Journal
NANO LETTERS
Volume 20, Issue 7, Pages 5008-5016Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c01129
Keywords
Hydrogen evolution reaction; Electrochemiluminescence; Single-nanoparticle; Carbon nitride; Electrochemistry; Blinking
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Funding
- National Natural Science Foundation of China [21974065, 21904063]
- Natural Science Foundation of Jiangsu Province [BK20190279]
- Fundamental Research Funds for the Central Universities [020514380173, 021314380151]
- Washington State University Start-up Fund
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Monitoring and characterization methods that provide performance tracking of hydrogen evolution reaction (HER) at the single-nanoparticle level can greatly advance our understanding of catalysts' structure and activity relationships. Electrochemiluminescence (ECL) microscopy is implemented for the first time to identify HER activities of single nanocatalysts and to provide a direction for further optimization. Here, we develop a novel ECL blinking technique at the single-nanoparticle level to directly monitor H-2 nanobubbles generated from hollow carbon nitride nanospheres (HCNSs). The ECL ON and OFF mechanisms are identified being closely related to the generation, growth, and collapse of H-2 nanobubbles. The power-law distributed durations of ON and OFF states demonstrate multiple catalytic sites with stochastic activities on a single HCNS. The power-law coefficients of ECL blinking increase with improved HER activities from modified HCNSs with other active HER catalysts. Besides, ECL blinking phenomenon provides an explanation for the low cathodic ECL efficiency of semiconductor nanomaterials.
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