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界面电荷传递产生双活性位点的RuO2-NiO/NF高效电催化析氢电极
陈慧, 刘雪华, 林燕, 陈松, 王卫国
PDF(5667 KB)
PDF(5667 KB)
界面电荷传递产生双活性位点的RuO2-NiO/NF高效电催化析氢电极
Interfacial charge transfer induced dual- active-sites of RuO2-NiO/NF electrode for high efficiency electrocatalytic hydrogen evolution
为制备高性能、低成本的稀贵金属电催化析氢材料,采用化学沉淀法结合热分解法制备RuO2-NiO/NF异质结构析氢电催化剂,该电极在碱性析氢反应(HER)中表现出优异的催化活性和稳定性。通过表征、测试以及理论(DFT)计算分析,证明RuO2和NiO结合产生的异质结构界面是该催化剂性能提升的核心,该界面上发生电荷转移导致双活性位点的产生,使不同种类的吸附质在不同活性位点选择性吸附,协同促进了析氢反应的各基元反应步骤,使得该催化剂在碱性析氢反应中表现优异:10 mA·cm-2电流密度下的析氢过电位仅为52 mV,Tafel斜率为47.5 mV·dec-1,100 mV下的TOF达到0.342 s-1,且在200 mA·cm-2的电流密度下、经100 h稳定性测试后仍维持稳定电势。综上所述,本工作从界面工程角度成功构筑RuO2-NiO/NF异质结构催化剂,并对其HER机理进行了探讨,为Ni基化合物异质结构催化剂的构建及在电催化领域的应用提供了新思路。
Renewable energy plays a crucial role in sustainable development amidst the global energy crisis. Hydrogen, owing to its high calorific value and environmental benignity, emerges as a promising energy source for the future. Hydrogen produced through water splitting boasts high purity, zero pollution during production, and recyclability, thereby holding vast potential. Platinum (Pt) stands out as an exceptional catalyst for the hydrogen evolution reaction (HER). While commercial Pt/C exhibits high alkaline HER performance, its high cost, material instability, and scarcity hinder widespread adoption. Consequently, this study focuses on developing a high-performance, low-cost, and less-noble transition metal electrocatalyst for HER via water splitting. Utilizing the thermal decomposition method, the heterostructural RuO2-NiO/NF electrode can be industrially produced based on heterogeneous interface engineering. Specifically, Ni(OH)2 and RuO2·H2O precursors are applied to a nickel foam (NF) substrate using a binder, followed by heating at 450 ℃ for 3 h in air to facilitate precursor decomposition, thereby successfully preparing RuO2-NiO/NF heterostructure electrocatalysts. The RuO2-NiO/NF electrodes exhibit remarkable catalytic activity and stability in alkaline HER. Characterization, testing, and density functional theory (DFT) calculations reveal that the heterostructural interface formed by the binding of RuO2 and NiO significantly enhances catalyst performance. At the interface, charge transfer results in the creation of dual active sites, enabling selective adsorption of different adsorbates at distinct active sites. This synergistically promotes the fundamental reactions of water splitting, leading to exceptional alkaline HER catalyst performance. Under a current density of 10 mA·cm-2 in 1 mol·L-1 KOH solution, an overpotential of 52 mV and a Tafel slope of 47.5 mV·dec-1 are achieved. Additionally, the turnover frequency (TOF) at 100 mV reaches 0.342 s-1, and a stable potential is maintained at a current density of 200 mA·cm-2 after 100 h of stability testing. In summary, a heterostructure RuO2-NiO/NF electrocatalyst has been successfully developed based on interface engineering principles, with a comprehensive investigation of its HER catalytic mechanism. This provides a novel perspective for constructing heterostructure catalysts based on Ni compounds and their application in electrocatalysis.
电催化 / 析氢反应 / 异质结构 / 催化剂 / 密度泛函理论 / 界面工程 / 热分解法
electrocatalysis / hydrogen evolution reaction / heterostructure / catalyst / density functional theory / interface engineering / thermal decomposition method
TB34 / O641.121 / TQ151
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