Constructing Ru-O-TM Bridge in NiFe-LDH Enables High Current Hydrazine-assisted H2 Production,Advanced Materials

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Constructing Ru-O-TM Bridge in NiFe-LDH Enables High Current Hydrazine-assisted H2 Production
Advanced Materials ( IF 27.4 ) Pub Date : 2024-05-09 , DOI: 10.1002/adma.202401694
Yin Zhu ₁ , Yanxu Chen ₁ , Yafei Feng ₁ , Xiangmin Meng ₂ , Jing Xia ₂ , Genqiang Zhang ₁

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Hydrazine oxidation-assisted water splitting is a critical technology to tackle the high energy consumption in large-scale H₂ production. Ru-based electrocatalysts hold promise for synergetic hydrogen reduction (HER) and hydrazine oxidation (HzOR) catalysis but are hindered by excessive superficial adsorption of reactant intermediate. Herein, this work designs Ru cluster anchoring on NiFe-LDH (denoted as Ru_c/NiFe-LDH), which effectively enhances the intermediate adsorption capacity of Ru by constructing Ru─O─Ni/Fe bridges. Notably, it achieves an industrial current density of 1 A cm⁻² at an unprecedentedly low voltage of 0.43 V, saving 3.94 kWh m⁻³_H2 in energy, and exhibits remarkable stability over 120 h at a high current density of 5 A cm⁻². Advanced characterizations and theoretical calculation reveal that the presence of Ru─O─Ni/Fe bridges widens the d-band width (W_d) of the Ru cluster, leading to a lower d-band center and higher electron occupation on antibonding orbitals, thereby facilitating moderate adsorption energy and enhanced catalytic activity of Ru.

中文翻译：

在 NiFe-LDH 中构建 Ru-O-TM 桥可实现高电流肼辅助氢气生产

联氨氧化辅助水分解是解决大规模H ₂生产高能耗问题的关键技术。钌基电催化剂有望实现协同氢还原（HER）和肼氧化（HzOR）催化，但受到反应物中间体过度表面吸附的阻碍。本工作设计了锚定在NiFe-LDH上的Ru簇（表示为Ru _c /NiFe-LDH），通过构建Ru─O─Ni/Fe桥，有效增强了Ru的中间吸附能力。值得注意的是，它在0.43 V的前所未有的低电压下实现了1 A cm ^-2的工业电流密度，节省了3.94 kWh m ^-3 _H2的能源，并且在5 A cm ^-的高电流密度下在120小时内表现出卓越的稳定性。 ² .先进的表征和理论计算表明，Ru─O─Ni/Fe桥的存在拓宽了Ru团簇的d带宽度（W _d ），导致d带中心更低，反键轨道上的电子占据更高，从而促进Ru的适度吸附能并增强催化活性。

更新日期：2024-05-09

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