Timescale correlation of shallow trap states increases electrochemiluminescence efficiency in carbon nitrides

被引:42
作者
Fang, Yanfeng [1 ]
Yang, Hong [1 ]
Hou, Yuhua [1 ]
Li, Wang [1 ]
Shen, Yanfei [2 ]
Liu, Songqin [1 ]
Zhang, Yuanjian [1 ,3 ]
机构
[1] Jiangsu Engn Res Ctr Carbon Rich Mat & Devices, Sch Chem & Chem Engn, Jiangsu Prov Hitech Key Lab Biomed Res, Nanjing 211189, Peoples R China
[2] Southeast Univ, Med Sch, Nanjing 210009, Peoples R China
[3] Southeast Univ, Zhongda Hosp, Dept Oncol, Nanjing 210009, Peoples R China
基金
中国国家自然科学基金;
关键词
TOTAL-ENERGY CALCULATIONS; ELECTROGENERATED CHEMILUMINESCENCE; SINGLE-ATOM; IMPEDANCE; TIO2; SEMICONDUCTORS;
D O I
10.1038/s41467-024-48011-y
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Highly efficient interconversion of different types of energy plays a crucial role in both science and technology. Among them, electrochemiluminescence, an emission of light excited by electrochemical reactions, has drawn attention as a powerful tool for bioassays. Nonetheless, the large differences in timescale among diverse charge-transfer pathways from picoseconds to seconds significantly limit the electrochemiluminescence efficiency and hamper their broad applications. Here, we report a timescale coordination strategy to improve the electrochemiluminescence efficiency of carbon nitrides by engineering shallow electron trap states via Au-N bond functionalization. Quantitative electrochemiluminescence kinetics measurements and theoretic calculations jointly disclose that Au-N bonds endow shallow electron trap states, which coordinate the timescale of the fast electron transfer in the bulk emitter and the slow redox reaction of co-reagent at diffusion layers. The shallow electron trap states ultimately accelerate the rate and kinetics of emissive electron-hole recombination, setting a new cathodic electrochemiluminescence efficiency record of carbon nitrides, and empowering a visual electrochemiluminescence sensor for nitrite ion, a typical environmental contaminant, with superior detection range and limit. Differences in timescales of electron transfer reactions limit the efficiency of electrochemiluminescence. Here, the authors coordinate the timescales using shallow trap states in carbon nitride to achieve high efficiencies applied in nitrite sensing.
引用
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页数:13
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