Atomically Dispersed W1-O3 Bonded on Pd Metallene for Cascade NO Electroreduction to NH3

被引:50
作者
Chen, Kai [1 ]
Wang, Fuzhou [1 ]
Lu, Xubin [1 ]
Li, Yunhe [1 ]
Chu, Ke [1 ]
机构
[1] Lanzhou Jiaotong Univ, Sch Mat Sci & Engn, Lanzhou 730070, Peoples R China
基金
中国国家自然科学基金;
关键词
single-atom catalysts; metallenes; electrocatalyticNO reduction to NH3; in situ spectroscopic measurements; theoretical calculations; SINGLE-ATOM CATALYSTS; OXIDE; NANOPARTICLES;
D O I
10.1021/acscatal.3c01963
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Electrocatalytic NO reduction to NH3 (NORR)offers aprospective method for removing hazardous NO and producing valuableNH(3) simultaneously. Herein, we demonstrate that atomicallydispersed W on Pd metallene (W1Pd) can be an efficientand robust NORR catalyst. Atomic coordination characterizations unravelthat W single atoms exist as W-1-O-3 moietiesbonded on Pd metallene. In situ spectroscopic measurements and theoreticalcalculations reveal the synergistic cascade effect of W-1-O-3 and Pd metallene to promote the NORR energeticsof W1Pd, in which the activation and hydrogenation of NOoccur on W-1-O-3, while Pd metallene dissociatesH(2)O and donates protons required for hydrogenation of NOto NH3. Consequently, W1Pd exhibits an NH3 yield rate of 758.5 & mu;mol h(-1) cm(-2) with an NH3-Faradaic efficiency of 91.3%in a flow cell (272.1 & mu;mol h(-1) cm(-2) and 93.7% in H-type cells), ranking almost the highest performanceamong all reported NORR catalysts.
引用
收藏
页码:9550 / 9557
页数:8
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