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    界面工程驱动的Fe@生物质碳复合材料电催化水氧化性能

    Electrocatalytic water oxidation performance of Fe@biomass-derived carbon composites

    • 摘要: 生物质衍生的碳材料因其独特的形貌、较高的比表面积以及分级多孔的结构在电催化水分解领域展现出潜力。然而,其固有缺陷如活性位点密度低和结构稳定性较差等问题,严重制约了其实际应用价值。研究通过高压水热碳化一次性筷子形成生物碳(BC),进一步采用浸渍和热处理将Fe修饰在其表面,构建了具有界面协同作用的Fe@BC复合催化剂,并研究了其电催化析氧反应(OER)性能。研究发现,Fe以氧化物的形式分布于BC载体表面。并且随着Fe的引入,BC的晶相和形貌结构发生了改变,形成了多孔的层状结构。重要的是,BC与Fe原子之间形成的Fe-O强界面相互作用能够诱导产生Fe2+与Fe3+双活性中心。随着OER反应的进行,催化剂表面形成更多缺陷羟基氧化物种,有效促进电子重新分布,补充OER过程中Fe位点的电荷累积,从而显著提升并稳定Fe3+和Fe2+活性中心的催化性能。该催化剂在碱性介质中展现出优异的OER催化性能,在电流密度10 mA/cm2和200 mA/cm2的条件下,其电位相对于可逆氢电极分别为1.482 V和1.550 V,显著优于商业RuO2催化剂。此外,该催化剂性能可以稳定保持48 h以上,该研究成果为设计新型高效的生物碳与过渡金属耦合的OER催化体系提供了创新思路。

       

      Abstract: Biomass-derived carbon materials exhibit great potential in the field of electrocatalytic water splitting due to their unique morphologies, high specific surface areas, and hierarchical porous structures. Nevertheless, inherent drawbacks of biomass-derived carbon materials, such as a relatively low density of active sites and inferior structural stability, severely hamper their practical application potential and significantly limit the realization of their full value in real-world scenarios. In this study, biochar (BC) was formed by subjecting disposable chopsticks to high-pressure hydrothermal carbonization. Subsequently, iron (Fe) was further modified on its surface through an impregnation and heat treatment process, resulting in the construction of a Fe@BC composite catalyst with interfacial synergistic effects. Moreover, the electrocatalytic oxygen evolution reaction (OER) performance of this catalyst was investigated. The study found that iron (Fe) was distributed on the surface of the BC support in the form of oxides. Moreover, with the introduction of Fe, the crystal phase and morphological structure of BC were altered, leading to the formation of a porous lamellar structure. Importantly, the strong Fe-O interfacial interaction formed between BC and Fe atoms can induce the generation of dual active centers of Fe2+ and Fe3+. As the oxygen evolution reaction (OER) proceeds, more defective hydroxyl oxide species are formed on the surface of the catalyst, which effectively promotes the redistribution of electrons and replenishes the charge accumulation at the Fe sites during the OER process. As a result, the catalytic performance of the active centers of Fe2+ and Fe3+ is significantly enhanced and stabilized. This catalyst exhibits excellent OER catalytic performance in an alkaline medium. Under the conditions of a current density of 10 mA/cm2 and 200 mA/cm2, its potentials relative to the reversible hydrogen electrode are 1.482 V and 1.550 V respectively, which are significantly superior to those of the commercial RuO2 catalyst. In addition, the performance of this catalyst can be stably maintained for more than 48 hours. The research findings provide innovative ideas for the design of a new type of highly efficient OER catalytic system coupling biochar with transition metals.

       

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