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Electron Paramagnetic Resonance Analysis of Hydroquinone Polymerization Catalyzed by Small Laccase

文献类型：期刊论文

作者Liu, Aokun2,3; Kuang, Jian3; Wei, Ruotong2; Zhang, Zhitao2; Li, Jiabin1,4; Tian, Changlin2,3; Yu, Lu2,3
刊名CHEMCATCHEM
出版日期2024-10-08
关键词EPR Free radical Reactive catalytic intermediate Small laccase Superhyperfine splitting
ISSN号1867-3880
DOI10.1002/cctc.202401048
通讯作者Tian, Changlin(cltian@ustc.edu.cn) ; Yu, Lu(luyuesr@ustc.edu.cn)
英文摘要Laccases are multi-copper oxidases (MCOs) that oxidize a broad range of substrates while reducing molecular oxygen to water. Although much effort has been made to elucidate the catalytic mechanism of laccases, information about reactive catalytic intermediates during catalysis is not yet fully understood. Herein, hydroquinone (HQ) polymerization catalyzed by prokaryotic small laccase (SLAC) was investigated by electron paramagnetic resonance (EPR) spectroscopy to provide more information on the catalytic mechanism. Briefly, free radical intermediates during the catalysis were investigated by real-time in situ EPR measurement to monitor the formation and transformation of free radicals. A paramagnetic species was identified which was attributed to a copolymer formed by hydroquinone, benzoquinone, and semiquinone radical. In addition, the low-temperature EPR spectrum of the trinuclear copper center during catalysis not only revealed tentative rotational motion of the histidine imidazole rings coordinating the TNC upon electron uptake but also provided evidence of the formation of oxygen bridge at TNC during the reaction, represented by the observation of a new type 2 copper component featured larger g// values and smaller A// values. Together, EPR spectroscopic insights into the catalytic intermediates during enzymatic hydroquinone polymerization have extended the knowledge of the biophysical characteristics and catalytic mechanism of SLAC. Real-time in situ EPR was employed to monitor the formation and evolution of free radical intermediates, while low-temperature EPR simultaneously revealed tentative rotational motion of the His residue coordinating the TNC upon electron uptake. These results have extended our knowledge of the biophysical characteristics and catalytic mechanism of SLAC. image
WOS关键词STREPTOMYCES-COELICOLOR ; ACTIVE-SITES ; REDUCTION ; INTERMEDIATE ; MECHANISM ; EXCHANGE ; CLUSTER ; CU(II) ; O-2
资助项目Strategic Priority Research Program of Chinese Academy of Sciences ; National Natural Science Foundation of China[21927814] ; National Key Research and Development Program of China[2019YFA0405600] ; National Key Research and Development Program of China[2019YFA0706900] ; National Key Research and Development Program of China[2021YFA1200104] ; National Key Research and Development Program of China[2022YFC3400500] ; Plans for Major Provincial Science & Technology Projects[202303a07020004] ; Youth Innovation Promotion Association, CAS[2022455] ; [XDB0960201] ; [XDB0540000]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:001328070200001
出版者WILEY-V C H VERLAG GMBH
资助机构Strategic Priority Research Program of Chinese Academy of Sciences ; National Natural Science Foundation of China ; National Key Research and Development Program of China ; Plans for Major Provincial Science & Technology Projects ; Youth Innovation Promotion Association, CAS
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/135794]  
专题中国科学院合肥物质科学研究院
通讯作者Tian, Changlin; Yu, Lu
作者单位1.Soochow Univ, Jiangsu Key Lab Neuropsychiat Dis, Suzhou 215123, Peoples R China
2.Chinese Acad Sci, Hefei Inst Phys Sci, High Magnet Field Lab, Hefei 230031, Peoples R China
3.Univ Sci & Technol China, Affiliated Hosp USTC 1, Inst Endocrine & Metab Dis, Joint Ctr Biol Analyt Chem,Dept Endocrinol,Div Lif, Hefei 230026, Peoples R China
4.Soochow Univ, Coll Pharmaceut Sci, Suzhou 215123, Peoples R China
推荐引用方式
GB/T 7714		 Liu, Aokun,Kuang, Jian,Wei, Ruotong,et al. Electron Paramagnetic Resonance Analysis of Hydroquinone Polymerization Catalyzed by Small Laccase[J]. CHEMCATCHEM,2024.
APA Liu, Aokun.,Kuang, Jian.,Wei, Ruotong.,Zhang, Zhitao.,Li, Jiabin.,...&Yu, Lu.(2024).Electron Paramagnetic Resonance Analysis of Hydroquinone Polymerization Catalyzed by Small Laccase.CHEMCATCHEM.
MLA Liu, Aokun,et al."Electron Paramagnetic Resonance Analysis of Hydroquinone Polymerization Catalyzed by Small Laccase".CHEMCATCHEM (2024).

入库方式： OAI收割

来源：合肥物质科学研究院

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