{"title":"通过电化学重构制备的银基催化材料用于高效二氧化碳还原","authors":"Fangshi Fan, Wei Ding, Lingjie Zhang, Junjun Xu, Weiwei Cai, Ningzhong Bao","doi":"10.1007/s11664-024-11323-2","DOIUrl":null,"url":null,"abstract":"<p>Silver-based catalytic materials have garnered considerable attention due to their high selectivity towards carbon monoxide (CO) in the electrochemical reduction (ECR) of CO<sub>2</sub>. However, the fabrication of silver-based ECR catalysts with high product selectivity and low competitive reaction activity using facile methods remains challenging. This study employed in situ electrochemical reconstruction to design high-performance silver-based catalytic materials for ECR, exploring performance enhancement mechanisms. Low-temperature electrochemical reconstruction was used to prepare silver-based catalysts, and the effects of metal ion chelating agents including ethylenediaminetetraacetic acid, citric acid, and sodium citrate were also investigated. Results showed that Ag-SC, namely the catalysts fabricated with sodium citrate as chelating agent, exhibited highly selective CO production, with faradaic efficiency of 93.23% at −0.85 V (versus reversible hydrogen electrode, RHE) and CO partial current density of −7.92 mA cm<sup>−2</sup>. Electrochemical impedance analysis confirmed low electron transfer resistance of Ag-SC, with 14.54 Ω, indicating superior electron transfer capability, and high ECR activity. Ag-SC also demonstrated excellent hydrophobicity, suppressing the competitive hydrogen evolution reaction and enhancing CO selectivity. In situ electrochemical reconstruction thus offers a simple, low-cost method for preparing silver-based catalysts tailored for ECR, with practical implications for electrode fabrication and catalytic material design.</p><h3 data-test=\"abstract-sub-heading\">Graphical Abstract</h3>","PeriodicalId":626,"journal":{"name":"Journal of Electronic Materials","volume":"10 1","pages":""},"PeriodicalIF":2.2000,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Silver-Based Catalytic Materials Prepared via Electrochemical Reconstruction for Efficient Carbon Dioxide Reduction\",\"authors\":\"Fangshi Fan, Wei Ding, Lingjie Zhang, Junjun Xu, Weiwei Cai, Ningzhong Bao\",\"doi\":\"10.1007/s11664-024-11323-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Silver-based catalytic materials have garnered considerable attention due to their high selectivity towards carbon monoxide (CO) in the electrochemical reduction (ECR) of CO<sub>2</sub>. However, the fabrication of silver-based ECR catalysts with high product selectivity and low competitive reaction activity using facile methods remains challenging. This study employed in situ electrochemical reconstruction to design high-performance silver-based catalytic materials for ECR, exploring performance enhancement mechanisms. Low-temperature electrochemical reconstruction was used to prepare silver-based catalysts, and the effects of metal ion chelating agents including ethylenediaminetetraacetic acid, citric acid, and sodium citrate were also investigated. Results showed that Ag-SC, namely the catalysts fabricated with sodium citrate as chelating agent, exhibited highly selective CO production, with faradaic efficiency of 93.23% at −0.85 V (versus reversible hydrogen electrode, RHE) and CO partial current density of −7.92 mA cm<sup>−2</sup>. Electrochemical impedance analysis confirmed low electron transfer resistance of Ag-SC, with 14.54 Ω, indicating superior electron transfer capability, and high ECR activity. Ag-SC also demonstrated excellent hydrophobicity, suppressing the competitive hydrogen evolution reaction and enhancing CO selectivity. 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引用次数: 0
摘要
银基催化材料在二氧化碳的电化学还原(ECR)过程中对一氧化碳(CO)具有高选择性,因而备受关注。然而,使用简便的方法制造具有高产物选择性和低竞争反应活性的银基 ECR 催化剂仍然具有挑战性。本研究利用原位电化学重构技术设计了用于 ECR 的高性能银基催化材料,并探索了性能增强机制。研究采用低温电化学重构法制备银基催化剂,并考察了乙二胺四乙酸、柠檬酸和柠檬酸钠等金属离子螯合剂的影响。结果表明,Ag-SC(即以柠檬酸钠为螯合剂制备的催化剂)表现出高选择性的 CO 生成,在 -0.85 V(相对于可逆氢电极 RHE)时的远电效率为 93.23%,CO 部分电流密度为 -7.92 mA cm-2。电化学阻抗分析证实,Ag-SC 的电子转移电阻较低,仅为 14.54 Ω,这表明其具有出色的电子转移能力和较高的 ECR 活性。Ag-SC 还表现出优异的疏水性,抑制了竞争性氢进化反应,提高了 CO 选择性。因此,原位电化学重构为制备适合 ECR 的银基催化剂提供了一种简单、低成本的方法,对电极制造和催化材料设计具有实际意义。
Silver-Based Catalytic Materials Prepared via Electrochemical Reconstruction for Efficient Carbon Dioxide Reduction
Silver-based catalytic materials have garnered considerable attention due to their high selectivity towards carbon monoxide (CO) in the electrochemical reduction (ECR) of CO2. However, the fabrication of silver-based ECR catalysts with high product selectivity and low competitive reaction activity using facile methods remains challenging. This study employed in situ electrochemical reconstruction to design high-performance silver-based catalytic materials for ECR, exploring performance enhancement mechanisms. Low-temperature electrochemical reconstruction was used to prepare silver-based catalysts, and the effects of metal ion chelating agents including ethylenediaminetetraacetic acid, citric acid, and sodium citrate were also investigated. Results showed that Ag-SC, namely the catalysts fabricated with sodium citrate as chelating agent, exhibited highly selective CO production, with faradaic efficiency of 93.23% at −0.85 V (versus reversible hydrogen electrode, RHE) and CO partial current density of −7.92 mA cm−2. Electrochemical impedance analysis confirmed low electron transfer resistance of Ag-SC, with 14.54 Ω, indicating superior electron transfer capability, and high ECR activity. Ag-SC also demonstrated excellent hydrophobicity, suppressing the competitive hydrogen evolution reaction and enhancing CO selectivity. In situ electrochemical reconstruction thus offers a simple, low-cost method for preparing silver-based catalysts tailored for ECR, with practical implications for electrode fabrication and catalytic material design.
期刊介绍:
The Journal of Electronic Materials (JEM) reports monthly on the science and technology of electronic materials, while examining new applications for semiconductors, magnetic alloys, dielectrics, nanoscale materials, and photonic materials. The journal welcomes articles on methods for preparing and evaluating the chemical, physical, electronic, and optical properties of these materials. Specific areas of interest are materials for state-of-the-art transistors, nanotechnology, electronic packaging, detectors, emitters, metallization, superconductivity, and energy applications.
Review papers on current topics enable individuals in the field of electronics to keep abreast of activities in areas peripheral to their own. JEM also selects papers from conferences such as the Electronic Materials Conference, the U.S. Workshop on the Physics and Chemistry of II-VI Materials, and the International Conference on Thermoelectrics. It benefits both specialists and non-specialists in the electronic materials field.
A journal of The Minerals, Metals & Materials Society.