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Biomimetic Aerobic Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in Deep Eutectic Solvents through the Efficient Electron Transfer. 5-羟甲基糠醛在深度共晶溶剂中通过高效电子转移仿生有氧氧化制2,5-呋喃二羧酸。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-19 DOI: 10.1002/cssc.202402589
Xingyao Wei, Fuhao Chu, Weiguang Wang, Qiaohong Zhang, Dongmei Hao, Zhiguo Zhu, Kaixuan Yang, Chen Chen, Hongying Lü
{"title":"Biomimetic Aerobic Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid in Deep Eutectic Solvents through the Efficient Electron Transfer.","authors":"Xingyao Wei, Fuhao Chu, Weiguang Wang, Qiaohong Zhang, Dongmei Hao, Zhiguo Zhu, Kaixuan Yang, Chen Chen, Hongying Lü","doi":"10.1002/cssc.202402589","DOIUrl":"10.1002/cssc.202402589","url":null,"abstract":"<p><p>Selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) has long been a formidable challenge under mild conditions. Deep eutectic solvents (DESs) have shown remarkable efficiency in the oxidation of HMF as a sustainable solvent. These solvents not only enhance solubilization but also activate biomass-derived hydroxyl compounds via hydrogen bonds reconstruction. This study leverages the architecture and functionality of natural enzymes and coenzymes in the respiratory chain system to develop a unique biomimetic catalytic system. In this system, HMF is oxidized to FDCA in imidazole-based DESs with polyoxometalates as catalyst and para-benzoquinone as electron transfer mediators. The findings demonstrate that the adjustment of hydrogen bond acceptor (HBA) or hydrogen bond donor (HBD) enables precise control over the hydrogen bond strength in DESs, thereby accurately regulating the distribution of HMF oxidation products. Furthermore, the optimization of hydrogen bond strength can also activate the OH bond in HMF, consequently expediting the oxidation reaction. The cyclic voltammetry measurements provide compelling evidence of dioxygen activation and efficient electron transferring in a biomimetic catalytic system, resulting in a remarkable 21-fold increase in current density. This research not only advances utilization and development of biomass resources but also offers novel perspectives into constructing efficient catalytic oxidation systems.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2402589"},"PeriodicalIF":7.5,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661712","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
Recyclable Organic Redox Molecules for Sustainable Batteries. 用于可持续电池的可回收有机氧化还原分子。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202402707
Kouki Oka, Hitoshi Kasai
{"title":"Recyclable Organic Redox Molecules for Sustainable Batteries.","authors":"Kouki Oka, Hitoshi Kasai","doi":"10.1002/cssc.202402707","DOIUrl":"10.1002/cssc.202402707","url":null,"abstract":"<p><p>Sustainable and environment-friendly rechargeable devices are required to meet increasing electrical energy demands. Organic batteries are fabricated using organic redox materials which are potentially synthesised from earth-abundant components. However, to avoid plastic pollution, these organic materials must display sufficient functions and ensure safe management post-utilisation. This study demonstrated a sustainable and environment-friendly recycling method for functional organic materials developed using organic redox molecules. These molecules could be prepared from earth-abundant and sustainable raw chemicals via environment-friendly preparation routes. The eco-friendly battery, which uses organic redox molecules as anode- and cathode-active materials and neutral aqueous solution as an electrolyte, exhibited high cyclability (>95 % capacity after 100 cycles) and high-rate capability (15 C). After use, the electrode-active material was separated and/or decomposed to the original raw chemicals, demonstrating a green and sustainable option to use conventional organic redox materials.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402707"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655861","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
Electrocatalytic Ammonia Oxidation Reaction: Selective Formation of Nitrite and Nitrate as Value-Added Products. 电催化氨氧化反应:选择性形成亚硝酸盐和硝酸盐作为增值产品。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202402516
Ieva A Cechanaviciute, Wolfgang Schuhmann
{"title":"Electrocatalytic Ammonia Oxidation Reaction: Selective Formation of Nitrite and Nitrate as Value-Added Products.","authors":"Ieva A Cechanaviciute, Wolfgang Schuhmann","doi":"10.1002/cssc.202402516","DOIUrl":"10.1002/cssc.202402516","url":null,"abstract":"<p><p>Ammonia (NH<sub>3</sub>) plays a pivotal role as a hydrogen carrier, offering a carbon-free energy alternative for sustainable energy systems. The ammonia electrooxidation reaction (AmOR) emerges as a promising avenue to leverage NH₃ in energy conversion and environmental applications. This review explores the multifaceted importance of NH<sub>3</sub> oxidation through three primary strategies: its integration into fuel cell technology for clean energy generation, its use in wastewater treatment for ammonia removal, and its application in electrolyzer setups for producing value-added products. Special emphasis is placed on oxidizing NH<sub>3</sub> to nitrite (NO<sub>2</sub> <sup>-</sup>) and nitrate (NO<sub>3</sub> <sup>-</sup>) in electrolyzers as a potential alternative to the energy-intensive Ostwald process. The review highlights recent advances in catalyst development for efficient NO<sub>2</sub> <sup>-</sup>/NO<sub>3</sub> <sup>-</sup> synthesis, the influence of the pH on reaction selectivity, and various reported experimental AmOR solutions. By addressing these critical aspects, this work aims to underscore the potential of NH<sub>3</sub> oxidation in electrolyzers for sustainable energy solutions. Potential future research directions and challenges are also discussed.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402516"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655825","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
Sustainable Quantum Dot-Vitrimer Composites: A Synergy of Quantum Dots and Dynamic Covalent Bonds. 可持续量子点-玻璃体复合材料:量子点和动态共价键的协同作用。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202500464
Yong-Yun Zhang, Meng-Yu Lin, Yi-Ting Tsai, Man-Kit Leung, Mu-Huai Fang
{"title":"Sustainable Quantum Dot-Vitrimer Composites: A Synergy of Quantum Dots and Dynamic Covalent Bonds.","authors":"Yong-Yun Zhang, Meng-Yu Lin, Yi-Ting Tsai, Man-Kit Leung, Mu-Huai Fang","doi":"10.1002/cssc.202500464","DOIUrl":"https://doi.org/10.1002/cssc.202500464","url":null,"abstract":"<p><p>Functional nanocomposites combining quantum dots (QDs) and polymers have garnered significant attention due to their unique optical properties. However, the presence of toxic heavy metal ions remains a significant challenge for eco-friendly material development. Here, we introduce the design and fabrication of a quantum-dot-in-vitrimer (QD@vitrimer) nanocomposite that leverages dynamic covalent bonds, providing chemical extractability of the embedded QDs from crosslinked polymers. Unlike commercially available UV-cured resins, our QD@vitrimer nanocomposite demonstrates uniform QD dispersion with minimal aggregation, as confirmed by synchrotron transmission small-angle X-ray scattering and high-resolution scanning transmission electron microscopy. The composites can be degraded via an alcoholysis process driven by built-in catalysts, enabling rapid breakdown and efficient QD extraction under neutral conditions. We achieved 99.9% QD extraction efficiency while preserving the crystal structure and photoluminescence quantum yield of the QDs, significantly enhancing the reusability of these valuable nanomaterials, as verified by inductively coupled plasma optical emission spectrometry and synchrotron X-ray absorption spectroscopy. Finally, we re-fabricated the QD@vitrimer nanocomposite using the recycled QDs, establishing a closed-loop system that extends the material's lifecycle. This work highlights the pioneering strategy for developing chemically recyclable, eco-friendly luminescent nanocomposite, offering a new direction for advancing green materials in advanced applications.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500464"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655864","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
Ti-MXene/α-Ni(OH)2 nanostructures as high performance electrocatalyst for oxygen evolution reaction. Ti-MXene/α-Ni(OH)2纳米结构作为析氧反应的高性能电催化剂
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202402603
Mrunal Bhosale, Sadhasivam Thangarasu, Nagaraj Murugan, Yoong Ahm Kim, Taehwan Oh
{"title":"Ti-MXene/α-Ni(OH)2 nanostructures as high performance electrocatalyst for oxygen evolution reaction.","authors":"Mrunal Bhosale, Sadhasivam Thangarasu, Nagaraj Murugan, Yoong Ahm Kim, Taehwan Oh","doi":"10.1002/cssc.202402603","DOIUrl":"https://doi.org/10.1002/cssc.202402603","url":null,"abstract":"<p><p>Herein, the strategy of homogenous inclusion of nanoparticles within the surface and interlayers of 2D MXenes was established to achieve effective OER performance. A greater quantity of ~6 nm sized Ni(OH)2 particles uniformly anchored on multi-layered accordion-like nanosheets of Ti3C2Tx. The strong interconnection of Ni(OH)2 on Ti3C2Tx promoting synergistic effects and improves electron transfer properties alongside the intrinsic OER activity. The Ti3C2Tx-Ni(OH)2-4 demonstrated remarkable OER activity by exhibiting a lower overpotential (235.54 mV at 10 mA/cm2) in alkaline conditions. Increased ECSA (2.925 mF cm-2), lower charge transfer resistance, lowering the reaction barrier and stabilizing/converting essential intermediates via the Ti3C2Tx-Ni(OH)2 electrocatalyst synergistically improve OER activity. The effective interaction between Ti3C2Tx and Ni(OH)2 in Ti3C2Tx-Ni(OH)2 improves stability during long-term operations. Moreover, a Ti3C2Tx-Ni(OH)2-4||Pt/C cell has 1.7V at 10 mA/cm2. It could be deduced that the usage of Ni(OH)2 as an electrocatalyst together with Ti3C2Tx can provide noteworthy water splitting properties.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402603"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143646719","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
Nafion-Based Proton Exchange Membranes for Vanadium Redox Flow Batteries. 钒氧化还原液流电池的钠基质子交换膜。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202402506
Siqi He, Shengchao Chai, Haolong Li
{"title":"Nafion-Based Proton Exchange Membranes for Vanadium Redox Flow Batteries.","authors":"Siqi He, Shengchao Chai, Haolong Li","doi":"10.1002/cssc.202402506","DOIUrl":"10.1002/cssc.202402506","url":null,"abstract":"<p><p>The sustainable development of future societies depends on advanced energy storage technologies. Vanadium redox flow batteries (VRFBs) are a preferred solution for large-scale, long-duration energy storage due to their high capacity, long lifespan, rapid response, and safety. The proton exchange membrane (PEM) is a pivotal component of VRFBs, playing a crucial role for conducting protons and preventing vanadium ion crossover. Currently, perfluorinated sulfonic acid membranes, represented by Nafion, are the most commonly used PEMs in VRFBs. However, the size discrepancy between vanadium ions (~0.6 nm) and the ionic domains in Nafion membranes (3-5 nm) leads to significant vanadium permeability, resulting in reduced battery performance. Therefore, rationally regulating the structure of Nafion membranes to enhance their conductive selectivity is an urgent issue. This review focuses on recent advancements in Nafion modification, offering valuable insights for inspiring the fundamental innovation of high-selective Nafion membranes for VRFB technology.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402506"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655775","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
19.36 % Efficiency in Binary Organic Solar Cells with Amine-Hydroxy-Substituted Perylene Diimide-Based Interface Layers. 以氨基-羟基取代苝二酰亚胺为界面层的二元有机太阳能电池效率为19.36%。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202500119
Xuanyan Luo, Chengcheng Xie, Xiaofeng Qin, Wenming Li, Weile Guo, Bin Zhang, Bo Xu, Zhuo Wang, Nian Zhang, Menglan Lv
{"title":"19.36 % Efficiency in Binary Organic Solar Cells with Amine-Hydroxy-Substituted Perylene Diimide-Based Interface Layers.","authors":"Xuanyan Luo, Chengcheng Xie, Xiaofeng Qin, Wenming Li, Weile Guo, Bin Zhang, Bo Xu, Zhuo Wang, Nian Zhang, Menglan Lv","doi":"10.1002/cssc.202500119","DOIUrl":"10.1002/cssc.202500119","url":null,"abstract":"<p><p>Organic solar cells (OSCs) have garnered extensive attention and experienced rapid development due to their immense potential in addressing future energy challenges. Among the critical components of OSCs, cathode interfacial materials (CIMs) play a pivotal role in reducing the work function of electrodes and enhancing charge carrier mobility. High-polarity functional groups are commonly incorporated into CIMs designs to improve interfacial contact with the active layer and mitigate the power loss at metal electrodes. Herein, we report a hydrogen-bonding interfacial material, hydroxyethylamine-functionalized perylene diimide (PDIN-OH), which further reduces the cathode work function while maintaining excellent interfacial contact with the active layer. The outstanding conductivity of PDIN-OH, combined with its doping interaction with acceptor materials, significantly enhances its tolerance to thick films. In binary OSCs using the classical active layers PM6:Y6 and D18:L8-BO, devices incorporating PDIN-OH achieved remarkable power conversion efficiencies (PCEs) of 17.51 % and 19.36 %, respectively, along with outstanding stability. These findings indicate the potential of PDIN-OH as an efficient and stable CIM, offering a promising pathway to enhance OSC performance and promote their practical applications.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500119"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655802","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
Photocatalytic Nitrate Reduction to Ammonia via Zr-Mediated Proton-Coupled Electron Transfer. 通过zr介导的质子耦合电子转移光催化硝酸还原为氨。
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202402630
Pedro J Jabalera-Ortiz, Alvaro M Rodriguez-Jimenez, Pablo Garrido-Barros
{"title":"Photocatalytic Nitrate Reduction to Ammonia via Zr-Mediated Proton-Coupled Electron Transfer.","authors":"Pedro J Jabalera-Ortiz, Alvaro M Rodriguez-Jimenez, Pablo Garrido-Barros","doi":"10.1002/cssc.202402630","DOIUrl":"10.1002/cssc.202402630","url":null,"abstract":"<p><p>The reduction of nitrate (NO<sub>3</sub> <sup>-</sup>) is a fundamentally exciting reaction with important environmental implications. From a mechanistic perspective, it involves the transfer of 8 e<sup>-</sup> and 9 H<sup>+</sup>, with the initial activation of NO<sub>3</sub> <sup>-</sup> representing a significant challenge. Here we propose a distinct and competitive mechanism for the redox activation of this inert anion based on photocatalytic proton-coupled electron transfer (PCET). The use of a PCET mediator based on a Zr coordination cage enabled formation of NH<sub>3</sub> under visible light irradiation (440 nm). Importantly, the incorporation of Li<sup>+</sup> as a Lewis acid within the cage structure further generated highly reactive sites that pre-associate and activate NO<sub>3</sub> <sup>-</sup>, enhancing the catalytic activity. We also show how the back oxidation of the intermediate NO<sub>2</sub> <sup>-</sup> has a dramatic impact in the efficiency and highlight the role of the sacrificial electron donor in outcompeting this side reaction. These aspects were finally combined with the use of silver as a d-block metal catalyst to facilitate the NO<sub>3</sub> <sup>-</sup> to NO<sub>2</sub> <sup>-</sup> reduction step, the identified bottleneck of the overall process.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402630"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655856","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
Polyvinylidene Fluoride-networked Sb2S3/CdS/Ag2S Membrane with Dual-junction Exciton Dynamics for In-depth Purification of Textile Printing/Dyeing Wastewater. 双结激子动力学的聚偏氟乙烯网络Sb2S3/CdS/Ag2S膜深度净化纺织印染废水
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202500051
Hua Qin, Wei Li, Guocheng Liao, Jiayuan Li, Wen Duan, Tenghao Ma, Chuanyi Wang
{"title":"Polyvinylidene Fluoride-networked Sb<sub>2</sub>S<sub>3</sub>/CdS/Ag<sub>2</sub>S Membrane with Dual-junction Exciton Dynamics for In-depth Purification of Textile Printing/Dyeing Wastewater.","authors":"Hua Qin, Wei Li, Guocheng Liao, Jiayuan Li, Wen Duan, Tenghao Ma, Chuanyi Wang","doi":"10.1002/cssc.202500051","DOIUrl":"10.1002/cssc.202500051","url":null,"abstract":"<p><p>The textile printing/dyeing (TPD) wastewater poses a serious threat to ecological safety, and it is essential and challenging to alleviate this environmental issue. The sunlight-driven catalysis technology is a promising strategy for wastewater purification. However, the photostability and recyclability of highly active photocatalysts are the main factors limiting its application in wastewater treatment. Herein, a double-shell Sb<sub>2</sub>S<sub>3</sub>/CdS/Ag<sub>2</sub>S (SCA) ternary nanorods with type-II and type-I exciton dynamics was constructed to prepare the polyvinylidene fluoride networked hybrid membrane (PVDF/SCA). Due to the synergistically interacted multi-phase interfaces and superior recyclability, this hybrid membrane exhibited excellent piezo-photocatalytic in-depth purification ability of industrial discharged TPD wastewater under the collaborative drives of ultrasonic mechanical energy and light energy following by a durably stable catalytic performance, surpassing most reported environmental photocatalysts. This study proposes a feasible strategy for in-depth treatment of industrial discharged TPD wastewater to acceptable levels for discharge.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202500051"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655858","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
In Situ/Operando Insights into the Selectivity of CH4/C2H4 in CO2 Electroreduction by Fine-Tuning the Composition of Cu/SiO2 Catalysts. Cu/SiO2催化剂对CO2电还原中CH4/C2H4选择性的原位/操作研究
IF 7.5 2区 化学
ChemSusChem Pub Date : 2025-03-18 DOI: 10.1002/cssc.202402461
Shen Yan, Shuyan Gong, Shengbo Zhang, Hao Sun, Hao Yu, Lang Chen, Jinyu Han, Hua Wang
{"title":"In Situ/Operando Insights into the Selectivity of CH4/C2H4 in CO2 Electroreduction by Fine-Tuning the Composition of Cu/SiO2 Catalysts.","authors":"Shen Yan, Shuyan Gong, Shengbo Zhang, Hao Sun, Hao Yu, Lang Chen, Jinyu Han, Hua Wang","doi":"10.1002/cssc.202402461","DOIUrl":"https://doi.org/10.1002/cssc.202402461","url":null,"abstract":"<p><p>Copper-silica-based catalysts have drawn much attention for the remarkable product selectivity in electrochemical CO2 reduction reaction, particularly towards CH4 and C2H4. However, there has been a lack of systematic studies exploring the underlying reasons for the selectivity differences. Herein, Cu/SiO2 catalysts with different Cu/Si ratio were controllably synthesized, enabling a selective CO2 electroreduction from CH4 to C2H4. Specifically, at a current density of 200 mA cm-2, Cu/SiO2-10 including majority of CuSiO3 facilitates the selective reduction of CO2 to CH4 with a high Faradaic ratio of CH4/C2H4 (7.2/1), whereas Cu/SiO2-50 primarily consisting of CuO exhibits a higher Faradaic ratio of C2H4/CH4 (17.9/1). XPS and in-situ Raman characterization revealed that CuSiO3 component in the catalysts serves as the active site remains stable and no valve state change occurred, while CuO component was reduced in situ to Cu0/Cu+ as active sites during the reaction. In-situ infrared spectroscopic and CO-TPD characterization further revealed that CuSiO3 has a stronger protonation capacity and promotes the direct protonation of adsorbed *CO species to CH4, while Cu0/Cu+ is more conducive to the C-C coupling between the intermediate species *CHO with adsorbed *CO species to form C2H4 due to the stronger CO adsorption capacity and higher coverage.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202402461"},"PeriodicalIF":7.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655758","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
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