Chen Zhengle, Yang Zhiqing, Li Xinyuan, Li Longhua, Lin Hua
School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, P. R. China.
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, P. R. China.
Dalton Trans. 2024 May 28;53(21):9011-9020. doi: 10.1039/d4dt00915k.
The development of efficient non-noble metal electrocatalysts for the oxygen evolution reaction (OER) under acidic conditions remains a critical challenge. Herein, we report a N-doped carbonaceous component-engineered CoO (NCEC) catalyst synthesized the sol-gel method. Dopamine hydrochloride (DA)-derived nitrogen-doped carbonaceous components were found to boost the OER performance of CoO. The optimized catalyst can reach an overpotential as low as 330 mV in 1 M HSO at a current density of 10 mA cm and maintains a good long-term stability of 60 hours. In particular, we found that the thermodynamic overpotential was inversely proportional to the content of oxidized N and pyridinic N, whereas it was directly proportional to the pyrrolic-N content. Our experiments and density functional theory (DFT) calculations confirm that the optimized catalyst exhibits enhanced charge transfer and the oxidized N species on CoO is responsible for the high catalytic activity. Our study suggests that the performance of NCEC in acidic media can be further optimized by enhancing the content of oxidized N species.
开发用于酸性条件下析氧反应(OER)的高效非贵金属电催化剂仍然是一项严峻挑战。在此,我们报道了一种通过溶胶 - 凝胶法合成的氮掺杂碳质组分工程化的CoO(NCEC)催化剂。发现盐酸多巴胺(DA)衍生的氮掺杂碳质组分可提高CoO的OER性能。优化后的催化剂在1 M HSO中,电流密度为10 mA cm时,过电位可低至330 mV,并保持60小时的良好长期稳定性。特别地,我们发现热力学过电位与氧化态N和吡啶型N的含量成反比,而与吡咯型N的含量成正比。我们的实验和密度泛函理论(DFT)计算证实,优化后的催化剂表现出增强的电荷转移,并且CoO上的氧化态N物种是高催化活性的原因。我们的研究表明,通过提高氧化态N物种的含量可以进一步优化NCEC在酸性介质中的性能。