In Situ Visualization of Electrocatalytic Reaction Activity at Quantum Dots for Water Oxidation

被引:35
作者
Chen, Ying [1 ]
Fu, Jiaju [1 ]
Cui, Chen [1 ]
Jiang, Dechen [1 ]
Chen, Zixuan [1 ]
Chen, Hong-Yuan [1 ]
Zhu, Jun-Jie [1 ]
机构
[1] Nanjing Univ, Sch Chem & Chem Engn, State Key Lab Analyt Chem Life Sci, Nanjing 210093, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
SINGLE CDS NANOPARTICLES; ELECTROGENERATED CHEMILUMINESCENCE; EVOLUTION ELECTROCATALYSTS; PHOTOCATALYTIC ACTIVITY; SURFACE-CHEMISTRY; ALKALINE-SOLUTION; ELECTROCHEMILUMINESCENCE; LUMINOL; NANOCRYSTALS; ELECTRODE;
D O I
10.1021/acs.analchem.8b01935
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
Exploring electrocatalytic reactions on the nanomaterial surface can give crucial information for the development of robust catalysts. Here, electrocatalytic reaction activity at single quantum dots (QDs) loaded silica microparticle involved in water oxidation is visualized using electrochemiluminescence (ECL) microscopy. Under positive potential, the active redox centers at QDs induce the generation of hydroperoxide surface intermediates as coreactants to remarkably enhance ECL emission from luminol derivative molecules for imaging. For the first time, in situ visualization of the catalytic activity of water oxidation with QDs catalyst was achieved, supported by a linear relation between ECL intensity and turn over frequency. A very slight diffusion trend attributed to only the luminol species proved in situ capture of hydroperoxide surface intermediates at catalytic active sites of QDs. This work provides tremendous potential in online imaging of electrocatalytic reactions and visual evaluation of catalyst performance.
引用
收藏
页码:8635 / 8641
页数:7
相关论文
共 56 条
[1]   Semiconductor clusters, nanocrystals, and quantum dots [J].
Alivisatos, AP .
SCIENCE, 1996, 271 (5251) :933-937
[2]   Electrochemical properties of CdSe and CdTe quantum dots [J].
Amelia, Matteo ;
Lincheneau, Christophe ;
Silvi, Serena ;
Credi, Alberto .
CHEMICAL SOCIETY REVIEWS, 2012, 41 (17) :5728-5743
[3]   Single-Molecule Catalysis Mapping Quantifies Site-Specific Activity and Uncovers Radial Activity Gradient on Single 2D Nanocrystals [J].
Andoy, Nesha May ;
Zhou, Xiaochun ;
Choudhary, Eric ;
Shen, Hao ;
Liu, Guokun ;
Chen, Peng .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (05) :1845-1852
[4]   Electrochemistry and electrogenerated chemiluminescence of CdTe nanoparticles [J].
Bae, Y ;
Myung, N ;
Bard, AJ .
NANO LETTERS, 2004, 4 (06) :1153-1161
[5]  
Bard A.J., 2004, Electrogenerated Chemiluminescence
[6]  
Biadala L, 2017, NAT NANOTECHNOL, V12, P569, DOI [10.1038/NNANO.2017.22, 10.1038/nnano.2017.22]
[7]  
Boles MA, 2016, NAT MATER, V15, P141, DOI [10.1038/NMAT4526, 10.1038/nmat4526]
[8]   Cobalt-Iron (Oxy)hydroxide Oxygen Evolution Electrocatalysts: The Role of Structure and Composition on Activity, Stability, and Mechanism [J].
Burke, Michaela S. ;
Kast, Matthew G. ;
Trotochaud, Lena ;
Smith, Adam M. ;
Boettcher, Shannon W. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (10) :3638-3648
[9]   Nanomaterials for renewable energy production and storage [J].
Chen, Xiaobo ;
Li, Can ;
Graetzel, Michael ;
Kostecki, Robert ;
Mao, Samuel S. .
CHEMICAL SOCIETY REVIEWS, 2012, 41 (23) :7909-7937
[10]   Imaging Local Heating and Thermal Diffusion of Nanomaterials with Plasmonic Thermal Microscopy [J].
Chen, Zixuan ;
Shan, Xiaonan ;
Guan, Yan ;
Wang, Shaopeng ;
Zhu, Jun-Jie ;
Tao, Nongjian .
ACS NANO, 2015, 9 (12) :11574-11581