2D Metal Oxyhalide-Derived Catalysts for Efficient CO2 Electroreduction
2D Metal Oxyhalide-Derived Catalysts for Efficient CO2 Electroreduction
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DOI：
10.1002/adma.201802858
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发表时间：
2018-09-20
影响因子：
29.4
通讯作者：
Sargent, Edward H.
中科院分区：
文献类型：
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作者：
de Arquer, F. Pelayo Garcia;Bushuyev, Oleksandr S.;Sargent, Edward H.
以碳基燃料的形式储存可再生电力，电化学还原二氧化碳是一条引人注目的途径。有效的电化学还原CO2需要结合高活性、高选择性和低过电位的催化剂。在高生产率操作条件下（高电流密度、高还原电位和可变pH值），金属催化剂的广泛表面重构使得定制催化剂的实现更具挑战性，从而最大限度地暴露出最有利的方面、活性位点的数量和氧化态。地球上丰富的过渡金属，如锡、铋和铅，已被证明是稳定的和特定产品，但表现出有限的局部电流密度。本文报道了一种采用氧化卤化铋作为模板的策略，由此衍生出二维铋基催化剂。biobr模板催化剂表现出高活性Bi （1T0）面优先暴露。因此，CO2还原反应选择性提高到90%以上的法拉第效率，同时实现了高达200毫安厘米（-2）的稳定电流密度，与以前最好的Bi催化剂相比，储能液体甲酸的产量增加了两倍多。
Electrochemical reduction of CO2 is a compelling route to store renewable electricity in the form of carbon-based fuels. Efficient electrochemical reduction of CO2 requires catalysts that combine high activity, high selectivity, and low overpotential. Extensive surface reconstruction of metal catalysts under high productivity operating conditions (high current densities, reducing potentials, and variable pH) renders the realization of tailored catalysts that maximize the exposure of the most favorable facets, the number of active sites, and the oxidation state all the more challenging. Earth-abundant transition metals such as tin, bismuth, and lead have been proven stable and product-specific, but exhibit limited partial current densities. Here, a strategy that employs bismuth oxyhalides as a template from which 2D bismuth-based catalysts are derived is reported. The BiOBr-templated catalyst exhibits a preferential exposure of highly active Bi (1T0) facets. Thereby, the CO2 reduction reaction selectivity is increased to over 90% Faradaic efficiency and simultaneously stable current densities of up to 200 mA cm(-2) are achieved-more than a twofold increase in the production of the energy-storage liquid formic acid compared to previous best Bi catalysts.