CO2 Electroreduction to Formate at a Partial Current Density up to 590 mA mg-1 via Micrometer-Scale Lateral Structuring of Bismuth Nanosheets
CO2 Electroreduction to Formate at a Partial Current Density up to 590 mA mg-1 via Micrometer-Scale Lateral Structuring of Bismuth Nanosheets
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通过铋纳米片的微米级横向结构，在高达 590 mA mg-1 的部分电流密度下进行 CO2 电还原生成甲酸盐
DOI：
10.1002/smll.202100602
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发表时间：
2021
期刊：
影响因子：
13.3
通讯作者：
Zhang Ying
中科院分区：
文献类型：
--
作者：
Wang Dan;Liu Chuangwei;Zhang Yaning;Wang Yanying;Wang Zhenlin;Ding Ding;Cui Yi;Zhu Xiangmiao;Pan Chengsi;Lou Yang;Li Fengwang;Zhu Yongfa;Zhang Ying
二维铋纳米片是一种很有前途的层状材料，用于通过电催化CO2转化产生甲酸盐。然而，铋纳米片在CO2电还原中的商业利益仍然是罕见的，这是由于甲酸盐在中等操作电位（约200 mA mg-1）和苛刻的合成条件（高温和/或高压）下的不期望的电流密度。本文报道了在常压和常温下，通过电化学阴极剥离法在水溶液中制备出横向尺寸为微米级的Bi纳米片。与最先进的结果相比，所制备的Bi LNS（L表示大的横向尺寸）在-0.44 V至-1.10 V（相对于RHE）的宽电位窗口内具有超过90%的高法拉第效率，并且对于甲酸盐具有约590 mA mg-1的上级部分电流密度。结构分析、电化学结果和密度泛函理论计算表明，随着Bi LNS中晶格拉伸应变的增加，d轨道重叠减少，d带宽度变窄，从而调节了中间结合能，提高了本征活性.
2D bismuth nanosheets are a promising layered material for formate‐producing via electrocatalytic CO2conversion. However, the commercial interest of bismuth nanosheets in CO2electroreduction is still rare due to the undesirable current density for formate at moderate operation potentials (about 200 mA mg−1) and harsh synthesis conditions (high temperature and/or high pressure). This work reports the preparation of Bi nanosheets with a lateral size in micrometer‐scale via electrochemical cathodic exfoliation in aqueous solution at normal pressure and temperature. As‐prepared Bi LNSs (L indicates large lateral size) possess high Faradaic efficiencies over 90% within a broad potential window from −0.44 to −1.10 V versus RHE and a superior partial current density about 590 mA mg−1for formate in comparison with state‐of‐the‐art results. Structure analysis, electrochemical results, and density functional theory calculations demonstrate that the increasing tensile lattice strain observed in Bi LNSs leads to less overlap of d orbitals and a narrower d‐band width, which tuning the intermediate binding energies, and therefore promotes the intrinsic activity.