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Template-Sacrificing Synthesis of Well-Defined Asymmetrically Coordinated Single-Atom Catalysts for Highly Efficient CO2 Electrocatalytic Reduction
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DOI：10.1021/acsnano.1c07746.png)
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Abstract
En 中文
Although various single-atom catalysts have been designed, atomically engineering their coordination environment remains a great challenge. Herein, a one-pot template-sacrificing pyrolysis approach is developed to synthesize well-defined Ni-N-4-O catalytic sites on highly porous graphitic carbon for electrocatalytic CO2 reduction to CO with high Faradaic efficiency (maximum of 97.2%) in a wide potential window (-0.56 to -1.06 V vs RHE) and with high stability. In-depth experimental and theoretical studies reveal that the axial Ni-O coordination introduces asymmetry to the catalytic center, leading to lower Gibbs free energy for the rate-limiting step, strengthened binding with *COOH, and a weaker association with *CO. The present results demonstrate the successful atomic-level coordination environment engineering of high-surface-area porous graphitic carbon-supported Ni single-atom catalysts (SACs), and the demonstrated method can be applied to synthesize an array of SACs (metal-N-4-O) for various catalysis applications.
Keywords:
Ni single-atom catalysts
CO2 reduction reaction
coordination environment
asymmetry
electronic structure
porous graphitic carbon
Journal
IF:
16
Papers:
2.6W
Citations:
25.6W
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Cited Papers