{"title":"具有高C2+选择性的多孔铜-聚四氟乙烯杂化电催化剂","authors":"Yoshitomo Seki, Mamiko Nakabayashi, Masakazu Sugiyama, Tsutomu Minegishi","doi":"10.1002/celc.202400536","DOIUrl":null,"url":null,"abstract":"<p>The electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to ethylene (C<sub>2</sub>H<sub>4</sub>) is one of the most promising approaches to obtaining value-added C<sub>2+</sub> hydrocarbons without net CO<sub>2</sub> emission. However, issues still to be solved for practical use include the improvement of Faradaic efficiency (FE) towards C<sub>2</sub>H<sub>4</sub>, electrode durability, and suppression of competitive hydrogen evolution reaction (HER). In this work, hydrophobic polymer, polytetrafluoroethylene (PTFE), added porous Cu electrocatalysts were firstly and successfully prepared on gas diffusion layer, and the significant enhancement of FEs toward C<sub>2+</sub> products, especially C<sub>2</sub>H<sub>4</sub>, and durability were found. CO<sub>2</sub>RR test in flow cell as a gas diffusion electrode (GDE) revealed that the GDE with porous Cu electrocatalysts showed higher FE(C<sub>2</sub>H<sub>4</sub>) to FE(CO) while significant HER and instability issues remained. Further modification by PTFE to form porous Cu-PTFE hybrid structure significantly decreased FE(H<sub>2</sub>) to 11.6 % in minimum, enhanced FE(C<sub>2</sub>H<sub>4</sub>) to 51.1 % in maximum and raised durable CO<sub>2</sub>RR for over 24 hours under current density of −300 mA cm<sup>−2</sup>. PTFE addition should form a secured pathway for gas species, including both reactant and product which was beneficial for durable and selective C<sub>2</sub>H<sub>4</sub> production. This work highlights chemical engineering aspects of CO<sub>2</sub>RR including the transportation of reactants and products.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 2","pages":""},"PeriodicalIF":3.5000,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202400536","citationCount":"0","resultStr":"{\"title\":\"Porous Copper-PTFE Hybrid Electrocatalyst for CO2 Reduction with High C2+ Selectivity\",\"authors\":\"Yoshitomo Seki, Mamiko Nakabayashi, Masakazu Sugiyama, Tsutomu Minegishi\",\"doi\":\"10.1002/celc.202400536\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to ethylene (C<sub>2</sub>H<sub>4</sub>) is one of the most promising approaches to obtaining value-added C<sub>2+</sub> hydrocarbons without net CO<sub>2</sub> emission. However, issues still to be solved for practical use include the improvement of Faradaic efficiency (FE) towards C<sub>2</sub>H<sub>4</sub>, electrode durability, and suppression of competitive hydrogen evolution reaction (HER). In this work, hydrophobic polymer, polytetrafluoroethylene (PTFE), added porous Cu electrocatalysts were firstly and successfully prepared on gas diffusion layer, and the significant enhancement of FEs toward C<sub>2+</sub> products, especially C<sub>2</sub>H<sub>4</sub>, and durability were found. CO<sub>2</sub>RR test in flow cell as a gas diffusion electrode (GDE) revealed that the GDE with porous Cu electrocatalysts showed higher FE(C<sub>2</sub>H<sub>4</sub>) to FE(CO) while significant HER and instability issues remained. Further modification by PTFE to form porous Cu-PTFE hybrid structure significantly decreased FE(H<sub>2</sub>) to 11.6 % in minimum, enhanced FE(C<sub>2</sub>H<sub>4</sub>) to 51.1 % in maximum and raised durable CO<sub>2</sub>RR for over 24 hours under current density of −300 mA cm<sup>−2</sup>. PTFE addition should form a secured pathway for gas species, including both reactant and product which was beneficial for durable and selective C<sub>2</sub>H<sub>4</sub> production. 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引用次数: 0
摘要
电化学CO2还原反应(CO2RR)制乙烯(C2H4)是获得无净CO2排放的高附加值C2+烃的最有前途的方法之一。然而,实际应用中仍有待解决的问题包括提高对C2H4的法拉第效率(FE)、电极耐久性和抑制竞争性析氢反应(HER)。本文首次在气体扩散层上成功制备了疏水聚合物聚四氟乙烯(PTFE)和添加多孔Cu的电催化剂,并发现了FEs对C2+产物,特别是C2H4的显著增强和耐久性。流动电池气体扩散电极(GDE)的CO2RR测试表明,多孔Cu电催化剂的GDE具有较高的FE(C2H4)到FE(CO),但仍存在明显的HER和不稳定性问题。PTFE进一步改性后,形成多孔Cu-PTFE杂化结构,FE(H2)最低降低至11.6%,FE(C2H4)最高提高至51.1%,在−300 mA cm−2电流密度下,CO2RR持续时间超过24小时。加注聚四氟乙烯应形成一个安全的气体通道,包括反应物和产物,这有利于持久和选择性的C2H4生产。这项工作强调了CO2RR的化学工程方面,包括反应物和产物的运输。
Porous Copper-PTFE Hybrid Electrocatalyst for CO2 Reduction with High C2+ Selectivity
The electrochemical CO2 reduction reaction (CO2RR) to ethylene (C2H4) is one of the most promising approaches to obtaining value-added C2+ hydrocarbons without net CO2 emission. However, issues still to be solved for practical use include the improvement of Faradaic efficiency (FE) towards C2H4, electrode durability, and suppression of competitive hydrogen evolution reaction (HER). In this work, hydrophobic polymer, polytetrafluoroethylene (PTFE), added porous Cu electrocatalysts were firstly and successfully prepared on gas diffusion layer, and the significant enhancement of FEs toward C2+ products, especially C2H4, and durability were found. CO2RR test in flow cell as a gas diffusion electrode (GDE) revealed that the GDE with porous Cu electrocatalysts showed higher FE(C2H4) to FE(CO) while significant HER and instability issues remained. Further modification by PTFE to form porous Cu-PTFE hybrid structure significantly decreased FE(H2) to 11.6 % in minimum, enhanced FE(C2H4) to 51.1 % in maximum and raised durable CO2RR for over 24 hours under current density of −300 mA cm−2. PTFE addition should form a secured pathway for gas species, including both reactant and product which was beneficial for durable and selective C2H4 production. This work highlights chemical engineering aspects of CO2RR including the transportation of reactants and products.
期刊介绍:
ChemElectroChem is aimed to become a top-ranking electrochemistry journal for primary research papers and critical secondary information from authors across the world. The journal covers the entire scope of pure and applied electrochemistry, the latter encompassing (among others) energy applications, electrochemistry at interfaces (including surfaces), photoelectrochemistry and bioelectrochemistry.