Concerted Chemoenzymatic Synthesis of alpha-Keto Acid through Compartmentalizing and Channeling of Metal-Organic Frameworks

doi:10.1021/acscatal.0c01985

	Concerted Chemoenzymatic Synthesis of alpha-Keto Acid through Compartmentalizing and Channeling of Metal-Organic Frameworks
	Wu, Yizhou 5; Shi, Jiafu 2,3,4; Mei, Shuang 5; Katimba, Hija Athman 5; Sun, Yiying 5; Wang, Xueying 2; Liang, Kang 1,7; Jiang, Zhongyi 3,5,6
刊名	ACS CATALYSIS
	2020-09-04
卷号	10 期号:17 页码:9664-9673
关键词	chemoenzymatic catalysis compartmentalization-channeling strategy metal-organic frameworks biocatalysis heterogeneous catalysis
ISSN号	2155-5435
DOI	10.1021/acscatal.0c01985
英文摘要	Chemoenzymatic catalysis inherits the attributes of enzymatic catalysis and chemical catalysis, where the efficiency is usually governed by the synergy of the two catalytic modules, particularly, the compatibility between two catalysts and the mass transfer between two catalytic processes. To achieve a high photosynthesis efficiency, green plants compartmentalize water oxidation and NADPH regeneration modules on two sides of the thylakoid membrane while conveying electron transfer and proton transport via the channeling of the electron transfer chain and ATP synthase, respectively. Herein, we demonstrate this principle in vitro by using UiO-66 to confine platinum nanoparticles (Pt NPs) inside and immobilize L-amino acid oxidase (LAAO) outside for the chemoenzymatic synthesis of a-keto acid. The framework structure of UiO-66 affords the compartmentalization of LAAO and Pt NPs to avoid the deactivation of LAAO by Pt NPs, while its angstrom-scale pore size ensures channeling of the byproduct, H2O2, from LAAO to Pt NPs for instant elimination. A 99.7% yield of alpha-keto acid is achieved, far surpassing that enabled by free LAAO (41.2%). The compartmentalization-channeling strategy offers a generic platform to coordinate reactions and mass transfer in complex catalytic processes beyond chemoenzymatic catalysis.
资助项目	National Natural Science Foundation of China[21621004] ; National Natural Science Foundation of China[21776213] ; Tianjin Natural Science Foundation[19JCYBJC19700] ; Open foundation of State Key Laboratory of Chemical Engineering[SKL-ChE19B01] ; Open Funding Project of the State Key Laboratory of Biochemical Engineering[2020KF-06] ; Tianjin Synthetic Biotechnology Innovation Capacity Improvement Project[TSBICIP-KJGG-003] ; Program of Introducing Talents of Discipline to Universities[B06006]
WOS关键词	CRYSTAL-STRUCTURE ; CARBON-DIOXIDE ; CATALYSIS ; OXIDASE ; ENZYMES ; DRIVEN ; INTEGRATION ; RESOLUTION ; REDUCTION ; SUBSTRATE
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000569376700001
资助机构	National Natural Science Foundation of China ; Tianjin Natural Science Foundation ; Open foundation of State Key Laboratory of Chemical Engineering ; Open Funding Project of the State Key Laboratory of Biochemical Engineering ; Tianjin Synthetic Biotechnology Innovation Capacity Improvement Project ; Program of Introducing Talents of Discipline to Universities
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/42110]
专题	中国科学院过程工程研究所
通讯作者	Shi, Jiafu; Jiang, Zhongyi
作者单位	1.Univ New South Wales, Australian Ctr NaiwMed, Sydney, NSW 2052, Australia 2.Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300072, Peoples R China 3.Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China 4.Chinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing 10090, Peoples R China 5.Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China 6.Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou 350207, Peoples R China 7.Univ New South Wales, Sch Chem Engn, Grad Sch Biomed Engn, Sydney, NSW 2052, Australia
推荐引用方式 GB/T 7714	Wu, Yizhou,Shi, Jiafu,Mei, Shuang,et al. Concerted Chemoenzymatic Synthesis of alpha-Keto Acid through Compartmentalizing and Channeling of Metal-Organic Frameworks[J]. ACS CATALYSIS,2020,10(17):9664-9673.
APA	Wu, Yizhou.,Shi, Jiafu.,Mei, Shuang.,Katimba, Hija Athman.,Sun, Yiying.,...&Jiang, Zhongyi.(2020).Concerted Chemoenzymatic Synthesis of alpha-Keto Acid through Compartmentalizing and Channeling of Metal-Organic Frameworks.ACS CATALYSIS,10(17),9664-9673.
MLA	Wu, Yizhou,et al."Concerted Chemoenzymatic Synthesis of alpha-Keto Acid through Compartmentalizing and Channeling of Metal-Organic Frameworks".ACS CATALYSIS 10.17(2020):9664-9673.