Cooperative catalysis by a single-atom enzyme-metal complex

Anchoring single metal atoms on enzymes has great potential to generate hybrid catalysts with high activity and selectivity for reactions that cannot be driven by traditional metal catalysts. Herein, we develop a photochemical method to construct a stable single-atom enzyme-metal complex by binding...

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Autores principales: Li, Xiaoyang, Cao, Yufei, Luo, Kai, Zhang, Lin, Bai, Yunxiu, Xiong, Jiarong, Zare, Richard N., Ge, Jun
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Article
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9023488/
https://www.ncbi.nlm.nih.gov/pubmed/35449166
http://dx.doi.org/10.1038/s41467-022-29900-6
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author Li, Xiaoyang
Cao, Yufei
Luo, Kai
Zhang, Lin
Bai, Yunxiu
Xiong, Jiarong
Zare, Richard N.
Ge, Jun
author_facet Li, Xiaoyang
Cao, Yufei
Luo, Kai
Zhang, Lin
Bai, Yunxiu
Xiong, Jiarong
Zare, Richard N.
Ge, Jun
author_sort Li, Xiaoyang
collection PubMed
description Anchoring single metal atoms on enzymes has great potential to generate hybrid catalysts with high activity and selectivity for reactions that cannot be driven by traditional metal catalysts. Herein, we develop a photochemical method to construct a stable single-atom enzyme-metal complex by binding single metal atoms to the carbon radicals generated on an enzyme-polymer conjugate. The metal mass loading of Pd-anchored enzyme is up to 4.0% while maintaining the atomic dispersion of Pd. The cooperative catalysis between lipase-active site and single Pd atom accelerates alkyl-alkyl cross-coupling reaction between 1-bromohexane and B-n-hexyl-9-BBN with high efficiency (TOF is 540 h(−1)), exceeding that of the traditional catalyst Pd(OAc)(2) by a factor of 300 under ambient conditions.
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spelling pubmed-90234882022-04-28 Cooperative catalysis by a single-atom enzyme-metal complex Li, Xiaoyang Cao, Yufei Luo, Kai Zhang, Lin Bai, Yunxiu Xiong, Jiarong Zare, Richard N. Ge, Jun Nat Commun Article Anchoring single metal atoms on enzymes has great potential to generate hybrid catalysts with high activity and selectivity for reactions that cannot be driven by traditional metal catalysts. Herein, we develop a photochemical method to construct a stable single-atom enzyme-metal complex by binding single metal atoms to the carbon radicals generated on an enzyme-polymer conjugate. The metal mass loading of Pd-anchored enzyme is up to 4.0% while maintaining the atomic dispersion of Pd. The cooperative catalysis between lipase-active site and single Pd atom accelerates alkyl-alkyl cross-coupling reaction between 1-bromohexane and B-n-hexyl-9-BBN with high efficiency (TOF is 540 h(−1)), exceeding that of the traditional catalyst Pd(OAc)(2) by a factor of 300 under ambient conditions. Nature Publishing Group UK 2022-04-21 /pmc/articles/PMC9023488/ /pubmed/35449166 http://dx.doi.org/10.1038/s41467-022-29900-6 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Li, Xiaoyang
Cao, Yufei
Luo, Kai
Zhang, Lin
Bai, Yunxiu
Xiong, Jiarong
Zare, Richard N.
Ge, Jun
Cooperative catalysis by a single-atom enzyme-metal complex
title Cooperative catalysis by a single-atom enzyme-metal complex
title_full Cooperative catalysis by a single-atom enzyme-metal complex
title_fullStr Cooperative catalysis by a single-atom enzyme-metal complex
title_full_unstemmed Cooperative catalysis by a single-atom enzyme-metal complex
title_short Cooperative catalysis by a single-atom enzyme-metal complex
title_sort cooperative catalysis by a single-atom enzyme-metal complex
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9023488/
https://www.ncbi.nlm.nih.gov/pubmed/35449166
http://dx.doi.org/10.1038/s41467-022-29900-6
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AT baiyunxiu cooperativecatalysisbyasingleatomenzymemetalcomplex
AT xiongjiarong cooperativecatalysisbyasingleatomenzymemetalcomplex
AT zarerichardn cooperativecatalysisbyasingleatomenzymemetalcomplex
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