中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
首页 机构 成果 学者
  
  1. CAS IR Grid
  2. 过程工程研究所
  3. 中国科学院过程工程研究所
Modulating Catalytic Activity and Stability of Atomically Precise Gold Nanoclusters as Peroxidase Mimics via Ligand Engineering

文献类型：期刊论文

作者Shan, Huiting1,2; Shi, Jiafu4,5,6; Chen, Tiankai3; Cao, Yitao2; Yao, Qiaofeng1,2; An, Hua1,2; Yang, Zhucheng1,2; Wu, Zhenhua4; Jiang, Zhongyi1,5,7; Xie, Jianping1,2
刊名ACS NANO
出版日期2023-02-01
页码10
关键词gold nanoclusters ligand engineering peroxidase mimic catalysis catalytic activity stability
ISSN号1936-0851
DOI10.1021/acsnano.2c09238
英文摘要Metal nanoclusters (NCs), composed of a metal core and protecting ligands, show promising potentials as enzyme mimics for producing fuels, pharmaceuticals, and valuable chemicals, etc. Herein, we explore the critical role of ligands in modulating the peroxidase mimic activity and stability of Au NCs. A series of Au15(SR)13 NCs with various thiolate ligands [SR = N-acetyl-L-cysteine (NAC), 3-mercapto-propionic acid (MPA), or 3-mercapto-2-methylpropanoic acid (MMPA)] are utilized as model catalysts. It is found that Au15(NAC)13 shows higher structural stability than Au15(MMPA)13 and Au15(MPA)13 against external stimuli (e.g., pH, oxidants, and temperature) because of the intramolecular hydrogen bonds. More importantly, detailed enzymatic kinetics data show that the catalytic activity of Au15(NAC)13 is about 4.3 and 2.7 times higher than the catalytic activity of Au15(MMPA)13 and Au15(MPA)13, respectively. Density functional theory (DFT) calculations reveal that the Au atoms on the motif of Au NCs should be the active centers, whereas the superior peroxidase mimic activity of Au15(NAC)13 should originate from the emptier orbitals of Au atoms because of the electron-withdrawing effect of acetyl amino group in NAC. This work demonstrates the ligand-engineered electronic structure and functionality of atomically precise metal NCs, which afford molecular and atomic level insights for artificial enzyme design.
WOS关键词AU-25 NANOCLUSTERS ; CRYSTAL-STRUCTURE ; CLUSTER ; AU-15(SR)(13) ; NANOPARTICLES ; REDUCTION ; INCREASES ; THIOLATE ; AU-15
资助项目Ministry of Education, Singapore[R-279-000- 580-112] ; Ministry of Education, Singapore[A-8000054-01-00] ; National Natural Science Foundation of China[22071174] ; National Natural Science Foundation of China[22122809] ; National Key R&D Program of China[2020KF- 06] ; Open Funding Project of the State Key Laboratory of Biochemical Engineering[2021YFC2102300] ; [2020YFA0907900]
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
语种英语
WOS记录号WOS:000927046300001
出版者AMER CHEMICAL SOC
资助机构Ministry of Education, Singapore ; National Natural Science Foundation of China ; National Key R&D Program of China ; Open Funding Project of the State Key Laboratory of Biochemical Engineering
源URL[http://ir.ipe.ac.cn/handle/122111/57088]  
通讯作者Shi, Jiafu; Jiang, Zhongyi; Xie, Jianping
作者单位1.Tianjin Univ, Joint Sch Natl Univ Singapore & Tianjin Univ, Int Campus, Fuzhou 350207, Peoples R China
2.Natl Univ Singapore, Dept Chem & Biomol Engn, Singapore 117585, Singapore
3.Chinese Univ Hong Kong, Sch Sci & Engn, Shenzhen 518000, Peoples R China
4.Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300072, Peoples R China
5.Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China
6.Chinese Acad Sci, Inst Proc Engn, State Key Lab Biochem Engn, Beijing, Peoples R China
7.Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China
推荐引用方式
GB/T 7714		 Shan, Huiting,Shi, Jiafu,Chen, Tiankai,et al. Modulating Catalytic Activity and Stability of Atomically Precise Gold Nanoclusters as Peroxidase Mimics via Ligand Engineering[J]. ACS NANO,2023:10.
APA Shan, Huiting.,Shi, Jiafu.,Chen, Tiankai.,Cao, Yitao.,Yao, Qiaofeng.,...&Xie, Jianping.(2023).Modulating Catalytic Activity and Stability of Atomically Precise Gold Nanoclusters as Peroxidase Mimics via Ligand Engineering.ACS NANO,10.
MLA Shan, Huiting,et al."Modulating Catalytic Activity and Stability of Atomically Precise Gold Nanoclusters as Peroxidase Mimics via Ligand Engineering".ACS NANO (2023):10.

入库方式： OAI收割

来源：过程工程研究所

浏览0
下载0
收藏0
其他版本

除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。