期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 22, 页码 7454-7465出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.1c00730
关键词
plasma nanotechnology; trimetallic phosphoxide; interface engineering; electrocatalysis; hydrogen generation
资金
- National Natural Science Foundation of China [22061002, 52067002, 51862001, 11665005, 51672249]
- Fundamental Research Funds of Zhejiang Sci-Tech University [2020Y005]
- HighLevel Talents Startup & Innovation 5213 Plan of Xiaoshan District (Hangzhou City)
- Hundred-Talent Voyage Project of Jiangxi Province
- Australian Research Council (ARC)
- QUT Centre for Materials Science (CMS)
By creating a unique heterointerface of Ni, Co, and W phosphoxide phases on a plasma-defect-engineered Ni-Co support, this study has achieved high-performance electrocatalytic properties with high current densities, excellent stability, and durability, outperforming industry benchmarks at industry-relevant current densities.
The fundamental obstacle that only a few part of hydrogen energy is currently produced by industrial electro-catalysis, is in insufficient performance and high cost of even the most advanced catalysts. To meet the demand for high-performance, lasting catalysts at industry-relevant current densities (>= 500 mA cm(-2)) with overpotentials <= 300 mV, here, we uniquely heterointerface the Ni, Co, and W phosphoxide phases in situ on plasma-defect-engineered Ni-Co support (MxO@MxP/PNCF (M = Ni, Co, W) core-shell heterostructure) to dramatically enhance the electrocatalytic performances with very high current densities. The achieved H-2 evolution requires low overpotentials of only 53 and 343 mV for current densities of 10 (j(10)) and 1000 mA cm(-2) (j(1000)) and shows fast reaction kinetics with a small Tafel slope of 40 mV dec(-1). Importantly, the MxO@MxP/PNCF presents spectacular activity at industry-relevant current densities (>j(300)) and outperforms the industry Pt/C benchmark. Our catalyst shows excellent long-term stability and durability with no significant activity loss after 10(4) cycles and 100 h of operation in an alkaline electrolyte. First-principles simulations reveal the best metal-phosphide combination to minimize the Gibbs energy for absorbing H+ ions on the reactive sites and to enhance the desorption of H-2.
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