Improving Alkaline Hydrogen Oxidation through Dynamic Lattice Hydrogen Migration in Pd@Pt Core‐Shell Electrocatalysts
Tonghui Zhao, Mengting Li, Dongdong Xiao, Xiaoju Yang, Lulu An, Zhiping Deng, Tao Shen, Mingxing Gong, Yi Chen, Hongfang Liu, Ligang Feng, Xuan Yang, Li Li, Deli Wang
Abstract
Abstract Tracking the trajectory of hydrogen intermediates during hydrogen electro‐catalysis is beneficial for designing synergetic multi‐component catalysts with division of chemical labor. Herein, we demonstrate a novel dynamic lattice hydrogen (LH) migration mechanism that leads to two orders of magnitude increase in the alkaline hydrogen oxidation reaction (HOR) activity on Pd@Pt over pure Pd, even ≈31.8 times mass activity enhancement than commercial Pt. Specifically, the polarization‐driven electrochemical hydrogenation process from Pd@Pt to PdH x @Pt by incorporating LH allows more surface vacancy Pt sites to increase the surface H coverage. The inverse dehydrogenation process makes PdH x as an H reservoir, providing LH migrates to the surface of Pt and participates in the HOR. Meanwhile, the formation of PdH x induces electronic effect, lowering the energy barrier of rate‐determining Volmer step, thus resulting in the HOR kinetics on Pd@Pt being proportional to the LH concentration in the in situ formed PdH x @Pt. Moreover, this dynamic catalysis mechanism would open up the catalysts scope for hydrogen electro‐catalysis.