Quantum Dots with Highly Efficient, Stable, and Multicolor Electrochemiluminescence

被引：139

作者：

Cao, Zhiyuan ^{[1
]}

Shu, Yufei ^{[1
]}

Qin, Haiyan ^{[1
]}

Su, Bin ^{[1
]}

Peng, Xiaogang ^{[1
]}

机构：

[1] Zhejiang Univ, Ctr Chem High Performance & Novel Mat, Inst Analyt Chem, Dept Chem, Hangzhou 310058, Peoples R China

来源：

ACS CENTRAL SCIENCE | 2020年 / 6卷 / 07期

基金：

中国国家自然科学基金;

关键词：

NEAR-INFRARED ELECTROCHEMILUMINESCENCE; ELECTROGENERATED CHEMILUMINESCENCE; CDSE NANOCRYSTALS; SEMICONDUCTOR NANOCRYSTALS; ELECTROCHEMISTRY; IMMUNOASSAY; EMISSION; ELECTRON; SURFACE; SIZE;

D O I：

10.1021/acscentsci.0c00484

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Outstanding photoluminescence (PL) and electro-luminescence properties of quantum dots (QDs) promise possibilities for them to meet challenging expectations of electrochemiluminescence (ECL), which at present relies on inefficient and spectral-irresolvable emitters based on transition-metal complexes (such as Ru(bpy)(3)(2+)). However, ECL is reported to be extremely sensitive to the surface traps on the QDs likely because of the spatially and temporally separated electrochemical charge injections. Results here reveal that, by engineering the interior inorganic structure (CdSe/CdS/ZnS core/shell/shell structure) and inorganic-organic interface using new synthetic methods, the trap-insensitive QDs with near-unity PL quantum yield and monoexponential PL decay dynamics in water generated narrow band-edge ECL with efficiencies about six orders of magnitude higher than that of the standard Ru(bpy)(3)(2+)). The band-edge and spectrally resolved ECL from CdSe/CdS/ZnS core/shell/shell QDs demonstrated a new readout scheme using electrochemical potential. Excellent ECL performance of QDs uncovered here offer opportunities to realize the full potential of ECL for biomedical detection and diagnosis.

引用

页码：1129 / 1137

页数：9

共 65 条

[1] Photochemical instability of CdSe nanocrystals coated by hydrophilic thiols [J].

Aldana, J ;

Wang, YA ;

Peng, XG .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2001, 123 (36) :8844-8850

[2] Electrochemistry and electrogenerated chemiluminescence of CdTe nanoparticles [J].

Bae, Y ;

Myung, N ;

Bard, AJ .

NANO LETTERS, 2004, 4 (06) :1153-1161

[3] Semiconductor nanocrystals as fluorescent biological labels [J].

Bruchez, M ;

Moronne, M ;

Gin, P ;

Weiss, S ;

Alivisatos, AP .

SCIENCE, 1998, 281 (5385) :2013-2016

[4] ELECTRON ELECTRON AND ELECTRON-HOLE INTERACTIONS IN SMALL SEMICONDUCTOR CRYSTALLITES - THE SIZE DEPENDENCE OF THE LOWEST EXCITED ELECTRONIC STATE [J].

BRUS, LE .

JOURNAL OF CHEMICAL PHYSICS, 1984, 80 (09) :4403-4409

[5] Quantum dot bioconjugates for ultrasensitive nonisotopic detection [J].

Chan, WCW ;

Nie, SM .

SCIENCE, 1998, 281 (5385) :2016-2018

[6]

Chen O, 2013, NAT MATER, V12, P445, DOI [10.1038/NMAT3539, 10.1038/nmat3539]

[7] (CdSe)ZnS core-shell quantum dots: Synthesis and characterization of a size series of highly luminescent nanocrystallites [J].

Dabbousi, BO ;

RodriguezViejo, J ;

Mikulec, FV ;

Heine, JR ;

Mattoussi, H ;

Ober, R ;

Jensen, KF ;

Bawendi, MG .

JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (46) :9463-9475

[8] Solution-processed, high-performance light-emitting diodes based on quantum dots [J].

Dai, Xingliang ;

Zhang, Zhenxing ;

Jin, Yizheng ;

Niu, Yuan ;

Cao, Hujia ;

Liang, Xiaoyong ;

Chen, Liwei ;

Wang, Jianpu ;

Peng, Xiaogang .

NATURE, 2014, 515 (7525) :96-99

[9] Deciphering exciton-generation processes in quantum-dot electroluminescence [J].

Deng, Yunzhou ;

Lin, Xing ;

Fang, Wei ;

Di, Dawei ;

Wang, Linjun ;

Friend, Richard H. ;

Peng, Xiaogang ;

Jin, Yizheng .

NATURE COMMUNICATIONS, 2020, 11 (01)

[10] Enhanced solid-state electrochemiluminescence of CdS nanocrystals composited with carbon nanotubes in H2O2 solution [J].

Ding, Shou-Nian ;

Xu, Jing-Juan ;

Chen, Hong-Yuan .

CHEMICAL COMMUNICATIONS, 2006, (34) :3631-3633

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