Promoting electrocatalytic CO2 reduction to formate via sulfur-boosting water activation on indium surfaces

Promoting electrocatalytic CO2 reduction to formate via sulfur-boosting water activation on indium surfaces
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通过铟表面的硫促进水活化促进电催化二氧化碳还原为甲酸盐

DOI:
10.1038/s41467-019-08805-x
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发表时间:
2019-02-21
影响因子:
16.6
通讯作者:
Wang, Ye
Wang, Ye
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Ma, Wenchao;Xie, Shunji;Wang, Ye

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电催化将二氧化碳还原为燃料和化学品是二氧化碳利用最具吸引力的途径之一。目前的催化剂在高电流密度(或反应速率)下,co2还原产物的法拉第效率较低。在这里,我们报道了一种硫掺杂铟催化剂在宽电流密度范围内(25-100 mA cm−2)表现出高甲酸的法拉第效率(85%),用于水介质中电催化CO2还原。甲酸的生成速率达到1449 μmol h−1 cm−2,法拉第效率为93%,是迄今为止报道的最高值。我们的研究表明,硫通过一种独特的机制加速了二氧化碳的减少。硫提高了水的活性,形成氢,氢可以很容易地与二氧化碳反应产生甲酸。硫改性剂的促进作用可推广到其他金属催化剂。这项工作为设计活性和选择性的二氧化碳还原电催化剂提供了一种简单而有用的策略。
Electrocatalytic reduction of CO2 to fuels and chemicals is one of the most attractive routes for CO2 utilization. Current catalysts suffer from low faradaic efficiency of a CO2-reduction product at high current density (or reaction rate). Here, we report that a sulfur-doped indium catalyst exhibits high faradaic efficiency of formate (85%) in a broad range of current density (25–100 mA cm−2) for electrocatalytic CO2 reduction in aqueous media. The formation rate of formate reaches 1449 μmol h−1 cm−2 with 93% faradaic efficiency, the highest value reported to date. Our studies suggest that sulfur accelerates CO2 reduction by a unique mechanism. Sulfur enhances the activation of water, forming hydrogen species that can readily react with CO2 to produce formate. The promoting effect of chalcogen modifiers can be extended to other metal catalysts. This work offers a simple and useful strategy for designing both active and selective electrocatalysts for CO2 reduction.