Phase-Dependent Electrochemical CO2 Reduction Ability of NiSn Alloys for Formate Generation-猫眼课题宝

DOI：

10.1021/acsaem.1c01207

发表时间：

2021-07

期刊：

ACS Applied Energy Materials

影响因子：

6.4

通讯作者：

中科院分区：

材料科学3区

文献类型：

作者：

Yoshikazu Ito;Suresh Kukunuri;Samuel Jeong;G. Elumalai;Aimi Asilah Haji Tajuddin;Zeyu Xi;Kailong Hu;Tatsuhiko Ohto

双金属合金是一种重要的催化剂，具有更高的催化活性和产物选择性。然而，双金属合金中催化活性的相关系呈现出一相催化主反应和另一相催化副反应的矛盾特征，这方面的双金属合金催化剂还没有得到研究。在本研究中，我们以催化制氢活性的镍和催化二氧化碳电化学还原活性的锡为原料，系统地合成了镍锡合金。将所制备的合金用于催化CO2的相依赖电化学还原，并对甲酸盐的生成机理进行了探讨。结果表明，甲酸盐的法拉第效率随锡原子浓度的增加而增加，Ni3Sn4对CO2的电化学还原表现出比单一锡更高的催化活性。密度泛函理论计算表明，Ni还可以在合适的相中为甲酸盐的生成提供催化活性中心。因此，我们的研究使我们更好地了解了由不同性质的金属制备的双金属合金对二氧化碳电化学还原的催化活性。

Bimetallic alloys are important catalysts with enhanced catalytic activities and product selectivities. However, the phase dependence of catalytic activity in bimetallic alloys afford contradictory characters in that one phase catalyzes the main reaction and the other catalyzes the side reaction; this aspect of bimetallic alloy catalysts has not been investigated. In this study, we systematically synthesized NiSn alloys from Ni, which is catalytically active in hydrogen generation, and Sn, which is catalytically active in electrochemical CO2reduction. The thus-prepared alloys were applied in catalyzing the phase-dependent electrochemical CO2reduction, and the formate generation mechanism was elucidated. The Faradaic efficiency of formate was found to increase with increasing Sn atomic concentration, and Ni3Sn4showed higher catalytic activity than only Sn for electrochemical CO2reduction. Density functional theory calculations revealed that Ni can additionally provide catalytically active sites for formate generation in a suitable phase. Thus, our investigation brings a better understanding of the catalytic activities of bimetallic alloys prepared from metals with different characters for electrochemical CO2reduction.

Phase-Dependent Electrochemical CO2 Reduction Ability of NiSn Alloys for Formate Generation

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