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CO2电还原过程中Cu(100)Cu(111)界面作为CO二聚反应超活性中心的研究
作者:小柯机器人 发布时间:2021/12/31 13:56:45

中科大Min-Rui Gao小组的一项最新研究阐明了CO2电还原过程中Cu(100)Cu(111)界面作为CO二聚反应超活性中心。这一研究成果发表在2021年12月28日出版的国际学术期刊《美国化学会杂志》上。

在该文中,小组报道了在1 M KHCO3 (pH ~ 8.4)中,在商业相关电流密度(300 mA cm-2)的情况下,由6个{100}和8个{111}晶面包裹的氧化物衍生铜晶体可以将CO2还原为多碳产物,法拉第效率高达74.9 ± 1.7%。结合实验和计算研究,该研究组发现Cu(100)/Cu(111)界面提供了良好的局部电子结构,增强了*CO吸附,降低了C-C耦合活化能垒,分别优于Cu(100)和Cu(111)表面。在该催化剂上,在300 mA cm-2的条件下,连续运行50小时,没有观察到明显的催化剂降解。

据悉,以二氧化碳(CO2)为原料的有价值的多碳化合物的电合成近年来取得了很大进展,但仍面临着相当大的挑战。形成碳-碳(C-C)键的缓慢动力学是一个主要的困难,特别是在中性介质中。

附:英文原文

Title: Identification of Cu(100)/Cu(111) Interfaces as Superior Active Sites for CO Dimerization During CO2 Electroreduction

Author: Zhi-Zheng Wu, Xiao-Long Zhang, Zhuang-Zhuang Niu, Fei-Yue Gao, Peng-Peng Yang, Li-Ping Chi, Lei Shi, Wen-Sen Wei, Ren Liu, Zhi Chen, Shaojin Hu, Xiao Zheng, Min-Rui Gao

Issue&Volume: December 28, 2021

Abstract: The electrosynthesis of valuable multicarbon chemicals using carbon dioxide (CO2) as a feedstock has substantially progressed recently but still faces considerable challenges. A major difficulty lines in the sluggish kinetics of forming carbon–carbon (C–C) bonds, especially in neutral media. We report here that oxide-derived copper crystals enclosed by six {100} and eight {111} facets can reduce CO2 to multicarbon products with a high Faradaic efficiency of 74.9 ± 1.7% at a commercially relevant current density of 300 mA cm–2 in 1 M KHCO3 (pH ~ 8.4). By combining the experimental and computational studies, we uncovered that Cu(100)/Cu(111) interfaces offer a favorable local electronic structure that enhances *CO adsorption and lowers C–C coupling activation energy barriers, performing superior to Cu(100) and Cu(111) surfaces, respectively. On this catalyst, no obvious degradation was observed at 300 mA cm–2 over 50 h of continuous operation.

DOI: 10.1021/jacs.1c09508

Source: https://pubs.acs.org/doi/10.1021/jacs.1c09508

 

期刊信息

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
官方网址:https://pubs.acs.org/journal/jacsat
投稿链接:https://acsparagonplus.acs.org/psweb/loginForm?code=1000