Journal
NATURE COMMUNICATIONS
Volume 12, Issue 1, Pages -Publisher
NATURE RESEARCH
DOI: 10.1038/s41467-020-20619-w
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Funding
- National Key R&D Program of China [0208300, 0700104]
- National Natural Science Foundation of China [21590812, 21522107, 21671180, 51978637, 51821006]
- State Key Laboratory of Organic Inorganic Composites [oic-201801007]
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In this study, a single-atomic-site Co catalyst supported by BCN was reported to simulate reductive dehalogenases, showing high activity and selectivity in CAP dechlorination compared to other catalysts. The Co SAs/BCN catalyst exhibited enhanced stability and efficiency, making it a promising candidate for sustainable organic chloride conversion.
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 (similar to 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.
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