Electronic metal–support interaction via Ni defect-induced Ru-modified Ni–CeO2 for enhanced hydrogen oxidation activity,Inorganic Chemistry Frontiers

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Electronic metal–support interaction via Ni defect-induced Ru-modified Ni–CeO2 for enhanced hydrogen oxidation activity
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2024-07-09 , DOI: 10.1039/d4qi01233j
Shuqing Zhou ₁ , Yi Liu ₁ , Lianrui Cheng ₁ , Tayirjan Taylor Isimjan ₂ , Jianniao Tian ₁ , Xiulin Yang ₁

Affiliation

The creation of refined surface vacancies, a crucial bridge between theoretical structural studies and catalyst design, has attracted significant attention. Herein, we utilize a MOF pyrolytic derivatization strategy to create monodispersed Ru nanoparticles anchored on Ni–CeO₂ mesoporous microspheres with abundant Ni vacancies (Ru/Ni–CeO₂). Introducing nickel vacancies in Ru/Ni–CeO₂ is conducive to enhancing electrical conductivity and accelerating mass-charge transfer efficiency. As anticipated, the Ru/Ni–CeO₂ displays admirable hydrogen oxidation reaction (HOR) electrocatalytic activity with exchange current density (j₀) and mass activity reaching 3.27 mA cm⁻² and 1.93 mA g_Ru⁻¹, respectively, surpassing the values for cutting-edge Pt/C and most recorded Ru-based HOR electrocatalysts. Surprisingly, Ru/Ni–CeO₂ demonstrates robust tolerance to 1000 ppm CO, outperforming Pt/C. Integrated analysis suggests that Ni defect-induced directional electron transfer at the Ru/Ni–CeO₂ heterointerface arises from a strong electron–metal support interaction (EMSI) effect between Ru and Ni–CeO₂. This interaction optimizes the adsorption of H and OH, thereby enhancing HOR behavior.

中文翻译：

通过 Ni 缺陷诱导的 Ru 改性 Ni-CeO2 实现电子金属-载体相互作用，增强氢氧化活性

精细表面空位的产生是理论结构研究和催化剂设计之间的重要桥梁，引起了人们的广泛关注。在此，我们利用 MOF 热解衍生化策略来制备锚定在具有丰富 Ni 空位的 Ni-CeO ₂ 介孔微球上的单分散 Ru 纳米颗粒（Ru/Ni-CeO ₂ ）。在Ru/Ni-CeO ₂ 中引入镍空位有利于增强导电性并加速质荷转移效率。正如预期的那样，Ru/Ni-CeO ₂ 显示出令人惊叹的氢氧化反应 (HOR) 电催化活性，交换电流密度 (j ₀ ) 和质量活性达到 3.27 mA cm ⁻² 和 1.93 mA g _Ru ⁻¹ 分别超过了尖端 Pt/C 和大多数记录的 Ru 基 HOR 电催化剂的值。令人惊讶的是，Ru/Ni–CeO ₂ 表现出对 1000 ppm CO 的强大耐受性，优于 Pt/C。综合分析表明，Ni 缺陷诱导的 Ru/Ni-CeO ₂ 异质界面上的定向电子转移源于 Ru 和 Ni-CeO ₂ 之间强电子-金属支持相互作用（EMSI）效应。 b10> .这种相互作用优化了 H 和 OH 的吸附，从而增强了 HOR 行为。

更新日期：2024-07-10

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