Journal
ACS NANO
Volume 12, Issue 5, Pages 4148-4155Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.7b08724
Keywords
electrochemical catalysis; hydrogen evolution reaction; carbon; nickel; polar
Categories
Funding
- World Premier International Center for Materials Nanoarhitectonics (MANA) of the National Institute for Material Science (NIMS)
- Ministry of Education and Science of the Russian Federation (Increase Competitiveness Program of NUST MISiS) [K2-2017-082]
- Australian Laureate Fellowship [FL160100089]
- QUT Project [322120-0355/51]
- RFBR [16-32-60138 mol_a_dk]
- 1000 Youth Talent plan project
- Excellent One Hundred project of Beijing Jiaotong University
- [11.937.2017]
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Electrocatalytic hydrogen evolution reaction (HER) in alkaline solution is hindered by its sluggish kinetics toward water dissociation. Nickel-based catalysts, as low-cost and effective candidates, show great potentials to replace platinum (Pt)-based materials in the alkaline media. The main challenge regarding this type of catalysts is their relatively poor durability. In this work, we conceive and construct a charge-polarized carbon layer derived from carbon quantum dots (CQDs) on Ni3N nanostructure (Ni3N@CQDs) surfaces, which simultaneously exhibit durable and enhanced catalytic activity. The Ni3N@CQDs shows an overpotential of 69 mV at a current density of 10 mA cm(-2) in a 1 M KOH aqueous solution, lower than that of Pt electrode (116 mV) at the same conditions. Density functional theory (DFT) simulations reveal that Ni3N and interfacial oxygen polarize charge distributions between originally equal C-C bonds in CQDs. The partially negatively charged C sites become effective catalytic centers for the key water dissociation step via the formation of new C-H bond (Volmer step) and thus boost the HER activity. Furthermore, the coated carbon is also found to protect interior Ni3N from oxidization/hydroxylation and therefore guarantees its durability. This work provides a practical design of robust and durable HER electrocatalysts based on nonprecious metals.
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