Zhao Chang-Xin, Liu Jia-Ning, Wang Juan, Wang Changda, Guo Xin, Li Xi-Yao, Chen Xiao, Song Li, Li Bo-Quan, Zhang Qiang
Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
Advanced Research Institute of Multidisciplinary Science, Beijing Institute of Technology, Beijing 100081, China.
Sci Adv. 2022 Mar 18;8(11):eabn5091. doi: 10.1126/sciadv.abn5091. Epub 2022 Mar 16.
Rechargeable zinc-air batteries call for high-performance bifunctional oxygen electrocatalysts. Transition metal single-atom catalysts constitute a promising candidate considering their maximum atom efficiency and high intrinsic activity. However, the fabrication of atomically dispersed transition metal sites is highly challenging, creating a need for for new design strategies and synthesis methods. Here, a clicking confinement strategy is proposed to efficiently predisperse transitional metal atoms in a precursor directed by click chemistry and ensure successful construction of abundant single-atom sites. Concretely, cobalt-coordinated porphyrin units are covalently clicked on the substrate for the confinement of the cobalt atoms and affording a Co-N-C electrocatalyst. The Co-N-C electrocatalyst exhibits impressive bifunctional oxygen electrocatalytic performances with an activity indicator Δ of 0.79 V. This work extends the approach to prepare transition metal single-atom sites for efficient bifunctional oxygen electrocatalysis and inspires the methodology on precise synthesis of catalytic materials.
可充电锌空气电池需要高性能的双功能氧电催化剂。过渡金属单原子催化剂因其最大的原子效率和高本征活性而成为有前途的候选者。然而,制备原子分散的过渡金属位点极具挑战性,因此需要新的设计策略和合成方法。在此,提出了一种点击限域策略,以在前体中通过点击化学有效地预分散过渡金属原子,并确保成功构建大量单原子位点。具体而言,钴配位的卟啉单元共价连接到基底上以限制钴原子,并提供一种Co-N-C电催化剂。该Co-N-C电催化剂表现出令人印象深刻的双功能氧电催化性能,活性指标Δ为0.79 V。这项工作扩展了制备用于高效双功能氧电催化的过渡金属单原子位点的方法,并激发了催化材料精确合成的方法学。