Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2023-07-25 , DOI: 10.1016/j.jcis.2023.07.151 Yongchao Hao 1 , Zhongyuan Guo 2 , Huiya Cheng 1 , Chenghao Yao 3 , Shuling Cheng 1 , Lizhi Yi 1 , Hao Li 4
The oxygen evolution reaction (OER) is a key process in various energy storage/generation technologies. Tuning the electronic structures of catalysts is an effective approach to improve the catalyst’s activity. In this work, we synthesized Ce-doped cobalt-organic frameworks with benzene-1, 4-dicarboxylic acid (BDC) as the ligand as efficient OER electrocatalysts (denoted as Co3Ce1 BDC) with excellent stability and improved catalytic performance. The introduced Ce in Co3Ce1 BDC changes the surface configuration and tunes electronic structures of the active Co site, leading to enhanced interaction between intermediates and catalysts. Besides, the specific surface area, reaction kinetics, charge transfer efficiency, and turnover frequency are also improved in the presence of Ce. As a result, the Co3Ce1 BDC demonstrated excellent performance with a low overpotential of 285 mV at a current of 10 mA·cm−2, a preferable Tafel slope of 56.1 mV·dec−1, and an excellent durability in 1 M KOH, indicating the potential for practical applications in water splitting and other energy storage technologies wherein the OER plays a critical role. Comprehensive theoretical calculations and modeling further identified the key role of Ce in modulating the electronic structure and OER activity of cobalt-organic frameworks. Most importantly, this work provides a new strategy to the development of efficient cobalt-organic framework catalysts in OER-related applications.
中文翻译:
调节钴有机框架的电子结构以实现有效的电催化析氧
析氧反应(OER)是各种能量存储/发电技术中的关键过程。调控催化剂的电子结构是提高催化剂活性的有效途径。在这项工作中,我们合成了以苯-1, 4-二羧酸(BDC)为配体的Ce掺杂钴有机骨架作为高效OER电催化剂(表示为Co 3 Ce 1 BDC),具有优异的稳定性和改进的催化性能。Co 3 Ce 1 BDC中引入的 Ce改变了表面构型并调整了活性 Co 位点的电子结构,从而增强了中间体和催化剂之间的相互作用。此外,Ce的存在也提高了比表面积、反应动力学、电荷转移效率和周转频率。结果,Co 3 Ce 1 BDC表现出优异的性能,在10 mA·cm -2的电流下具有285 mV的低过电势、 56.1 mV·dec -1的优选塔菲尔斜率和1 M优异的耐久性。 KOH,表明在水分解和其他储能技术中实际应用的潜力,其中 OER 起着关键作用。综合理论计算和建模进一步确定了 Ce 在调节钴有机骨架的电子结构和 OER 活性中的关键作用。最重要的是,这项工作为 OER 相关应用中高效钴有机骨架催化剂的开发提供了新策略。