The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study,ACS Energy Letters

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The Predominance of Hydrogen Evolution on Transition Metal Sulfides and Phosphides under CO2 Reduction Conditions: An Experimental and Theoretical Study
ACS Energy Letters ( IF 19.3 ) Pub Date : 2018-05-31 00:00:00 , DOI: 10.1021/acsenergylett.8b00237
Alan T. Landers _{1,

2} , Meredith Fields _{2,

3} , Daniel A. Torelli ₄ , Jianping Xiao _{2,

3} , Thomas R. Hellstern _{2,

3} , Sonja A. Francis ₄ , Charlie Tsai _{2,

3} , Jakob Kibsgaard _{2,

3,

5} , Nathan S. Lewis ₄ , Karen Chan _{2,

3} , Christopher Hahn _{2,

3} , Thomas F. Jaramillo _{2,

3}

Affiliation

A combination of experiment and theory has been used to understand the relationship between the hydrogen evolution reaction (HER) and CO₂ reduction (CO₂R) on transition metal phosphide and transition metal sulfide catalysts. Although multifunctional active sites in these materials could potentially improve their CO₂R activity relative to pure transition metal electrocatalysts, under aqueous testing conditions, these materials showed a high selectivity for the HER relative to CO₂R. Computational results supported these findings, indicating that a limitation of the metal phosphide catalysts is that the HER is favored thermodynamically over CO₂R. On Ni-MoS₂, a limitation is the kinetic barrier for the proton–electron transfer to *CO. These theoretical and experimental results demonstrate that selective CO₂R requires electrocatalysts that possess both favorable thermodynamic pathways and surmountable kinetic barriers.

中文翻译：

在CO ₂还原条件下氢在过渡金属硫化物和磷酸盐上的逸出优势：实验和理论研究

实验和理论的结合已被用于理解在过渡金属磷化物和过渡金属硫化物催化剂上的氢释放反应（HER）和CO ₂还原（CO ₂ R）之间的关系。尽管这些材料中的多功能活性位点可以相对于纯过渡金属电催化剂潜在地提高其CO ₂ R活性，但是在水质测试条件下，这些材料对HER的选择性相对于CO ₂ R具有很高的选择性。计算结果支持了这些发现，表明金属磷化物催化剂的一个局限性是，热力学上HER比CO ₂ R更受青睐。在Ni-MoS _2上，一个限制是质子-电子转移到* CO的动力学障碍。这些理论和实验结果表明，选择性CO ₂ R需要具有良好的热力学路径和可克服的动力学障碍的电催化剂。

更新日期：2018-05-31

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