Ru-Enriched Metal–Organic Framework Enabling a Self-Powered Hydrogen Production System

Constructing a direct hydrazine fuel cell (DHzFC)-driven overall hydrazine splitting (OHzS) system is a conceptual idea for hydrogen generation with theoretical zero-energy consumption, which remains a formidable challenge. Herein, a two-dimensional Ru-enriched metal–organic framework catalyst (NiRu-ABDC) is prepared via a self-sacrificing template strategy. The experimental and density functional theory (DFT) calculation results indicate that Ru serves as an active site for both the hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR), endowing NiRu-ABDC∥NiRu-ABDC with outstanding OHzS performance. The DFT results further clarify that Ru incorporation facilitates electron localization and strengthens the M–O bonds in the Ni-ABDC framework, enabling the NiRu-ABDC∥NiRu-ABDC electrolyzer cell to be stable for over 100 h. Further, a self-powered hydrogen production system is constructed with anodic NiRu-ABDC, in which OHzS is successfully powered by synthesized DHzFCs, achieving hydrogen yield of 14.3 mol h–1 m–2, showing its feasibility for practical applications.