Abstract

A new electrocatalyst of Pt single atoms dispersed into Mo 2 C nanocrystals in 3D porous carbon matrix derived from metal-organic frameworks pyrolysis exhibits remarkably enhanced HER activity and stability in 1 M KOH. Hydrogen generation from electrochemical water splitting powered by renewable energy is important to the sustainable society, but the prohibitive cost of current Pt electrocatalyst has impeded the large-scale production of hydrogen by water electrolysis. In this contribution, a new low-Pt electrocatalyst for hydrogen evolution reaction (HER) has been fabricated by a facile one-pot synthesis approach, in which Pt 2+ cations and phosphomolybdic acid confined in the metal–organic frameworks (MOFs) were submitted to pyrolysis to yield Pt single atoms dispersed into Mo 2 C nanocrystals in 3D porous carbon matrix. The as-synthesized Pt 1 -Mo 2 C-C catalyst with Pt content of only 0.7 wt% exhibited remarkably enhanced activity for HER in 1 M KOH, with overpotential at 10 mA/cm 2 lowered from 211 mV to 155 mV and 7-fold higher mass activity (7.14 A/mg Pt ) than the benchmark 20 wt% Pt/C. The promoted activity can be attributed to the electronic interaction between Pt single atoms and Mo 2 C surface, which not only improved water activation but also strengthened hydrogen adsorption, as indicated by FTIR and microcalorimetric characterizations.

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