电解质
原位
选择性
化学
电合成
氢
分子
无机化学
电化学
法拉第效率
联轴节(管道)
拉曼光谱
电极
还原(数学)
分析化学(期刊)
氧化还原
氢分子
催化作用
材料科学
磷酸
光化学
作者
Zihong Wang (1567717),Yecheng Li (1832878),Xin Zhao (71840),Shunqiang Chen (11593275),Qingshun Nian (6817307),Xuan Luo (270185),Jiajia Fan (343396),Digen Ruan (11885357),Bing-Qing Xiong (9537665),Xiaodi Ren (1471981)
出处
期刊:
[Figshare (United Kingdom)]
标识
DOI:10.1021/jacs.2c13384.s001
摘要
Electrocatalytic CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) is one of the most promising routes to facilitate carbon\nneutrality.\nAn alkaline electrolyte is typically needed to promote the production\nof valuable multi-carbon molecules (such as ethylene). However, the\nreaction between CO<sub>2</sub> and OH<sup>–</sup> consumes\na significant quantity of CO<sub>2</sub>/alkali and causes the rapid\ndecay of CO<sub>2</sub>RR selectivity and stability. Here, we design\na catalyst–electrolyte interface with an effective electrostatic\nconfinement of in situ generated OH<sup>–</sup> to improve\nethylene electrosynthesis from CO<sub>2</sub> in neutral medium. In\nsitu Raman measurements indicate the direct correlation between ethylene\nselectivity and the intensities of surface Cu–CO and Cu–OH\nspecies, suggesting the promoted C–C coupling with the surface\nenrichment of OH<sup>–</sup>. Thus, we report a CO<sub>2</sub>-to-ethylene Faradaic efficiency (FE) of 70% and a partial current\ndensity of 350 mA cm<sup>–2</sup> at −0.89 V vs the\nreversible hydrogen electrode. Furthermore, the system demonstrated\na 50 h stable operation at 300 mA cm<sup>–2</sup> with an average\nethylene FE of ∼68%. This study offers a universal strategy\nto tune the reaction micro-environment, and a significantly improved\nethylene FE of 64.5% was obtained even in acidic electrolytes (pH\n= 2).
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