Journal
ACS NANO
Volume 15, Issue 11, Pages 18125-18134Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c06796
Keywords
electronic structure tuning; iodine doping; single-atom catalysts; metal-nitrogen-carbon materials; hydrogen evolution reaction
Categories
Funding
- National Natural Science Foundation of China [51902099]
- Hunan high-level talent gathering project [2019RS1021]
- Fundamental Research Funds for the Central Universities [531119200087, 531118010707, JKVJ1211022]
- Innovative Research Groups of Hunan Province [2020JJ1001]
- Hunan Province Natural Science Foundation [2020JJ4204]
- Youth Innovation Promotion Association CAS
- Guangdong Innovative and Entrepreneurial Research Team Program [2017ZT07C341]
- Bureau of Industry and Information Technology of Shenzhen [201901171523]
- Shanghai Rising-star Program [20QA1402400]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
- Frontiers Science Center for Materiobiology and Dynamic Chemistry
- Feringa Nobel Prize Scientist Joint Research Center
- Postgraduate Scientific Research Innovation Project of Hunan Province [CX20200440]
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Iodine doping effectively modulates the electronic structure of single-atom catalysts, improving the catalytic activity of cobalt-nitrogen-carbon catalyst towards the hydrogen evolution reaction. The introduction of iodine dopants optimizes hydrogen adsorption and facilitates HER kinetics, providing an alternative strategy for enhancing SAC performance.
The development of strategies for tuning the electronic structure of the metal sites in single-atom catalysts (SACs) is the key to optimizing their activity. Herein, we report that iodine doping within the carbon matrix of a cobalt-nitrogen-carbon (Co-N-C) catalyst can effectively modulate its electronic structure and catalytic activity toward the hydrogen evolution reaction (HER). The iodine-doped Co-N-C catalyst shows exceptional HER activity in acid with an overpotential of merely 52 mV at 10 mA cm(-2), a small Tafel slope of 56.1 mV dec(-1), making it among the best SACs based on both precious and nonprecious metals. Moreover, this catalyst possesses a high turnover frequency (TOF) value of 1.88 s(-1) (eta = 100 mV), which is about 1 order of magnitude larger than that (0.2 s(-1)) of the iodine-free counterpart. Experimental and theoretical studies demonstrate that the introduction of iodine dopants lowers the chemical oxidation state of the Co sites, resulting in the optimized hydrogen adsorption and facilitated HER kinetics. This work provides an alternative strategy to regulate the electronic structure of SACs for improved performance.
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