Journal
ADVANCED MATERIALS
Volume 33, Issue 12, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202006965
Keywords
hydrogen evolution reaction; metal− organic frameworks; ordered porous structures; superstructures; ultrafine Ru nanoclusters
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Funding
- One Thousand Young Talents Program under the Recruitment Program of Global Experts
- National Natural Science Foundation of China (NSFC) [21771179, 21233009]
- Natural Science Foundation of Fujian Province [2020J01116]
- Strategic Priority Research Program of CAS [XDB20010200]
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This study has developed an ordered macroporous superstructure of N-doped nanoporous carbon anchored with ultrafine Ru nanoclusters for electrocatalytic micro/nanoreactors, showing unparalleled performance for pH-universal hydrogen evolution reactions. The superstructure exhibits significantly higher mass activity compared to the benchmark Pt/C, with remarkably low overpotential and ultra-high turnover frequency in alkaline solution.
The electrochemical hydrogen evolution reaction (HER) is an attractive technology for the mass production of hydrogen. Ru-based materials are promising electrocatalysts owing to the similar bonding strength with hydrogen but much lower cost than Pt catalysts. Herein, an ordered macroporous superstructure of N-doped nanoporous carbon anchored with the ultrafine Ru nanoclusters as electrocatalytic micro/nanoreactors is developed via the thermal pyrolysis of ordered macroporous single crystals of ZIF-8 accommodating Ru(III) ions. Benefiting from the highly interconnected reticular macro-nanospaces, this superstrucure affords unparalleled performance for pH-universal HER, with order of magnitude higher mass activity compared to the benchmark Pt/C. Notably, an exceptionally low overpotential of only 13 mV@10 mA cm(-2) is required for HER in alkaline solution, with a low Tafel slope of 40.41 mV dec(-1) and an ultrahigh turnover frequency value of 1.6 H-2 s(-1) at 25 mV, greatly outperforming Pt/C. Furthermore, the hydrogen generation rates are almost twice those of Pt/C during practical overall alkaline water splitting. A solar-to-hydrogen system is also demonstrated to further promote the application. This research may open a new avenue for the development of advanced electrocatalytic micro/nanoreactors with controlled morphology and excellent performance for future energy applications.
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