Accelerating H* Redistribution via Hydrogen Spillover for Enhanced Electrochemical Hydrogen Production From Formaldehyde

Authors:
Publisher website
Google Scholar
Abstract
Producing hydrogen from formaldehyde oxidation reaction (FOR) offers a promising low‐energy approach for generating clean fuel. However, the FOR involves continuous C─H bond cleavage of adsorbed intermediates to generate abundant surface H*. This necessitates rapid transfer and consumption of H* to sustain fast oxidation kinetics. Herein, we developed a hydrogen‐spillover strategy to redistribute these surface H* to accelerate FOR kinetics by constructing RhCu single‐atom alloy supported on a Cu single‐atom‐rich carbon matrix (RhCu@Cu SA NC). In this design, Cu incorporation creates a favorable landscape for H* migration toward the Cu SA NC support, which acts as efficient H* acceptors and H─H coupling centers. Verified through multiple analyses, this hydrogen‐spillover mechanism is demonstrated to enhance FOR activity by accelerating H* redistribution. Consequently, RhCu@Cu SA NC shows outstanding FOR performance, achieving a current density of 800 mA cm − 2 at 0.39 V with nearly 100% H 2 selectivity and excellent durability. When integrated into a hybrid alkali‐acid cell, it provides an open circuit voltage of 1.72 V and peak power density of 152.6 mW cm − 2 with stable H 2 production for over 1200 h at 10 mA cm − 2 . These results demonstrate that hydrogen spillover boosts oxidative electrocatalysis, providing a general design principle for multicomponent catalysts with coordinated hydrogen dynamics.
Funding Information
  • National Natural Science Foundation of China (22278364)
  • National Natural Science Foundation of China (22208296)
  • National Natural Science Foundation of China (22425805)
  • National Natural Science Foundation of China (U22A20432)
  • National Natural Science Foundation of China (22211530045)
  • National Natural Science Foundation of China (22178308)
  • National Natural Science Foundation of China (22578393)
  • National Natural Science Foundation of China (22238008)
  • National Natural Science Foundation of China (U25A203261)
  • National Natural Science Foundation of China (22508349)
  • National Natural Science Foundation of China (12564025)
  • China Postdoctoral Science Foundation (2025M780157)
  • Fundamental Research Funds for the Central Universities (226‐2025‐00043)
  • Fundamental Research Funds for the Central Universities (JC2026TS‐006)
  • Fundamental Research Funds for the Central Universities (XJ2026008901)

This publication has 42 references indexed in Scilit: