Boosting oxygen reduction performances in Pd-based metallenes by co-confining interstitial H and p-block single atoms
Yu Qiu, Mingzi Sun, Jiandong Wu, Chunxiao Chai, Shengwei Wang, Hong Huang, Xiao Zhao, Dongxu Jiao, Shan Xu, Dewen Wang, Xin Ge, Wei Zhang, Weitao Zheng, Yujiang Song, Jinchang Fan, Bolong Huang, Xiaoqiang Cui
Abstract
The efficiency of the oxygen reduction reaction (ORR) is limited by the scaling relationship in the conventional oxygen associative pathway. To break such limitations, we present an approach to effectively activate the oxygen dissociative pathway through co-confining single p-block (In, Sn, Pb) atoms and interstitial H atoms within Pd metallenes, leading to good ORR performance. PdPbHx metallenes exhibit a high mass activity of 1.36 A mg−1 at 0.95 V (vs. RHE), which is 46.9 times higher than that of the benchmark Pt/C. The minimal performance decay after 50,000 potential cycles confirms a good stability. In situ vibrational spectroscopy investigations and theoretical calculations highlight that interstitial H atoms facilitate the direct dissociation of O2 while single Pb atoms enhance O2 adsorption strength. The electroactive PdPbHx metallenes is attributed to the up-shifted Pd-4d orbitals induced by H and Pb atoms. This research supplies critical inspiration for developing highly efficient ORR electrocatalysts. The oxygen reduction reaction (ORR) is limited by the scaling relationship in the conventional oxygen associative pathway. In this study, single p-block atoms and interstitial H are incorporated into Pd metallenes favoring the direct dissociation mechanism, leading to high alkaline ORR performance.