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

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2023-07-05 DOI:10.1021/acscatal.3c01963

Kai Chen, Fuzhou Wang, Xubin Lu, Yunhe Li and Ke Chu*,

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引用次数: 11

Abstract

Electrocatalytic NO reduction to NH₃ (NORR) offers a prospective method for removing hazardous NO and producing valuable NH₃ simultaneously. Herein, we demonstrate that atomically dispersed W on Pd metallene (W₁Pd) can be an efficient and robust NORR catalyst. Atomic coordination characterizations unravel that W single atoms exist as W₁–O₃ moieties bonded on Pd metallene. In situ spectroscopic measurements and theoretical calculations reveal the synergistic cascade effect of W₁–O₃ and Pd metallene to promote the NORR energetics of W₁Pd, in which the activation and hydrogenation of NO occur on W₁–O₃, while Pd metallene dissociates H₂O and donates protons required for hydrogenation of NO to NH₃. Consequently, W₁Pd exhibits an NH₃ yield rate of 758.5 μmol h^–1 cm^–2 with an NH₃-Faradaic efficiency of 91.3% in a flow cell (272.1 μmol h^–1 cm^–2 and 93.7% in H-type cells), ranking almost the highest performance among all reported NORR catalysts.

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原子分散W1-O3键合在Pd金属烯上的级联NO电还原制NH3

电催化NO还原为NH3 (NORR)提供了去除有害NO和同时产生有价值NH3的有前途的方法。在此，我们证明了原子分散的W在Pd金属烯(W1Pd)上可以成为一种高效且坚固的NORR催化剂。原子配位表征表明，W单原子以W1-O3基团的形式存在于钯金属烯上。原位光谱测量和理论计算表明，W1-O3和钯金属烯的协同级联效应促进了W1Pd的NORR动力学，其中W1-O3上发生NO的活化和加氢，而钯金属烯解离H2O并将NO加氢所需的质子提供给NH3。结果表明，W1Pd的NH3产率为758.5 μmol h-1 cm-2, NH3-法拉第效率为91.3%(在h型电池中为272.1 μmol h-1 cm-2，在h型电池中为93.7%)，几乎是所有报道的NORR催化剂中性能最高的。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.