Asymmetric Coordination of Iridium Single‐atom IrN3O Boosting Formic Acid Oxidation Catalysis

Author:

Wang Lei12,Ji Bifa1,Zheng Yongping1ORCID,Tang Yongbing13ORCID

Affiliation:

1. Advanced Energy Storage Technology Research Center Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences Shenzhen 518055 China

2. Nano Science and Technology Institute University of Science and Technology of China Suzhou 215123 China

3. University of Chinese Academy of Sciences Beijing 100049 China

Abstract

AbstractRational design of the proximal coordination of an active site to achieve its optimum catalytic activity is the ultimate goal in single‐atom catalysis, but still challenging. Here, we report theoretical prediction and experimental realization of an asymmetrically coordinated iridium single‐atom catalyst (IrN3O) for the formic acid oxidation reaction (FAOR). Theoretical calculations reveal that the substitution of one or two nitrogen with more electronegative oxygen in the symmetric IrN4 motif splits and downshifts the Ir 5d orbitals with respect to the Fermi level, moderating the binding strength of key intermediates on IrN4−xOx (x=1, 2) sites, especially that the IrN3O motif shows ideal activity for FAOR with a near‐zero overpotential. The as‐designed asymmetric Ir motifs were realized by pyrolyzing Ir precursor with oxygen‐rich glucose and nitrogen‐rich melamine, exhibiting a mass activity of 25 and 87 times greater than those of state‐of‐the‐art Pd/C and Pt/C, respectively.

Funder

National Key Research and Development Program of China

National Natural Science Foundation of China

Postdoctoral Science Foundation of Jiangsu Province

Publisher

Wiley

Subject

General Chemistry,Catalysis

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