Controllable hydrogen generation through catalytic decomposition of hydrazine monohydrate (N2H4·H2O) holds promise for mobile and portable applications. However, the existing catalysts (such as Ni60Pt40/CeO2, CoPt/CeOx) often suffer from poor stability, and active site poisoning appears an important cause of deactivation. Here, we present a simple yet effective method to address this issue. By adding a Ce3+ salt during the precipitation-deposition process, we observed enhanced interactions between Ni–Pt alloy and CeO2 matrix, impacting the electronic structure and dispersion of Ni–Pt nanoparticles. Thus-obtained Ni4Pt/CeO2 catalyst exhibited an over two-fold increase in activity and an 80% retention after 10 cycles, outperforming conventional methods. The novel approach simultaneously improved activity and stability while maintaining a constant alloy composition. This catalyst demonstrated high activity, 100% H2 selectivity, and good stability in N2H4·H2O decomposition. Additionally, it enabled the construction of a high-capacity N2H4·H2O-based hydrogen generation system with rapid dynamic response.
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