Engineering Pt-free catalysts for hydrogen evolution reaction (HER) with high activity and stability is of great significance in electrochemical hydrogen production. Herein, in situ chemical H intercalation into ultrafine Pd to activate this otherwise HER-inferior material to form the ultrafine IrPdH hydride as an efficient and stable HER electrocatalyst is proposed. The formation of PdIrH depends on a new hydrogenation strategy via using ethanol as the hydrogen resource. It is demonstrated that H atoms in IrPdH originate from the OH and CH₂ of ethanol, which fills the gap of ethanol as the hydrogen source for the preparation of Pd hydride. Thanks to the incorporation of H/Ir atoms and ultrafine structure, the IrPdH exhibits superior HER activity and stability in the whole pH range. The IrPdH delivers very low overpotentials of 14, 25 and 60 mV at a current density of 10 mA cm^–2 respectively in 0.5 m H₂SO₄, 1 m KOH, and 1 m PBS electrolytes, which are much better than those of commercial Pt/C and most reported noble metal electrocatalysts. Theoretical calculations confirm that interstitial hydrogen availably refines the electronic density of Pd and Ir sites, which optimizes the adsorption of *H and leads to the significant enhancement of HER performance.

中文翻译：

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乙醇诱导的超细 IrPdH 中的氢插入促进了 pH 值的普遍析氢

设计具有高活性和稳定性的析氢反应（HER）无铂催化剂在电化学制氢中具有重要意义。在此，提出了将化学 H 原位嵌入超细 Pd 以激活这种原本 HER 劣质的材料以形成超细 IrPdH 氢化物作为高效且稳定的 HER 电催化剂。PdIrH的形成依赖于一种新的加氢策略，即使用乙醇作为氢资源。证明 IrPdH 中的 H 原子来源于 OH 和 CH ₂ 乙醇，填补了乙醇作为氢源制备氢化钯的空白。由于 H/Ir 原子的结合和超细结构，IrPdH 在整个 pH 范围内表现出优异的 HER 活性和稳定性。IrPdH在 0.5  m H ₂ SO ₄、1  m KOH 和 1  m的电流密度分别为 10 mA cm ^–2时提供 14、25 和 60 mV 的极低过电势PBS 电解质，比商业 Pt/C 和大多数报道的贵金属电催化剂要好得多。理论计算证实，间隙氢有效地改善了 Pd 和 Ir 位点的电子密度，从而优化了 *H 的吸附并导致 HER 性能的显着提高。