| 引用本文: | 公维佳,张鸿宇,杨柳,唐小斌.钴氮共掺杂碳基电催化剂的制备及性能调控[J].哈尔滨工业大学学报,2022,54(2):40.DOI:10.11918/202106124 |
| GONG Weijia,ZHANG Hongyu,YANG Liu,TANG Xiaobin.Fabrication and performance optimization of cobalt/nitrogen co-doped carbon-based electrocatalyst[J].Journal of Harbin Institute of Technology,2022,54(2):40.DOI:10.11918/202106124 |
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| 摘要: |
| 贵金属基电催化剂是促进燃料电池及金属-空气电池技术发展的关键材料,然而,其单一的氧还原/氧析出催化功能及高昂的制备成本制约了其推广应用。为此,开发低成本、高效的非贵金属双功能电催化剂至关重要。以核壳金属有机框架（MOFs）为前驱体,通过高温煅烧法制备具有核壳结构、高催化活性、高导电性的钴/氮共掺杂碳基电催化剂（Co/Co3O4@NGC）。结果表明:煅烧温度是影响电催化剂微纳结构、物化组成和催化活性的关键因素,最佳烧结温度为900 ℃；制备的电催化剂（Co/Co3O4@NGC-900）具有清晰的核壳结构和3D十二面体形貌,微表面遍布Co/Co3O4纳米颗粒和Co-Nx位点。同时,Co/Co3O4@NGC-900有机地结合了多元活性成分（如活性Co/Co3O4纳米颗粒、Co-Nx及N掺杂）和高度石墨化碳基底的共同作用,具备高效的氧还原性（ORR,起始电位为0.89 V、半波电位为0.82 V、塔菲尔斜率为58.1 mV/dec、传荷电阻为26.6 Ω）和氧析出性（OER,过电势为410 mV、塔菲尔斜率为132 mV/dec、传荷电阻为24.5 Ω）,且具有与传统贵金属基电催化剂（Pt/C, RuO2/C）相匹配的电催化性能,在保障高效电催化活性的前提下实现了催化剂制造成本的大幅削减,为新型MOFs电催化材料的制备和应用提供了理论和技术支撑。 |
| 关键词: 核壳金属有机框架 钴/氮共掺杂 电催化剂制备 Co/Co3O4 催化活性 |
| DOI：10.11918/202106124 |
| 分类号:O643.36 |
| 文献标识码:A |
| 基金项目:城市水资源与水环境国家重点实验室开放课题(QA202012);东北农业大学“学术骨干”项目(20XG06) |
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| Fabrication and performance optimization of cobalt/nitrogen co-doped carbon-based electrocatalyst |
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GONG Weijia1,ZHANG Hongyu1,YANG Liu2,TANG Xiaobin2
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(1.School of Engineering, Northeast Agricultural University, Harbin 150030, China; 2.State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology), Harbin 150090, China)
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| Abstract: |
| Noble metal-based electrocatalysts are the key materials to promote the technical development of fuel cells and metal-air batteries. However, the single catalytic function towards oxygen reduction/oxygen evolution and the prohibitive cost restrict their extensive application. Therefore, it is of great significance to develop non-noble metal-based bi-functional electrocatalysts with low-cost and high-efficiency. In this study, taking core-shell metal organic frameworks (MOFs) as precursors, cobalt/nitrogen co-doped carbon-based electrocatalyst (Co/Co3O4@NGC) was fabricated using high-temperature calcination technology, with a core-shell structure, high catalytic activity, and high conductivity. Results show that the calcination temperature was the key factor affecting the micro-nano structure, physicochemical composition, and catalytic activity of the electrocatalyst. The optimal temperature of calcination was 900 ℃. The fabricated electrocatalyst (Co/Co3O4@NGC-900) had a clear core-shell structure and 3D-dodecahedron morphology with Co/Co3O4 nanoparticles and Co-Nx sites on its micro-surface. In addition, Co/Co3O4@NGC-900 inherently combined the synergistic effects of both multiple active ingredients (e.g., active Co/Co3O4 nanoparticles, Co-Nx, and N dopants) and highly graphitized carbon substrates, and thus exhibited efficient oxygen reduction performance (ORR, onset potential of 0.89 V, half-wave potential of 0.82 V, Tafel slope of 58.1 mV/dec, and charge transfer resistance of 26.6 Ω) and oxygen evolution performance (OER, overpotential of 410 mV, Tafel slope of 132 mV/dec, and charge transfer resistance of 24.5 Ω). Therefore, Co/Co3O4@NGC-900 exerted electrocatalytic performance comparable to that of typical noble metal-based electrocatalysts (e.g., Pt/C, RuO2/C), and achieved significant reduction of catalyst fabrication cost on the premise of ensuring its high-efficient electrocatalytic activity, providing theoretical and technical support for the fabrication and application of innovative MOFs derived electrocatalytic materials. |
| Key words: core-shell metalorganic framework (MOF) cobalt/nitrogen co-doped electrocatalyst fabrication Co/Co3O4 catalytic activity |
