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Gas-balancing adsorption strategy towards noble-metal-based nanowire electrocatalysts
Nature Catalysis ( IF 42.8 ) Pub Date : 2024-06-03 , DOI: 10.1038/s41929-024-01167-8
Jiashun Liang , Shenzhou Li , Xuan Liu , Yangyang Wan , Yu Xia , Hao Shi , Siyang Zhang , Hsing-Lin Wang , Gang Lu , Gang Wu , Yunhui Huang , Qing Li

The preparation of noble metal nanowire electrocatalysts is greatly limited by the thermodynamically symmetric growth of face-centred-cubic structures. Here we report a gas-balancing adsorption strategy to prepare ultrathin palladium-, platinum- and gold-based nanowires (diameter < 2 nm) by controlling the competitive adsorption of in situ-generated H2 and CO. We prepare a library of 43 nanowires consisting of the three above-mentioned noble metals as hosts and 14 metals as guests. The ternary Pd85Pt8Ni7H41 nanowires with interstitial hydrogen exhibit impressive mass and specific activities of \(11.1 \, {\rm{A}}\,{\rm{mg}}_{{\rm{PGM}}}^{-1}\) and 13.9 mA cm−2, respectively, for the oxygen reduction reaction at 0.9 VRHE in alkali. Operando X-ray absorption spectroscopy demonstrates breathing-like Pd–Pd bond length and strain changes at the applied potential, with Pd85Pt8Ni7H41 nanowires exhibiting larger compressive strain at relevant potentials, as well as low oxygen coverage. Theoretical calculations suggest that the interstitial hydrogen induces an sd orbital interaction between palladium and hydrogen, which enhances the activity of the oxygen reduction reaction. The Pd85Pt8Ni7H41 nanowires can generate a high power density of 0.87 W cm−2 in H2/air (CO2-free) at 70 °C in an anion-exchange membrane fuel cell.



中文翻译:


贵金属纳米线电催化剂的气体平衡吸附策略



贵金属纳米线电催化剂的制备受到面心立方结构的热力学对称生长的极大限制。在这里,我们报告了一种气体平衡吸附策略,通过控制原位生成的 H 2和 CO 的竞争吸附来制备超薄钯、铂和金基纳米线(直径 < 2 nm)。我们准备了 43 个库由上述三种贵金属作为主体和 14 种金属作为客体组成的纳米线。具有间隙氢的三元 Pd 85 Pt 8 Ni 7 H 41纳米线表现出令人印象深刻的质量和比活性\(11.1 \, {\rm{A}}\,{\rm{mg}}_{{\rm{PGM} }}^{-1}\)和 13.9 mA cm -2 ,分别用于碱中 0.9 V RHE下的氧还原反应。 Operando X射线吸收光谱显示了在施加电位下类似呼吸的Pd-Pd键长和应变变化,其中Pd 85 Pt 8 Ni 7 H 41纳米线在相关电位下表现出更大的压缩应变以及低氧覆盖率。理论计算表明,间隙氢诱导钯和氢之间的s - d轨道相互作用,从而增强了氧还原反应的活性。 Pd 85 Pt 8 Ni 7 H 41纳米线可以在阴离子交换膜燃料电池中在70℃的H 2 /空气(无CO 2 )中产生0.87 W cm -2的高功率密度。

更新日期:2024-06-03
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