氨生产
价(化学)
电化学
可逆氢电极
氨
纳米技术
选择性
氮气
氢
吸附
催化作用
解吸
材料科学
化学
氧化还原
电极
无机化学
工作电极
有机化学
物理化学
作者
Jianyun Zheng,Yanhong Lyu,Man Qiao,Jean Pierre Veder,Roland De Marco,John L. Bradley,Ruilun Wang,Yafei Li,Aibin Huang,San Ping Jiang,Shuangyin Wang
标识
DOI:10.1002/anie.201909477
摘要
The (photo)electrochemical N2 reduction reaction (NRR) provides a favorable avenue for the production of NH3 using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH3 selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoOx layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N2 to NH3 . The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH3 yield rate of 15.1 μg cm-2 h-1 and a good faradic efficiency of 19 % at -0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N2 adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH3 .
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