Qiu Yu, Jiao Dongxu, Huang Hong, Wu Jiandong, Wang Mingming, Gao Tianyi, Zhao Xiao, Ge Xin, Zhang Wei, Zheng Weitao, Singh David J, Fan Jinchang, Cui Xiaoqiang
School of Materials Science and Engineering, Key Laboratory of Automobile Materials of MOE, Electron Microscopy Center, Jilin University, Changchun, China.
Key Laboratory of Pathobiology of MOE, Nanomedicine and Translational Research Center, The Third Bethune Hospital of Jilin University, Changchun, China.
Nat Commun. 2025 Jul 2;16(1):6103. doi: 10.1038/s41467-025-61524-4.
Palladium hydride (PdH) metallenes are efficient electrocatalysts for the oxygen reduction reaction (ORR) due to their high atomic utilization and optimized oxygen binding energies modulated by interstitial hydrogen. However, their practical application is restricted by the highly unstable nature of interstitial hydrogen at working temperatures around 353 K. Here, we report that the use of Mn effectively locks hydrogen atoms within the Pd metallenes lattice, resulting in high alkaline ORR performance across a temperature range of 303-353 K. In contrast, the ORR activity of PdH metallenes declines sharply with increasing temperature. At 353 K, the mass activity of PdMnH metallenes at 0.95 V reaches 1.41 A mg, which is 14.1 times higher than that of PdH metallenes. Multiple spectroscopic analyses and theoretical calculations reveal that strong electronic interactions within the immiscible Pd-Mn alloy are critical for locking interstitial hydrogen, thereby enhancing the ORR activity under high temperatures.
氢化钯（PdH）金属烯由于其高原子利用率以及由间隙氢调节的优化氧结合能，是氧还原反应（ORR）的高效电催化剂。然而，在约353 K的工作温度下，间隙氢的高度不稳定性质限制了它们的实际应用。在此，我们报告，使用锰有效地将氢原子锁定在钯金属烯晶格内，从而在303 - 353 K的温度范围内产生高碱性ORR性能。相比之下，PdH金属烯的ORR活性随温度升高而急剧下降。在353 K时，PdMnH金属烯在0.95 V下的质量活性达到1.41 A mg，比PdH金属烯高14.1倍。多种光谱分析和理论计算表明，互不相溶的Pd-Mn合金内的强电子相互作用对于锁定间隙氢至关重要，从而在高温下增强ORR活性。
