硝酸盐
吸附
催化作用
过渡金属
掺杂剂
氨
电化学
氨生产
电子转移
电解质
法拉第效率
无机化学
化学
材料科学
化学工程
电极
光化学
兴奋剂
物理化学
有机化学
光电子学
工程类
作者
Yuanbo Zhou,Lifang Zhang,Zhi‐Jun Zhu,Mengfan Wang,Najun Li,Tao Qian,Chenglin Yan,Jianmei Lu
标识
DOI:10.1002/anie.202319029
摘要
Electrochemical reduction of nitrate to ammonia (NO3RR) is a promising and eco-friendly strategy for ammonia production. However, the sluggish kinetics of the eight-electron transfer process and poor mechanistic understanding strongly impedes its application. To unveil the internal laws, herein, a library of Pd-based bimetallene with various transition metal dopants (PdM (M=Fe, Co, Ni, Cu)) are screened to learn their structure-activity relationship towards NO3RR. The ultra-thin structure of metallene greatly facilitates the exposure of active sites, and the transition metals dopants break the electronic balance and upshift its d-band center, thus optimizing intermediates adsorption. The anisotropic electronic characteristics of these transition metals make the NO3RR activity in the order of PdCu>PdCo≈PdFe>PdNi>Pd, and a record-high NH3 yield rate of 295 mg h-1 mgcat-1 along with Faradaic efficiency of 90.9 % is achieved in neutral electrolyte on PdCu bimetallene. Detailed studies further reveal that the moderate N-species (*NO3 and *NO2) adsorption ability, enhanced *NO activation, and reduced HER activity facilitate the NH3 production. We believe our results will give a systematic guidance to the future design of NO3RR catalysts.
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