Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-11816-3
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Funding
- National Natural Science Foundation of China [21834004, 21327902, 21427807, 21605081]
- Natural Science Foundation of Jiangsu Province [BK20160638]
- International Cooperation Foundation from the Ministry of Science and Technology [2016YFE0130100]
- Fundamental Research Funds for the Central Universities [020514380173]
- Excellent Research Program of Nanjing University [ZYJH004]
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Measurement of electron transfer at single-molecule level is normally restricted by the detection limit of faraday current, currently in a picoampere to nanoampere range. Here we demonstrate a unique graphene-based electrochemical microscopy technique to make an advance in the detection limit. The optical signal of electron transfer arises from the Fermi level-tuned Rayleigh scattering of graphene, which is further enhanced by immobilized gold nanostars. Owing to the specific response to surface charged carriers, graphene-based electrochemical microscopy enables an attoampere-scale detection limit of faraday current at multiple individual gold nanoelectrodes simultaneously. Using the graphene-based electrochemical microscopy, we show the capability to quantitatively measure the attocoulomb-scale electron transfer in cytochrome c adsorbed at a single nanoelectrode. We anticipate the graphene-based electrochemical microscopy to be a potential electrochemical tool for in situ study of biological electron transfer process in organelles, for example the mitochondrial electron transfer, in consideration of the anti-interference ability to chemicals and organisms.
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