Operando Surface Ligands Boost Pt Nanozyme Activity for H2O2 Catalysis via Bridged Electron Transfer

被引:3
作者
Wei, Shuangshuang [1 ]
Zhang, Wentao [2 ]
Wang, Ziyi [1 ]
Zhang, Guoyang [1 ]
Li, Wen-Wei [3 ,4 ]
Zeng, Guixiang [5 ]
Zhang, Shujuan [1 ]
机构
[1] Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resource Reuse, Nanjing 210023, Peoples R China
[2] Tsinghua Univ, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Peoples R China
[3] Univ Sci & Technol China, Dept Environm Sci & Engn, CAS Key Lab Urban Pollutant Convers, Hefei 230026, Peoples R China
[4] City Univ Hong Kong, Dept Mat Sci & Engn, Hong Kong 999077, Peoples R China
[5] Nanjing Univ, Kuang Yaming Honors Sch, Nanjing 210023, Peoples R China
基金
中国国家自然科学基金;
关键词
microenvironment; photoreduction; surface ligand; noble-metal; electron transfer; hydrogen bond; NANOPARTICLES; FUNCTIONALIZATION; PHOTOLYSIS; ACID;
D O I
10.1021/acscatal.5c00961
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nanozymes, while possessing greater stability and durability than their natural counterparts, still face limitations of low catalytic activity and inefficient production. Here, we report a one-step method for the efficient construction of highly active nanozymes. The photolysis of butanedione was leveraged to generate surface-functionalized metal nanozymes. The in situ generated surface acetate (Ac) ligands serve as electron bridges between the substrates to boost the electron transfer, thus drastically improving the catalytic activity. The resulting Ac-Ptzyme, with a precisely tuned surface Ac content, demonstrated a peroxidase-like activity superior to that of the natural horseradish peroxidase and was approximately 200 times greater than that of Fe3O4. This superior activity endowed the Ac-Ptzyme with enhanced performance for visually monitoring the oxidative stress in bloom-forming cyanobacterial cells and for killing pathogenic bacteria in biofilm. This work paves a path to the facile synthesis of high-activity nanozymes for catalysis.
引用
收藏
页码:6439 / 6449
页数:11
相关论文
共 55 条
[1]  
Boles MA, 2016, NAT MATER, V15, P141, DOI [10.1038/nmat4526, 10.1038/NMAT4526]
[2]   PHOTOREDUCTION OF BENZOPHENONE IN BENZENE .2. FLASH PHOTOLYSIS STUDY OF PRIMARY PHOTOCHEMICAL REACTIONS [J].
BUETTNER, AV ;
DEDINAS, J .
JOURNAL OF PHYSICAL CHEMISTRY, 1971, 75 (02) :187-&
[3]   The role of organic ligand shell structures in colloidal nanocrystal synthesis [J].
Calvin, Jason J. ;
Brewer, Amanda S. ;
Alivisatos, A. Paul .
NATURE SYNTHESIS, 2022, 1 (02) :127-137
[4]   Shape-controlled synthesis of platinum nanocrystals for catalytic and electrocatalytic applications [J].
Chen, Jingyi ;
Lim, Byungkwon ;
Lee, Eric P. ;
Xia, Younan .
NANO TODAY, 2009, 4 (01) :81-95
[5]   Block-Polymer-Restricted Sub-nanometer Pt Nanoclusters Nanozyme-Enhanced Immunoassay for Monitoring of Cardiac Troponin I [J].
Chen, Shuyun ;
Yu, Zhichao ;
Wang, Yunsen ;
Tang, Juan ;
Zeng, Yongyi ;
Liu, Xiaolong ;
Tang, Dianping .
ANALYTICAL CHEMISTRY, 2023, 95 (38) :14494-14501
[6]   Optimization of Fe3O4 nanozyme activity via single amino acid modification mimicking an enzyme active site [J].
Fan, Kelong ;
Wang, Hui ;
Xi, Juqun ;
Liu, Qi ;
Meng, Xiangqin ;
Duan, Demin ;
Gao, Lizeng ;
Yan, Xiyun .
CHEMICAL COMMUNICATIONS, 2017, 53 (02) :424-427
[7]   Aqueous-phase photolysis of biacetyl (an alpha-dicarbonyl compound): A sink for biacetyl, and a source of acetic acid, peroxyacetic acid, hydrogen peroxide, and the highly oxidizing acetylperoxyl radical in aqueous aerosols, fogs, and clouds [J].
Faust, BC ;
Powell, K ;
Rao, CJ ;
Anastasio, C .
ATMOSPHERIC ENVIRONMENT, 1997, 31 (03) :497-510
[8]   Hydroxyl radical yields in the Fenton process under various pH, ligand concentrations and hydrogen peroxide/Fe(II) ratios [J].
Fischbacher, Alexandra ;
von Sonntag, Clemens ;
Schmidt, Torsten C. .
CHEMOSPHERE, 2017, 182 :738-744
[9]   Redox homeostasis and antioxidant signaling: A metabolic interface between stress perception and physiological responses [J].
Foyer, CH ;
Noctor, G .
PLANT CELL, 2005, 17 (07) :1866-1875
[10]   Citrate Coordination and Bridging of Gold Nanoparticles: The Role of Gold Adatoms in AuNP Aging [J].
Grys, David-Benjamin ;
de Nijs, Bart ;
Salmon, Andrew R. ;
Huang, Junyang ;
Wang, Wenting ;
Chen, Wei-Hsin ;
Scherman, Oren A. ;
Baumberg, Jeremy J. .
ACS NANO, 2020, 14 (07) :8689-8696