Qiu Yu, Sun Mingzi, Wu Jiandong, Chai Chunxiao, Wang Shengwei, Huang Hong, Zhao Xiao, Jiao Dongxu, Xu Shan, Wang Dewen, Ge Xin, Zhang Wei, Zheng Weitao, Song Yujiang, Fan Jinchang, Huang Bolong, Cui Xiaoqiang
School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Electron Microscopy Center, Jilin University, 2699 Qianjin Street, Changchun, 130012, China.
Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong SAR, China.
Nat Commun. 2025 Jun 6;16(1):5262. doi: 10.1038/s41467-025-60400-5.
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. PdPbH metallenes exhibit a high mass activity of 1.36 A mg 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 O while single Pb atoms enhance O adsorption strength. The electroactive PdPbH 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.
氧还原反应（ORR）的效率受到传统氧缔合途径中比例关系的限制。为了打破这种限制，我们提出了一种方法，通过在钯烯中共同限制单个p区（铟、锡、铅）原子和间隙氢原子来有效激活氧解离途径，从而获得良好的ORR性能。PdPbH钯烯在0.95 V（相对于可逆氢电极）下表现出1.36 A mg的高质量活性，比基准Pt/C高46.9倍。在50000次电位循环后最小的性能衰减证实了良好的稳定性。原位振动光谱研究和理论计算表明，间隙氢原子促进了氧的直接解离，而单个铅原子增强了氧的吸附强度。电活性PdPbH钯烯归因于氢和铅原子诱导的钯4d轨道上移。这项研究为开发高效ORR电催化剂提供了关键灵感。
