Cao Yiwen, Zhang Jieling, Han Jinxiu, Li Guoxiang, Ma Wenjing, Zheng Haoquan, Liang Zuozhong, Cao Rui
Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China.
Chemistry. 2025 Jul 11;31(39):e202501464. doi: 10.1002/chem.202501464. Epub 2025 Jun 24.
The design and development of efficient oxygen reduction reaction (ORR) electrocatalysts have become a key challenge for fuel cells and metal-air batteries. As a cutting-edge field in electrocatalysis, single-atom catalysts have been widely used in ORR due to their maximum atomic utilization and tunable coordination environment. In this study, multinuclear metal clusters were selected as precursors to construct metal nanoparticles and single-atomic metal sites doped carbon materials for electrocatalytic ORR. Specifically, Co-based metal clusters CoO were prepared as precursors and Zn-based zeolitic imidazolate frameworks ZIF-8 were selected as supports. The resulting metal Co-supported nitrogen-doped carbon (Co@NC) materials were obtained by pyrolyzing ZIF-8-CoO hybrids. Both Co nanoparticles and single-atomic Co-N sites were observed on porous NC supports. Porous structures were attributed to the departure of Zn and O at the high-temperature. Co@NC catalyst exhibits a half-wave potential of 0.86 V (vs. reversible hydrogen electrode, vs. RHE) for the ORR measured in a 0.1 M KOH solution. This work provides a new idea for constructing single-atomic catalysts for electrocatalysis using multinuclear metal clusters as active sites.
高效氧还原反应（ORR）电催化剂的设计与开发已成为燃料电池和金属空气电池的关键挑战。作为电催化领域的前沿方向，单原子催化剂因其最大的原子利用率和可调控的配位环境而被广泛应用于ORR。在本研究中，选择多核金属簇作为前驱体，构建用于电催化ORR的金属纳米颗粒和单原子金属位点掺杂的碳材料。具体而言，制备了Co基金属簇CoO作为前驱体，并选择Zn基沸石咪唑酯骨架ZIF-8作为载体。通过热解ZIF-8-CoO杂化物得到金属Co负载的氮掺杂碳（Co@NC）材料。在多孔NC载体上观察到了Co纳米颗粒和单原子Co-N位点。多孔结构归因于高温下Zn和O的离去。Co@NC催化剂在0.1 M KOH溶液中对ORR的半波电位为0.86 V（相对于可逆氢电极，相对于RHE）。这项工作为使用多核金属簇作为活性位点构建用于电催化的单原子催化剂提供了新思路。
