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Title: Template-sacrificing synthesis of well-defined asymmetrically coordinated single-atom catalysts for highly efficient CO₂ electrocatalytic reduction
Authors: Huang, Ming
Deng, Bangwei
Zhao, Xiaoli
Zhang, Zheye
Li, Fei
Li, Kanglu
Cui, Zhihao
Kong, Lingxuan
Lu, Jianmei
Dong, Fan
Zhang, Lili
Chen, Peng
Keywords: Engineering::Chemical technology
Issue Date: 2022
Source: Huang, M., Deng, B., Zhao, X., Zhang, Z., Li, F., Li, K., Cui, Z., Kong, L., Lu, J., Dong, F., Zhang, L. & Chen, P. (2022). Template-sacrificing synthesis of well-defined asymmetrically coordinated single-atom catalysts for highly efficient CO₂ electrocatalytic reduction. ACS Nano, 16(2), 2110-2119.
Project: A1983c0025 
Journal: ACS Nano 
Abstract: 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-N4-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-N4-O) for various catalysis applications.
ISSN: 1936-0851
DOI: 10.1021/acsnano.1c07746
DOI (Related Dataset): 10.21979/N9/AQPEO0
Schools: School of Chemical and Biomedical Engineering 
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Nano, © 2022 American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see
Fulltext Permission: open
Fulltext Availability: With Fulltext
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