Ordered Macroporous Superstructure of Nitrogen-Doped Nanoporous Carbon Implanted with Ultrafine Ru Nanoclusters for Efficient pH-Universal Hydrogen Evolution Reaction.

Wu, Yu-Lin; Li, Xiaofang; Wei, Yong-Sheng; Fu, Zhaoming; Wei, Wenbo; Wu, Xin-Tao; Zhu, Qi-Long; Xu, Qiang · Adv Mater · 2021

basic_science · Level V

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Abstract

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<sup>-2</sup> is required for HER in alkaline solution, with a low Tafel slope of 40.41 mV dec<sup>-1</sup> and an ultrahigh turnover frequency value of 1.6 H<sub>2</sub> s<sup>-1</sup> 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.