International Journal of Hydrogen Energy ( IF 8.1 ) Pub Date : 2021-05-08 , DOI: 10.1016/j.ijhydene.2021.04.084 Yuanyuan Guo , Qi Huang , Junyang Ding , Li Zhong , Ting-Ting Li , Junqing Pan , Yue Hu , Jinjie Qian , Shaoming Huang
The rational design and facile synthesis of transition metal-based catalysts supported by carbon nanomaterials with high activity, selectivity and stability remain a great challenge. Recently, the low-cost, stable and high-performance electrocatalysts for efficient oxygen evolution reaction (OER) derived from porous metal-organic framework (MOF) precursors have attracted numerous attention. Herein, a new type of CoMo carbide/nitride embedded in the flower-like carbon materials (CoMo-MI-T, MI = 2-Methylimidazole, T = 400, 500, 600, 700 °C) has been synthesized by a simple pyrolysis, in which bimetallic CoMo-MI precursors can be conveniently converted from crystalline cobalt-based MOFs of Co-MI by solvothermal reaction. The pyrolyzed CoMo-MI-T series exhibits a hierarchically porous nanostructure, high Co3Mo3C/N content, suitable N-doping, graphitic carbon layers as well as well-preserved flower-shaped morphology, which shows an excellent OER performance. Among them, the most optimal CoMo-MI-600 owns the small overpotential of 316 mV at 10 mA cm−2 and Tafel slope of 89.9 mV dec−1 in 1.0 M KOH solution. Meanwhile, the rotating ring-disk electrode technique is examined to verify near 4-electron transfer process for CoMo-MI-600 together with a high Faradaic efficiency of 98.7%. The well-performed CoMo-MI-600 electrocatalyst may be stemmed from the best balance of the synergistic effect of abundant multi-component, suitable electrical conductivity and large porosity. The current work will provide a new route to prepare MOF-derived bimetallic active sites in porous carbon nanomaterials with satisfactory activity and robust stability in the relevant energy applications.
中文翻译:
来自双金属 MOF 前驱体的 CoMo 碳化物/氮化物可提高 OER 性能
具有高活性、选择性和稳定性的碳纳米材料负载过渡金属基催化剂的合理设计和简便合成仍然是一个巨大的挑战。最近,源自多孔金属有机骨架 (MOF) 前驱体的低成本、稳定和高性能的用于高效析氧反应 (OER) 的电催化剂引起了广泛关注。在此,通过简单的热解合成了一种嵌入花状碳材料(CoMo-MI-T,MI = 2-甲基咪唑,T = 400, 500, 600, 700 °C)中的新型 CoMo 碳化物/氮化物,其中双金属CoMo-MI前体可以通过溶剂热反应方便地从Co-MI的结晶钴基 MOF 转化而来。热解CoMo-MI-T系列具有分层多孔纳米结构、高 Co 3 Mo 3 C/N 含量、合适的 N 掺杂、石墨碳层以及保存完好的花形形态,显示出优异的 OER 性能。其中,最优化的CoMo-MI-600在10 mA cm -2 下具有316 mV的小过电位和在1.0 M KOH溶液中89.9 mV dec -1 的Tafel斜率。同时,检查旋转环盘电极技术以验证CoMo-MI-600 的近 4 电子转移过程以及 98.7% 的高法拉第效率。性能良好的CoMo-MI-600电催化剂可能源于多组分、合适的导电性和大孔隙率的协同效应的最佳平衡。目前的工作将为在多孔碳纳米材料中制备 MOF 衍生的双金属活性位点提供一条新途径,该材料在相关能源应用中具有令人满意的活性和强大的稳定性。