Catalyst Particle Density Controls Hydrocarbon Product Selectivity in CO2 Electroreduction on CuOx.
Catalyst Particle Density Controls Hydrocarbon Product Selectivity in CO2 Electroreduction on CuOx.
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DOI：
10.1002/cssc.201701179
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发表时间：
2017-11
期刊：
影响因子：
8.4
通讯作者：
Xingli Wang;A. Varela;A. Bergmann;S. Kühl;P. Strasser
中科院分区：
文献类型：
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作者：
Xingli Wang;A. Varela;A. Bergmann;S. Kühl;P. Strasser
铜基纳米颗粒上二氧化碳电还原（CO2RR）的一个关键挑战是其对高价值产物（如乙烯）的低faradic选择性。在这里，我们展示了一种简单的方法，通过改变纳米颗粒的面密度来调节CuOx纳米颗粒系综上的碳氢化合物选择性。实验乙烯选择性对催化剂颗粒面密度的敏感依赖归因于颗粒间的扩散耦合，这种耦合控制了CO的脱吸附和再吸附，从而有效地覆盖了COad中间体。因此，较高的面密度构成了CO再吸附和*CO二聚化的动态有利条件，导致乙烯的形成不受pH和施加过电位的影响。
A key challenge of the carbon dioxide electroreduction (CO2RR) on Cu-based nanoparticles is its low faradic selectivity toward higher-value products such as ethylene. Here, we demonstrate a facile method for tuning the hydrocarbon selectivities on CuOx nanoparticle ensembles by varying the nanoparticle areal density. The sensitive dependence of the experimental ethylene selectivity on catalyst particle areal density is attributed to a diffusional interparticle coupling that controls the de- and re-adsorption of CO and thus the effective coverage of COad intermediates. Thus, higher areal density constitutes dynamically favored conditions for CO re-adsorption and *CO dimerization leading to ethylene formation independent of pH and applied overpotential.