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Interfacial hydrogen spillover on Pt/C3N4 enables industrial-level alkaline hydrogen evolution reaction
Jian Cui1, Qian Zheng2, Yifeng Zeng1
1State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, China University of Petroleum (Beijing), Beijing 102249, China.
None:
Hydrogen spillover provides a powerful route to overcome hydrogen binding ability and sluggish water dissociation kinetics in alkaline hydrogen evolution reaction (HER). Here, we present a catalyst with Pt nanoparticles supported on a nonmetallic support (C3N4), which achieves efficient hydrogen evolution kinetics and exceptional stability through the hydrogen spillover effect. Density functional theory (DFT) calculations reveal that strong PtN coordination induces interfacial electron transfer from Pt to C3N4, establishing a vertical interfacial electric field that drives hydrogen spillover. As a result, Pt/C3N4-500 delivers industrial-level current densities of 500 and 1000 mA cm-2 at ultralow overpotentials of 89.8 ± 1.5 and 137.7 ± 2.1 mV, respectively, in a three-electrode system. It also maintains stable operation at 500 mA cm-2 for 300 h with a minimal potential variation of 42.2 mV. In situ electrochemical impedance spectroscopy, in situ Raman spectroscopy, and DFT calculations reveal that the C3N4 support induces a hydrogen spillover effect, optimizes the kinetics of H2 desorption (0.8 × 10-4 s), and facilitates the transfer of H* intermediates to the C3N4 (0.37 eV) surface for desorption via low ΔGH⁎ (-0.04 eV) at the interfacial Pt sites. Anion exchange membrane water electrolyzers (AEMWE) using Pt/C3N4-500 as the cathode requires only 1.73 ± 0.02 V to achieve a current density of 1 A cm-2 and operates stably for over 150 h at 1 A cm-2.
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