Electrochemical reduction of SnO2 to Sn from the Bottom: In-Situ formation of SnO2/Sn heterostructure for highly efficient electrochemical reduction of carbon dioxide to formate
Electrochemical reduction of SnO2 to Sn from the Bottom: In-Situ formation of SnO2/Sn heterostructure for highly efficient electrochemical reduction of carbon dioxide to formate
复制标题
从底部将 SnO2 电化学还原为 Sn：原位形成 SnO2/Sn 异质结构，用于高效电化学还原二氧化碳生成甲酸盐
DOI：
10.1016/j.jcat.2021.04.028
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发表时间：
2021-07
影响因子：
7.3
通讯作者：
Kang Xiongwu
中科院分区：
文献类型：
--
作者：
Ning Shunlian;Wang Jigang;Xiang Dong;Huang Shaobin;Chen Wei;Chen Shaowei;Kang Xiongwu
设计和制造低成本、高性能的催化剂是电化学二氧化碳还原(CO2R)生产附加值化学品和燃料的关键步骤。本论文采用简单的水热法制备了SnO2/Cf/SnO2纳米粒子，通过在CO2R电解过程中生成SnO2/SnMott-Schottky异质结，表现出良好的电催化活性，X射线衍射、X射线光电子能谱和拉曼光谱测试表明，SnO2纳米粒子对CO2R具有良好的电催化活性。异质结构SnO2/SnO_2电极在H型电池(保持稳定9小时)中的可逆氢电极和174.86 mA/cm−_2的气体扩散电极上，在流动电池中的气体扩散电极上产生甲酸盐的部分电流密度为28.7 mA/cm−_2和28.7 mA/cm−_2，在H型电池中的可逆氢电极中(保持9小时的稳定)，法拉第效率为93±0.01%，部分电流密度为28.7 mA/cm−_2。密度泛函理论计算表明，在CO2R条件下原位生成的SnO2/Sn异质结构与原始SnO2和Sn2+相比，有助于降低生成甲酸盐的势垒，是甲酸盐生成的高活性和高选择性的原因。这一研究结果揭示了SnO2催化剂在CO2R条件下的演化动力学，为进一步了解SnO2催化剂在CO2R中的活性成分提供了依据。
Design and engineering of low-cost, high-performance catalysts is a critical step in electrochemical CO2reduction (CO2R) to value-added chemicals and fuels. Herein, SnO2nanoparticles were grown onto carbon cloth (SnO2/CF) by a facile hydrothermal procedure and exhibited excellent electrocatalytic activity towards CO2R due to reconstruction into SnO2/Sn Mott-Schottky heterojunctions during CO2R electrolysis, as manifested in X-ray diffraction, X-ray photoelectron spectroscopy, and operando Raman spectroscopy measurements. The heterostructured SnO2/Sn electrode delivered a high faradaic efficiency of 93 ± 1% and a partial current density of 28.7 mA cm−2for formate production at − 1.0 V vs. reversible hydrogen electrode in an H-type cell (which remained stable for 9 h), and 174.86 mA cm−2at − 1.18 V on a gas-diffusion electrode in a flow cell. Density functional theory calculations show that the SnO2/Sn heterostructures in situ formed under CO2R conditions helped decrease the energy barrier to form formate as compared to pristine SnO2and Sn, and were responsible for the high activity and selectivity of formate production. Results from this study unravels the evolution dynamics of SnO2catalysts under CO2R condition and provides a further understanding of the active component of SnO2catalyst in CO2R.
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影响因子：
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作者：
Li C;Zheng M;Wang X;Yao L;Ma L;Shen W
通讯作者：
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影响因子：
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作者：
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作者：
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影响因子：
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作者：
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通讯作者：
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