研究人员报道了一种基于铁磁性六方密排(hcp)Co纳米片(NSs)的新型催化剂,用于选择性地将CO2RR转化为乙醛,CH3CHO。在0.5 M KHCO3溶液中从0.2至1.0 V(vs RHE)测试的所有还原电位中,还原产生的主要产物为乙醛,次要产物为乙醇/甲醇。在0.4 V下,乙醛的法拉第效率(FE)达到60%,电流密度为5.1 mA cm–2,质量活度为3.4 A g–1(乙醛/乙醇/甲醇的总FE为82%)。
密度泛函理论(DFT)计算表明,hcp-Co表面对乙醛的高CO2RR选择性归因于独特的层内电子转移,其不仅促进[OC–Co]*偶联,而且抑制偶联中间体完全氢化为乙烯,导致CH3CHO的高选择性形成。
附:英文原文
Title: A New Hexagonal Cobalt Nanosheet Catalyst for Selective CO2 Conversion to Ethanal
Author: Jie Yin, Zhouyang Yin, Jing Jin, Mingzi Sun, Bolong Huang, Honghong Lin, Zhenhui Ma, Michelle Muzzio, Mengqi Shen, Chao Yu, Hong Zhang, Yong Peng, Pinxian Xi, Chun-Hua Yan, Shouheng Sun
Issue&Volume: September 14, 2021
Abstract: We report a new form of catalyst based on ferromagnetic hexagonal-close-packed (hcp) Co nanosheets (NSs) for selective CO2RR to ethanal, CH3CHO. In all reduction potentials tested from 0.2 to 1.0 V (vs RHE) in 0.5 M KHCO3 solution, the reduction yields ethanal as a major product and ethanol/methanol as minor products. At 0.4 V, the Faradaic efficiency (FE) for ethanal reaches 60% with current densities of 5.1 mA cm–2 and mass activity of 3.4 A g–1 (total FE for ethanal/ethanol/methanol is 82%). Density functional theory (DFT) calculations suggest that this high CO2RR selectivity to ethanal on the hcp Co surface is attributed to the unique intralayer electron transfer, which not only promotes [OC–CO]* coupling but also suppresses the complete hydrogenation of the coupling intermediates to ethylene, leading to highly selective formation of CH3CHO.
DOI: 10.1021/jacs.1c06877
Source: https://pubs.acs.org/doi/10.1021/jacs.1c06877
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:14.612
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