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作 者:赵正一 王佳玮 张娟[1] 李嘉丞 吴旭[1] ZHAO Zhengyi;WANG Jiawei;ZHANG Juan;LI Jiacheng;WU Xu(College of Chemistry,Taiyuan University of Technology,Taiyuan 030024,China)
出 处:《功能材料》2024年第7期7022-7030,共9页Journal of Functional Materials
基 金:国家自然科学基金资助项目(22272116)。
摘 要:双碳背景下,电催化CO_(2)制甲醇等化合物有重要研究价值。为了提高CO_(2)的转化率和甲醇的选择性,本文借助兼具酸碱性的铜铝类水滑石(CuAl-LDHs)和具有优异导电性的碳纳米管材料(CNTs),协调构筑了LDHs/CNTs杂化物,实现了两种材料的优势互补,使其制甲醇性能和导电性能双向提高。研究结果表明,相较于LDHs,杂化物中二者良好的分散性和丰富的弱碱位点更有利于CO_(2)分子在其表面大量吸附并快速扩散,同时具有高迁移率的晶格氧和高还原电位的一价铜物种在催化剂表面形成了氧化还原循环,显著降低了传质阻力和电子转移难度,使得CuAl-LDHs/5%CNTs在-0.6 V(针对可逆氢电极)下对甲醇拥有较高的选择性和电流密度,最高可达80.7%和-6.5 mA/cm 2,为开发在低电位高电流密度下具有高CO_(2)转化率的LDHs基电催化剂提供了重要参考。Electrocatalysis of CO_(2) to methanol has important research value in the carbon peaking and carbon neutrality goals.In order to improve the conversion rate of CO_(2) and selectivity of methanol,this paper coordinated the construction of LDHs/CNTs hybrid with acid-alkaline CuAl-LDHs and carbon nanotube materials(CNTs)with excellent electrical conductivity,realizing the complementary advantages of the two materials,and improving their methanol production performance and electrical conductivity in both directions.The results show that compared with LDHs,the good dispersion and abundant weak base sites of the two compounds are more conducive to the adsorption and rapid diffusion of CO_(2) molecules on the surface of the catalyst.Meanwhile,lattice oxygen with high mobility and monovalent copper species with high reduction potential form redox cycles on the catalyst surface,significantly reducing the mass transfer resistance and electron transfer difficulty.The results showed that CuAl-LDHs/5%CNTs had high selectivity and current density towards methanol at-0.6 V(for reversible hydrogen electrodes),up to 80.7%and-6.5 mA/cm 2,providing reference value for the development of LDHs-based electrocatalysts with high CO_(2) conversion at low potential and high current density.
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