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Partial Amorphization of Proton-Conducting Perovskites Triggers Interfacial Water Optimization to Boost Proton
Shijie Gao1, Xixi Wang2, Xiaolin Yu1
1State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, China.
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Modulating the interfacial water structure at the catalyst-electrolyte interface and optimizing the hydrogen adsorption/desorption kinetics of ruthenium-based electrocatalysts are essential for hydrogen evolution reaction (HER), yet these remain significant challenges. Herein, we propose a hybrid catalyst ac-Ru/BaZr0.1Ce0.7Y0.1Yb0.1O3-δ-C (ac-Ru/BZCYYb-C), featuring an amorphous/crystalline substrate fabricated via an in situ electrochemical reconstruction strategy. Comprehensive in situ Raman and electrochemical investigations reveal that partial amorphization of the proton-conducting perovskite BZCYYb optimizes the interfacial water structure. This reconstruction promotes the conversion of 4-coordinated hydrogen-bonded water (4-HB-H2O) into free-H2O and 2-HB-H2O. Such optimized interfacial water structure improves the hydrogen adsorption/desorption kinetics on Ru sites, thus promoting HER kinetics. Consequently, the ac-Ru/BZCYYb-C catalyst demonstrates excellent acidic HER activity, requiring an overpotential of only 17 mV to deliver -10 mA cm-2 and showing remarkable long-term durability for 200 h with negligible degradation. Moreover, PEMWE cell employing ac-Ru/BZCYYb-C as the cathode catalyst achieves 2 A cm-2 at only 1.84 V and maintains outstanding stability over 150 h in pure water at 2 A cm-2.
