Journal
CHEMICAL ENGINEERING JOURNAL
Volume 436, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.135186
Keywords
Alkaline hydrogen evolution reaction; Accelerated water dissociation; Pt nanocluster; Nitrogen-doped carbon; Ordered macroporous structure
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Funding
- National Natural Science Foundation of China [51621001, 52103354]
- Natural Science Foundation of Guangdong Province [2021A1515012362]
- Central South University Faculty Start-Up Fund [202045020]
- High Performance Computing Center of Central South University
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In this study, Pt nanoclusters were uniformly anchored on an ordered macroporous nitrogen-doped carbon support to enhance the electrocatalytic performance for alkaline hydrogen evolution reaction. The catalyst exhibited superior activity and stability compared to the solid counterpart without ordered macropores, and even outperformed commercial Pt/C catalysts.
Developing effective electrocatalysts with reduced Pt content for fast hydrogen evolution reaction (HER) kinetics toward efficient and stable hydrogen production in alkaline media is highly desirable but rather challenging. Herein, Pt nanoclusters (~1.6 nm) uniformly anchored on ordered macroporous nitrogen-doped carbon support (Pt-30/NCM) with only 3.39 wt% Pt loading is rationally constructed via a polystyrene spheres (PS) template method followed by an impregnating method as a highly enhanced electrocatalyst for alkaline HER. Benefiting from the enhanced mass and charge transport via the ordered macroporous carbon structure as well as the strong metal-support interaction between Pt nanoclusters and nitrogen-doped carbon framework, Pt-30/NCM exhibits superior intrinsic activity and operation stability compared to the solid counterpart without ordered macropores (Pt-30/NCS), even affording a more than 10 times higher mass activity and much better operation stability after 3000 cycles than those of commercial 20 wt% Pt/C. The density functional theory (DFT) calculations reveal that the strong coupling between Pt nanoclusters and nitrogen-doped carbon support can induce favorable charge transfer for accelerated water dissociation as well as desirable d-band center position for suitable adsorption and desorption of alkaline HER intermediates, thus contributing to remarkably improved kinetics of hydrogen production.
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