Integrating single-cobalt-site and electric field of boron nitride in dechlorination electrocatalysts by bioinspired design

Yuan Min, Xiao Zhou (), Jie-Jie Chen (), Wenxing Chen, Fangyao Zhou, Zhiyuan Wang, Jia Yang, Can Xiong, Ying Wang, Fengting Li, Han-Qing Yu and Yuen Wu ()
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Yuan Min: University of Science and Technology of China
Xiao Zhou: University of Science and Technology of China
Jie-Jie Chen: University of Science and Technology of China
Wenxing Chen: Beijing Institute of Technology
Fangyao Zhou: University of Science and Technology of China
Zhiyuan Wang: University of Science and Technology of China
Jia Yang: University of Science and Technology of China
Can Xiong: University of Science and Technology of China
Ying Wang: Tongji University
Fengting Li: Tongji University
Han-Qing Yu: University of Science and Technology of China
Yuen Wu: University of Science and Technology of China

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract The construction of enzyme-inspired artificial catalysts with enzyme-like active sites and microenvironment remains a great challenge. Herein, we report a single-atomic-site Co catalyst supported by carbon doped boron nitride (BCN) with locally polarized B–N bonds (Co SAs/BCN) to simulate the reductive dehalogenases. Density functional theory analysis suggests that the BCN supports, featured with ionic characteristics, provide additional electric field effect compared with graphitic carbon or N-doped carbon (CN), which could facilitate the adsorption of polarized organochlorides. Consistent with the theoretical results, the Co SAs/BCN catalyst delivers a high activity with nearly complete dechlorination (~98%) at a potential of −0.9 V versus Ag/AgCl for chloramphenicol (CAP), showing that the rate constant (k) contributed by unit mass of metal (k/ratio) is 4 and 19 times more active than those of the Co SAs/CN and state-of-the-art Pd/C catalyst, respectively. We show that Co single atoms coupled with BCN host exhibit high stability and selectivity in CAP dechlorination and suppress the competing hydrogen evolution reaction, endowing the Co SAs/BCN as a candidate for sustainable conversion of organic chloride.

Date: 2021
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DOI: 10.1038/s41467-020-20619-w

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