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

doi:10.1038/s41467-022-29900-6

Cited by 29 publications

(34 citation statements)

References 27 publications

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“…In this process, lipase-AuNCs was Reproduced with permission. [13] Copyright 2022, Springer Nature. first synthesized by controlled reduction of Au ions on lipase using the reducing amino acid of protein as the reducing agent.…”

Section: Polymers As Self-assemble Modulesmentioning

confidence: 99%

“…Ge and co‐workers developed a photochemical method to construct single‐atom enzyme‐metal complex by binding single metal atoms to the carbon radicals generated on an enzyme‐polymer conjugate (Figure 2). [13] The Pd single atoms were successfully anchored on lipase (CALB), alcohol dehydrogenase (ADH), laccase (Lac), catalase (CAT), and glucose oxidase‐pluronic conjugates after the UV treatment of solution containing PdCl 2 , enzyme‐pluronic conjugate, and benzophenone (BP). The photoexcited benzophenone readily abstracted H from the methylene group of pluronic and formed the alkyl radical intermediates which was characterized by electron spin resonance (ESR).…”

Section: Enzyme‐polymer Conjugate As Nanoreactorsmentioning

confidence: 99%

“…c) Magnified AC-STEM image of Pd 1 /CALBÀ P in which the bright dots represent Pd single atoms. d) Schematic illustration of the mechanism for the synthesis of Pdanchored enzyme.Reproduced with permission [13]. Copyright 2022, Springer Nature.…”

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confidence: 99%

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Efficient Enzyme‐Metal Hybrid Catalysts Constructed with Polymer

Fan

Liao

et al. 2022

ChemCatChem

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Section: Polymers As Self-assemble Modulesmentioning

confidence: 99%

Section: Enzyme‐polymer Conjugate As Nanoreactorsmentioning

confidence: 99%

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Efficient Enzyme‐Metal Hybrid Catalysts Constructed with Polymer

Fan

Liao

et al. 2022

ChemCatChem

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“…The coupling of enzymatic catalysis with other types of catalysis, such as chemocatalysis, − photocatalysis, , electrocatalysis, etc., is promising for developing cascaded processes for chemical production. However, the optimal conditions for enzymatic catalysis and other processes are often quite different.…”

Section: Introductionmentioning

confidence: 99%

Efficient Electroenzymatic Cascade Catalysis for Ortho-Selective Chlorination of Phenol

Zhu

Ding

et al. 2022

ACS Sustainable Chem. Eng.

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The integration of enzymatic catalysis and electrocatalysis is promising for developing new green techniques for chemical production; however, how to coordinate the two processes for one-pot cascade reactions is a challenge. In this work, the electrocatalytic reduction of O 2 to H 2 O 2 by a reduced graphene oxide (rGO)/polyethylenimine (PEI) composite to initiate an enzymatic reaction by ionic liquid modified chloroperoxidase (CPO-IL EMB ) is presented. The whole cascade process is very efficient due to the four strategies, including avoiding the inactivation of CPO through the competitive reaction of oxidant (H 2 O 2 ), utilizing nanoproximity effects to construct substrate diffusion channels, fine-tuning the microenvironment of the enzymatic active site by IL EMB to increase the electron transfer efficiency as well as enhance the stability, and improving the selectivity of the 2e-ORR (oxidation reduction reaction) of rGO by PEI. The cascade efficiency is enhanced 5.5 times compared to manually adding H 2 O 2 , and 2.3 times compared to free CPO. Moreover, the rapid generation of intermediate (compounds I and X) and the orientation of substrate lead to ortho-selectivity of phenol chlorination.

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“…Recently, Li et al utilized protein–polymer nanoconjugates as confined nanoreactors to in situ fabricate enzyme–metal nanoparticle hybrids . Subsequently, the same team used photochemical methods to construct a stable single-atom enzyme–metal complex on the enzyme–polymer conjugate . Both types of enzyme–metal hybrid catalysts with synergistic effects possessed excellent catalytic activity in one-pot chemoenzymatic reactions.…”

Section: Introductionmentioning

confidence: 99%

General Synergistic Hybrid Catalyst Synthesis Method Using a Natural Enzyme Scaffold-Confined Metal Nanocluster

Liu

Zhang

et al. 2022

ACS Appl. Mater. Interfaces

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Due to differences in the chemical properties or optimal reaction conditions of the catalysts, the challenge in the design of bio-chemical hybrid catalysts is that the bio-catalysts or chemical catalysts usually cannot maintain the initial catalytic performance. Herein, we report a general bio-chemical hybrid catalyst synthesis method using a natural enzyme scaffold-confined metal nanocluster. A redox-active enzyme is a nanoreactor that allows access to and reduces metal ions into metal nanoclusters in situ, resulting in the enzyme-confined metal nanocluster hybrid catalyst with a synergistic effect to boost catalytic performance. Specifically, bilirubin oxidase-Ir nanoclusters (BOD-Ir NCs) with catalytic properties for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are designed. The BOD-Ir NCs exhibit an approximately 2-fold ORR activity compared with pure BOD and a 4-fold OER activity compared with pure Ir NCs. BOD-Ir NCs exhibit stability for over 50,000 s, exceeding that of pure Ir NCs (22,000 s). The synergistic catalytic performance is attributed to the following: the mild preparation condition and matched sizes of BOD and the Ir NCs maintain the natural activity of BOD; the highly conductive Ir NCs improve the ORR activity of BOD; and the confining effect of BOD, which improves the stability and activity of the Ir NCs during the OER. In particular, BOD-Ir NCs exhibit a high half-wave potential of 0.97 V for the ORR and a low overpotential of 319 mV at 10 mA cm −2 for the OER, surpassing most of reported catalysts under neutral conditions. Furthermore, laccase-Ir NCs and glucose oxidase-Pd NCs with synergistic catalytic performances are fabricated, proving the universality of this synthetic method. This facile strategy for designing synergistic hybrid catalysts is expected to be applied to more complex chemical transformations.

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Cooperative catalysis by a single-atom enzyme-metal complex

Cited by 29 publications

References 27 publications

Efficient Enzyme‐Metal Hybrid Catalysts Constructed with Polymer

Efficient Enzyme‐Metal Hybrid Catalysts Constructed with Polymer

Efficient Electroenzymatic Cascade Catalysis for Ortho-Selective Chlorination of Phenol

General Synergistic Hybrid Catalyst Synthesis Method Using a Natural Enzyme Scaffold-Confined Metal Nanocluster

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