Interparticle Charge-Transport-Enhanced Electrochemiluminescence of Quantum-Dot Aerogels

被引:96
作者
Gao, Xuwen [1 ]
Jiang, Guocan [2 ]
Gao, Cunyuan [1 ]
Prudnikau, Anatol [2 ]
Huebner, Rene [3 ]
Zhan, Jinhua [1 ]
Zou, Guizheng [1 ]
Eychmueller, Alexander [2 ]
Cai, Bin [1 ]
机构
[1] Shandong Univ, Sch Chem & Chem Engn, Jinan 250100, Peoples R China
[2] Tech Univ Dresden, Phys Chem, D-01069 Dresden, Germany
[3] Helmholtz Zentrum Dresden Rossendorf, Inst Ion Beam Phys & Mat Res, D-01328 Dresden, Germany
关键词
Charge Transfer; Electrochemiluminescence; Electrochemistry; Quantum Dots; Sol-Gel Processes; ELECTROGENERATED CHEMILUMINESCENCE; COLLOIDAL NANOCRYSTALS; EFFICIENT; ELECTROCHEMISTRY; LUMINESCENCE; SURFACE;
D O I
10.1002/anie.202214487
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemiluminescence (ECL) represents a widely explored technique to generate light, in which the emission intensity relies critically on the charge-transfer reactions between electrogenerated radicals. Two types of charge-transfer mechanisms have been postulated for ECL generation, but the manipulation and effective probing of these routes remain a fundamental challenge. Here, we demonstrate the design of quantum dot (QD) aerogels as novel ECL luminophores via a versatile water-induced gelation strategy. The strong electronic coupling between adjacent QDs enables efficient charge transport within the aerogel network, leading to the generation of highly efficient ECL based on the selectively improved interparticle charge-transfer route. This mechanism is further verified by designing CdSe-CdTe mixed QD aerogels, where the two mechanistic routes are clearly decoupled for ECL generation. We anticipate our work will advance the fundamental understanding of ECL and prove useful for designing next-generation QD-based devices.
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页数:7
相关论文
共 42 条
[1]   Collective topo-epitaxy in the self-assembly of a 3D quantum dot superlattice [J].
Abelson, Alex ;
Qian, Caroline ;
Salk, Trenton ;
Luan, Zhongyue ;
Fu, Kan ;
Zheng, Jian-Guo ;
Wardini, Jenna L. ;
Law, Matt .
NATURE MATERIALS, 2020, 19 (01) :49-+
[2]  
[Anonymous], 2015, ANGEW CHEM, V127, P15053
[3]  
[Anonymous], 2016, ANGEW CHEM, V128, P6442
[4]   Sol-gel assembly of CdSe nanoparticles to form porous aerogel networks [J].
Arachchige, Indika U. ;
Brock, Stephanie L. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (24) :7964-7971
[5]  
Boles MA, 2016, NAT MATER, V15, P364, DOI [10.1038/NMAT4578, 10.1038/nmat4578]
[6]   Next-generation in vivo optical imaging with short-wave infrared quantum dots [J].
Bruns, Oliver T. ;
Bischof, Thomas S. ;
Harris, Daniel K. ;
Franke, Daniel ;
Shi, Yanxiang ;
Riedemann, Lars ;
Bartelt, Alexander ;
Jaworski, Frank B. ;
Carr, Jessica A. ;
Rowlands, Christopher J. ;
Wilson, Mark W. B. ;
Chen, Ou ;
Wei, He ;
Hwang, Gyu Weon ;
Montana, Daniel M. ;
Coropceanu, Igor ;
Achorn, Odin B. ;
Kloepper, Jonas ;
Heeren, Joerg ;
So, Peter T. C. ;
Fukumura, Dai ;
Jensen, Klavs F. ;
Jain, Rakesh K. ;
Bawendi, Moungi G. .
NATURE BIOMEDICAL ENGINEERING, 2017, 1 (04)
[7]   Quantum Dots with Highly Efficient, Stable, and Multicolor Electrochemiluminescence [J].
Cao, Zhiyuan ;
Shu, Yufei ;
Qin, Haiyan ;
Su, Bin ;
Peng, Xiaogang .
ACS CENTRAL SCIENCE, 2020, 6 (07) :1129-1137
[8]  
Chuang Chia-Hao M, 2014, Nat Mater, V13, P796, DOI 10.1038/nmat3984
[9]   Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals [J].
Coropceanu, Igor ;
Janke, Eric M. ;
Portner, Joshua ;
Haubold, Danny ;
Nguyen, Trung Dac ;
Das, Avishek ;
Tanner, Christian P. N. ;
Utterback, James K. ;
Teitelbaum, Samuel W. ;
Hudson, Margaret H. ;
Sarma, Nivedina A. ;
Hinkle, Alex M. ;
Tassone, Christopher J. ;
Eychmuller, Alexander ;
Limmer, David T. ;
de la Cruz, Monica Olvera ;
Ginsberg, Naomi S. ;
Talapin, Dmitri, V .
SCIENCE, 2022, 375 (6587) :1422-+
[10]   Electrochemistry and electrogenerated chemiluminescence from silicon nanocrystal quantum dots [J].
Ding, ZF ;
Quinn, BM ;
Haram, SK ;
Pell, LE ;
Korgel, BA ;
Bard, AJ .
SCIENCE, 2002, 296 (5571) :1293-1297