电催化剂
材料科学
还原(数学)
氮气
芯(光纤)
壳体(结构)
氧还原反应
催化作用
碳纤维
无机化学
化学工程
物理化学
复合数
电极
电化学
复合材料
有机化学
化学
几何学
数学
工程类
作者
Yankun Wen,Tongde Wang,Jiace Hao,Zechao Zhuang,Guohua Gao,Feili Lai,Shuanglong Lu,Xiaofan Wang,Qi Kang,Guangming Wu,Mingliang Du,Han Zhu
标识
DOI:10.1002/adfm.202400849
摘要
Abstract The manipulation of surface catalytic sites has rarely been explored for metal borides, and the subsurface effects on the electrocatalytic activity of the nitrogen reduction reaction (NRR) remain unknown. Herein, this work develops a core–shell nanoparticle catalyst with a Pd core that ensures high electron transfer rates and an Pd 16 B 3 atomical shell that possess tunable active sites for regulating the NRR. The atomic structural evolution from Pd to Pd 16 B 3 is investigated by precisely controlling the B atom diffusion, molecular rearrangement, and d – sp orbital hybridization. Pd/Pd 16 B 3 core–shell nanocrystals exhibit an exceptional NRR performance with a high NH 3 Faradaic efficiency of 30.8%, which is superior to those of pristine Pd (1.2%) and B‐doped Pd (4.8%) under identical conditions, and a yield rate of 0.81 µmol h −1 cm −2 . This work discovers that the Pd 16 B 3 shell could promote the NRR selectivity by separating the separating the hydrogen evolution reaction proceeded on hole sites and NRR proceeded on bridge sites, and the Pd core could provide the excellent conductivity to Pd 16 B 3 shell through regulated electron interactions. Consequently, the controlled chemical ordering of palladium boride on palladium surfaces provides insight into the synthesis of advanced NRR electrocatalysts.
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