Granum-Inspired Photoenzyme-Coupled Catalytic System via Stacked Polymeric Carbon Nitride

doi:10.1021/acscatal.1c01555

	Granum-Inspired Photoenzyme-Coupled Catalytic System via Stacked Polymeric Carbon Nitride
	Jia, Jingshan 1,2; Huo, Qian 1,2; Yang, Dong 2,3; Sun, Yiying 1,2; Zhang, Songping 4; Li, Shihao 1,2; Shi, Jiafu 2,3,5; Jiang, Zhongyi 1,2,5
刊名	ACS CATALYSIS
	2021-08-06
卷号	11 期号:15 页码:9210-9220
关键词	photoenzyme-coupled catalytic system polymeric carbon nitride granum-inspired stacked structure chlorperoxidase hydrogen peroxide
ISSN号	2155-5435
DOI	10.1021/acscatal.1c01555
英文摘要	Photoenzyme-coupled catalysis has become a powerful platform for chemical manufacturing, in which energy-bearing intermediates are often shuttled between a photocatalytic module and an enzymatic module. A photoenzyme-coupled catalytic system (PECCS) to realize the generation of intermediates by the photocatalytic module and utilization of intermediates by the enzymatic module is highly desired. Inspired by the structure and function of a granum, stacked tubular polymeric carbon nitride (st-PCN) is designed as both a photocatalyst and a carrier for chlorperoxidase (CPO), constructing the st-PCN@CPO PECCS to implement the cascade chlorination reaction. st-PCN* ensures oriented electron transfer, achieving the H2O2 evolution rate of 150 mu mol h(-1) g(-1) (st-PCN), over 55- and 2-fold that of bulky PCN (b-PCN) and bulky PCN (b-PCN). Meanwhile, st-PCN shortens the diffusion distance of H2O2 from st-PCN* to CPO. Under simulated sunlight irradiation, our st-PCN*@CPO PECCS realizes in situ, continuous, and controllable supply of H2O2 to CPO, followed by converting monochlorodimedone (MCD) into dichlordimedone (DCD) with a final conversion ratio of similar to 39.5%. The initial reaction rate could reach 0.29 mM h(-1), over 20-fold that of its counterpart PECCS with a nonstacked structured photocatalyst. Our study unveils the potential of exploring the stacked structure to coordinate cascade catalytic processes.
资助项目	National Natural Science Funds of China[21776213] ; National Natural Science Funds of China[21621004] ; Natural Science Fund of Tianjin[19JCYBJC19700] ; Open Funding Project of the State Key Laboratory of Biochemical Engineering[2020KF-06] ; Open Funding Project of the State Key Laboratory of Chemical Engineering[SKL-ChE19B01] ; Tianjin Synthetic Biotechnology Innovation Capacity Improvement Project[TSBICIP-KJGG-003] ; Royal Society International Collaboration Award[ICA \R1\180317]
WOS关键词	ELECTRON-TRANSFER ; PHOTOCATALYTIC DEGRADATION ; HYDROGEN-PEROXIDE ; EFFICIENT ; ENZYME ; OXYFUNCTIONALIZATION ; PEROXYGENASES ; INACTIVATION ; OXIDATION ; CAPSULES
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000684035000021
资助机构	National Natural Science Funds of China ; Natural Science Fund of Tianjin ; Open Funding Project of the State Key Laboratory of Biochemical Engineering ; Open Funding Project of the State Key Laboratory of Chemical Engineering ; Tianjin Synthetic Biotechnology Innovation Capacity Improvement Project ; Royal Society International Collaboration Award
内容类型	期刊论文
源URL	[http://ir.ipe.ac.cn/handle/122111/49877]
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.Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China 2.Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China 3.Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300072, Peoples R China 4.Chinese Acad Sci, State Key Lab Biochem Engn, Inst Proc Engn, Beijing 10090, Peoples R China 5.Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus Tianjin Univ, Fuzhou 350207, Peoples R China
推荐引用方式 GB/T 7714	Jia, Jingshan,Huo, Qian,Yang, Dong,et al. Granum-Inspired Photoenzyme-Coupled Catalytic System via Stacked Polymeric Carbon Nitride[J]. ACS CATALYSIS,2021,11(15):9210-9220.
APA	Jia, Jingshan.,Huo, Qian.,Yang, Dong.,Sun, Yiying.,Zhang, Songping.,...&Jiang, Zhongyi.(2021).Granum-Inspired Photoenzyme-Coupled Catalytic System via Stacked Polymeric Carbon Nitride.ACS CATALYSIS,11(15),9210-9220.
MLA	Jia, Jingshan,et al."Granum-Inspired Photoenzyme-Coupled Catalytic System via Stacked Polymeric Carbon Nitride".ACS CATALYSIS 11.15(2021):9210-9220.