Trends in the Catalytic Activity of Hydrogen Evolution during CO2 Electroreduction on Transition Metals,ACS Catalysis

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Trends in the Catalytic Activity of Hydrogen Evolution during CO2 Electroreduction on Transition Metals
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-03-09 00:00:00 , DOI: 10.1021/acscatal.7b03807
Etosha R. Cave _{1,

2} , Chuan Shi _{1,

2} , Kendra P. Kuhl _{1,

2} , Toru Hatsukade _{1,

2} , David N. Abram _{1,

2} , Christopher Hahn _{1,

2} , Karen Chan _{1,

2} , Thomas F. Jaramillo _{1,

2}

Affiliation

During CO₂ electroreduction (CO₂R), the hydrogen evolution reaction (HER) is a competing reaction. We present a combined experimental and theoretical investigation of the HER activity of transition metals under CO₂R conditions. Experimental HER polarization curves were measured for six polycrystalline metal surfaces (Au, Ag, Cu, Ni, Pt, and Fe) in the presence of CO₂ gas. We found that the HER activity of the transition metals is significantly shifted, relative to the CO₂-free case. Density functional theory (DFT) calculations suggest that this shift arises from adsorbate–adsorbate interactions between *CO and *H on intermediate and strong binding metals, which weakens the *H binding energy. Using a simple model for the effect of *CO on the *H binding energy, we construct an activity volcano for HER in the presence of CO₂ gas that is consistent with experimental trends. The significant changes in HER activity in the presence of CO₂ gas is an important consideration in catalyst design and could help develop catalysts that are more selective for CO₂R than the HER.

中文翻译：

过渡金属在CO ₂电还原过程中析氢的催化活性趋势

在CO ₂电还原（CO ₂ R）过程中，析氢反应（HER）是竞争反应。我们提出了在CO ₂ R条件下过渡金属的HER活性的组合实验和理论研究。在存在CO ₂气体的情况下，针对六个多晶金属表面（Au，Ag，Cu，Ni，Pt和Fe）测量了HER极化实验曲线。我们发现，过渡金属的HER活性相对于CO ₂发生了显着变化-无案。密度泛函理论（DFT）的计算表明，这种转变是由于* CO和* H在中间和强结合金属上的吸附物-吸附物相互作用而产生的，这削弱了* H的结合能。使用简单的* CO对* H结合能影响的模型，我们在存在CO ₂气体的情况下构建了与实验趋势一致的HER活火山。在存在CO ₂气体的情况下，HER活性的显着变化是催化剂设计中的重要考虑因素，并且可以帮助开发对HER _2的选择性比HER高的催化剂。

更新日期：2018-03-09

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