wang, Riming Hu, Ruochen Zhu, Liang Xue, Shuaijun Yang, Yong Nie, Jiayuan Yu, Xuchuan Jiang","doi":"10.1002/cssc.202400808","DOIUrl":"10.1002/cssc.202400808","url":null,"abstract":"Developing active sites with flexibility and diversity is crucial for single atom catalysts (SACs) towards sustainable nitrogen fixation at ambient conditions. Herein, the effects of doping main group metal elements (MGM) on the stability, catalytic activity, and selectivity of vanadium-based SACs is systematically investigated based on density functional theory calculations. It is found that the catalytic activity of V site can be significantly enhanced by the synergistic effect between MGM and vanadium atoms. More importantly, a volcano curve between the catalytic activity and the adsorption free energy of NNH* can be established, in which V-Pb dimer embedded on N-coordinated graphene (VPb-NG) exhibits optimal NRR activity due to its location at the top of volcano. Further analysis of electronic structures reveals that the unoccupancy ratio (eg/t2g) of V site is dramatically increased by the strong d-p orbital hybridization between V and Pb atoms, subsequently, N2 is activated to a larger extent. These interesting findings may provide a new path for designing active sites in SACs with excellent performance.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400808"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142007913","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Cellulose Acetates in Hydrothermal Carbonization: A Green Pathway to Valorize Residual Bioplastics. 热液碳化中的醋酸纤维素：实现残余生物塑料价值化的绿色途径。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-18 DOI: 10.1002/cssc.202401163

Giulia Ischia, Filippo Marchelli, Nicola Bazzanella, Riccardo Ceccato, Marco Calvi, Graziano Guella, Claudio Gioia, Luca Fiori

{"title":"Cellulose Acetates in Hydrothermal Carbonization: A Green Pathway to Valorize Residual Bioplastics.","authors":"Giulia Ischia, Filippo Marchelli, Nicola Bazzanella, Riccardo Ceccato, Marco Calvi, Graziano Guella, Claudio Gioia, Luca Fiori","doi":"10.1002/cssc.202401163","DOIUrl":"10.1002/cssc.202401163","url":null,"abstract":"Bioplastics possess the potential to foster a sustainable circular plastic economy, but their end-of-life is still challenging. To sustainably overcome this problem, this work proposes the hydrothermal carbonization (HTC) of residual bioplastics as an alternative green path. The focus is on cellulose acetate - a bioplastic used for eyewear, cigarette filters and other applications - showing the proof of concept and the chemistry behind the conversion, including a reaction kinetics model. HTC of pure and commercial cellulose acetates was assessed under various operating conditions (180-250 °C and 0-6 h), with analyses on the solid and liquid products. Results show the peculiar behavior of these substrates under HTC. At 190-210 °C, the materials almost completely dissolve into the liquid phase, forming 5-hydroxymethylfurfural and organic acids. Above 220 °C, intermediates repolymerize into carbon-rich microspheres (secondary char), achieving solid yields up to 23 %, while itaconic and citric acid form. A comparison with pure substrates and additives demonstrates that the amounts of acetyl groups and derivatives of the plasticizers are crucial in catalyzing HTC reactions, creating a unique environment capable of leading to a total rearrangement of cellulose acetates. HTC can thus represent a cornerstone in establishing a biorefinery for residual cellulose acetate.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401163"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11739857/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141974618","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

¹³C-Labelled Glucose Reveals Shifts in Fermentation Pathway During Cathodic Electro-Fermentation with Mixed Microbial Culture. 13C 标记的葡萄糖揭示了混合微生物培养阴极电发酵过程中发酵途径的转变。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-11-11 DOI: 10.1002/cssc.202401033

Gaia Salvatori, Ottavia Giampaoli, Angela Marchetti, Alfredo Miccheli, Bernardino Virdis, Fabio Sciubba, Marianna Villano

{"title":"13C-Labelled Glucose Reveals Shifts in Fermentation Pathway During Cathodic Electro-Fermentation with Mixed Microbial Culture.","authors":"Gaia Salvatori, Ottavia Giampaoli, Angela Marchetti, Alfredo Miccheli, Bernardino Virdis, Fabio Sciubba, Marianna Villano","doi":"10.1002/cssc.202401033","DOIUrl":"10.1002/cssc.202401033","url":null,"abstract":"Cathodic Electro-Fermentation (CEF) is an innovative approach to manage the spectrum of products deriving from anaerobic fermentation. Herein, mixed microbial culture fermentation using a ternary mixture containing labelled 13C glucose and non-labelled acetate and ethanol was studied to identify the role of polarization on the metabolic pathways of glucose fermentation. CEF at an applied potential of -700 mV (vs. SHE, Standard Hydrogen Electrode) enhanced the production yield of acetate, propionate, and butyrate (0.90±0.10, 0.22±0.03, and 0.34±0.05 mol/mol; respectively) compared to control tests performed at open circuit potential (OCP) (0.54±0.09, 0.15±0.04, and 0.20±0.001 mol/mol, respectively). Results indicate that CEF affected the 13C labelled fermented product levels and their fractional 13C enrichments, allowing to establish metabolic pathway models. This work demonstrates that, under cathodic polarization, the abundance of both fully 13C labelled propionate and butyrate isotopomers increased compared to control tests. The effect of CEF is mainly due to intermediates initially produced from the glucose metabolic transformation in the presence of non-labelled acetate and ethanol as external substrates. These findings represent a significant advancement in current knowledge of CEF, which offers a promising tool to control mixed cultures bioprocesses.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401033"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11739826/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142118542","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Superprotonic Conductivity by Synergistic Blending of Coordination Polymers with Organic Polymers: Fabrication of Durable and Flexible Proton Exchange Membranes. 通过配位聚合物与有机聚合物的协同混合实现超质子传导性：制造耐用、灵活的质子交换膜。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-25 DOI: 10.1002/cssc.202401463

Mouli Das Dawn, Sambit Roy, Abhijit Garai, Susanta Banerjee, Kumar Biradha

{"title":"Superprotonic Conductivity by Synergistic Blending of Coordination Polymers with Organic Polymers: Fabrication of Durable and Flexible Proton Exchange Membranes.","authors":"Mouli Das Dawn, Sambit Roy, Abhijit Garai, Susanta Banerjee, Kumar Biradha","doi":"10.1002/cssc.202401463","DOIUrl":"10.1002/cssc.202401463","url":null,"abstract":"Creation of an efficient and cost-effective proton exchange membrane (PEM) has emerged as a propitious solution to address the challenges of renewable energy development. Coordination polymers (CPs) have garnered significant interest due to their multifunctional applications and moldability, along with long-range order. To leverage the potential of CPs in fuel cells, it is essential to integrate microcrystalline CPs into organic polymers to prepare membranes and avoid grain boundary issues. In this study, we designed and synthesized CPs containing imidazole and sulfonate moieties via gel-to-crystal transformation. The integration of CPs into the PVDF-PVP matrix resulted in superprotonic conductivity in the order of 10-2 S cm-1 at room temperature (30 °C) and 98 % RH. The proton conductivity achieved with CP-integrated composite membrane was 4.69×10-2 S cm-1 at 80 °C and 98 % RH, the highest among all CP/MOF-integrated PVDF-PVP membranes under hydrous conditions. The excellent compatibility of CPs with PVDF-PVP produced highly flexible membranes with superior mechanical, chemical, and thermal stability. About 25 times higher proton conductivity value was achieved with membrane, compared to intrinsic CPs, at RT and 98 % RH. Thus, we present a cost-effective CP-integrated mixed-matrix membrane with superprotonic conductivity and long-term durability for cutting-edge fuel cell development.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401463"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11739856/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142071547","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Electrochemical Kinetics of LiFePO₄ Cathode Material in Non-flammable Inorganic Liquid Electrolyte. 非易燃无机液态电解质中磷酸铁锂阴极材料的电化学动力学。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-09-25 DOI: 10.1002/cssc.202400122

Vishwanathan Ramar, Christian Pszolla, Manuel Weinberger, Markus Borck, Laurent Zinck

引用次数: 0

Modification Strategies of Bismuth-Based Halide Perovskites for Solar to Fuel Conversion by Photocatalytic CO₂ Reduction. 光催化CO2还原太阳能转化为燃料的铋基卤化物钙钛矿改性策略。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 DOI: 10.1002/cssc.202402106

Pei Tian, Yan Ding, Fei Zhang, Yihao Zhang, Jinjia Wei, Jie Chen

{"title":"Modification Strategies of Bismuth-Based Halide Perovskites for Solar to Fuel Conversion by Photocatalytic CO2 Reduction.","authors":"Pei Tian, Yan Ding, Fei Zhang, Yihao Zhang, Jinjia Wei, Jie Chen","doi":"10.1002/cssc.202402106","DOIUrl":"10.1002/cssc.202402106","url":null,"abstract":"In light of the increasingly pressing energy and environmental challenges, the use of photocatalysis to convert solar energy into chemical energy has emerged as a promising solution. Halide perovskites have recently attracted considerable interest as photocatalysts due to their outstanding properties. Early developments focused on Lead-based perovskites, but their use has been severely restricted due to the toxicity of Lead. Consequently, researchers have introduced non-toxic elements to replace Lead, with common substitutes being transition metals such as Tin (Sn), Bismuth (Bi), and Antimony (Sb). Among them, Bi-based perovskites have demonstrated superior photocatalytic performance. Nevertheless, the inherent instability of perovskites and the severe recombination of charge carriers have necessitated the development of various modification strategies to enhance their performance. This Review discusses the modification strategies for Bi-based halide perovskites and illustrates the impact of these strategies on the photocatalytic performance. Finally, future research directions and challenges of Bi-based perovskites for photocatalysis are proposed.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402106"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142982278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Photothermal Assisted Biomass Oxidation for Pairing Carbon Dioxide Electroreduction with Low Cell Potential. 光热辅助生物质氧化，将二氧化碳电还原与低电池电位结合起来。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-10 DOI: 10.1002/cssc.202400493

Houjun Chen, Rongcheng Peng, Ting Hu, Naizhuo Tang, Yahan Wang, Yan Zhang, Wenpeng Ni, Shiguo Zhang

{"title":"Photothermal Assisted Biomass Oxidation for Pairing Carbon Dioxide Electroreduction with Low Cell Potential.","authors":"Houjun Chen, Rongcheng Peng, Ting Hu, Naizhuo Tang, Yahan Wang, Yan Zhang, Wenpeng Ni, Shiguo Zhang","doi":"10.1002/cssc.202400493","DOIUrl":"10.1002/cssc.202400493","url":null,"abstract":"Integrating anodic biomass valorization with carbon dioxide electroreduction (CO2RR) can produce value-added chemicals on both the cathode and anode; however, anodic oxidation still suffers from high overpotential. Herein, a photothermal-assisted method was developed to reduce the potential of 5-hydroxymethyl furfural (HMF) electrooxidation. Capitalizing on the copious oxygen vacancies, defective Co3O4 (D-Co3O4) exhibited a stronger photothermal effect, delivering a local temperature of 175.47 °C under near infrared light illumination. The photothermal assistance decreased the oxidation potential of HMF from 1.7 V over pristine Co3O4 to 1.37 V over D-Co3O4 to achieve a target current density of 30 mA cm-2, with 2,5-furandicarboxylic acid as the primary product. Mechanistic analysis disclosed that the photothermal effect did not change the HMF oxidation route but greatly enhanced the adsorption capacity of HMF. Meanwhile, faster electron transfer for direct HMF oxidation and the surface conversion to cobalt (oxy)hydroxide, which contributed to indirect HMF oxidation, was observed. Thus, rapid HMF conversion was realized, as evidenced by in situ surface-enhanced infrared spectroscopy. Upon coupling cathodic CO2RR with an atomically dispersed Ni-N/C catalyst, the Faradaic efficiencies of CO (cathode) and 2,5-furandicarboxylic acid (FDCA, anode) exceeded 90.0 % under a low cell potential of 1.77 V.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400493"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141900224","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Semiconductor Effect from Pd(II) Porphyrin Metal to Its Ligand in Photocatalytic N-Dealkylation. 光催化 N-脱烷基反应中 Pd(II) 卟啉金属与其配体的半导体效应。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-10 DOI: 10.1002/cssc.202401381

Borong Liao, Junhao Gao, Pei Weng, Linya He, Yusheng Zhang, Qiuhua Liu, Zaichun Zhou

引用次数: 0

Toluene-Poisoning-Resistant High-Entropy Non-Noble Metal Anode for Direct One-Step Hydrogenation of Toluene to Methylcyclohexane. 用于将甲苯直接一步加氢转化为甲基环己烷的抗甲苯中毒高熵非贵金属阳极。

IF 7.5 2区化学

ChemSusChem Pub Date : 2025-01-14 Epub Date: 2024-10-24 DOI: 10.1002/cssc.202401071

Aimi A H Tajuddin, Tatsuhiko Ohto, Hisanori Tanimoto, Takeshi Fujita, Samuel Jeong, Atsushi Fukazawa, Yuto Shimoyama, Yoshitatsu Misu, Kaori Takano, Koji Matsuoka, Yoshikazu Ito

{"title":"Toluene-Poisoning-Resistant High-Entropy Non-Noble Metal Anode for Direct One-Step Hydrogenation of Toluene to Methylcyclohexane.","authors":"Aimi A H Tajuddin, Tatsuhiko Ohto, Hisanori Tanimoto, Takeshi Fujita, Samuel Jeong, Atsushi Fukazawa, Yuto Shimoyama, Yoshitatsu Misu, Kaori Takano, Koji Matsuoka, Yoshikazu Ito","doi":"10.1002/cssc.202401071","DOIUrl":"10.1002/cssc.202401071","url":null,"abstract":"The direct one-step hydrogenation of toluene to methylcyclohexane facilitated by a proton-exchange membrane water electrolyzer driven by renewable energy has garnered considerable attention for stable hydrogen storage and safe hydrogen transportation. However, a persistent challenge lies in the crossover of toluene from the cathode to the anode chamber, which deteriorates the anode and decreases its energy efficiency and lifetime. To address this challenge, the catalyst-poisoning mechanism is systematically investigated using IrO2 and high-entropic non-noble-metal alloys as anodes in acidic electrolytes saturated with toluene and toluene-oxidized derivatives, such as benzaldehyde, benzyl alcohol, and benzoic acid. Benzoic acid plays an important role in polymer-like carbon-film formation by blocking the catalytically active sites on the anode surface. Moreover, Nb and the highly entropic state on the surface of the multi-element alloy lower the adsorbing ability of toluene and prevent polymer-like carbon film formation. This study contributes to the design of catalyst-poisoning-resistant anodes for organic hydride technology, advanced fuel cells, and batteries.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401071"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142015773","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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