Liu Chunlian, Yang Ruizhe, Wang Jiacheng, Liu Bowen, Chang Xiaowan, Feng Pingxian, Zhang Xuanzhen, Zhong Lijie, Zhao Xiaoli, Niu Li, Gan Shiyu, Xi Yuebin, Huang Ming, Wang Huan
Guangdong Engineering Technology Research Center for Sensing Materials Devices, Guangzhou Key Laboratory of Sensing Materials Devices School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou, 510006, China.
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 611731, China.
Angew Chem Int Ed Engl. 2025 May;64(21):e202501266. doi: 10.1002/anie.202501266. Epub 2025 Mar 16.
The design of cost-effective and efficient catalysts based on transition metal-based electrocatalysts for the oxygen reduction reaction (ORR) is crucial yet challenging for energy-conversion devices like metal-air batteries. In this work, we present a cost-effective strategy for preparing catalysts consisting of single-atomic Fe sites and FeC clusters encapsulated in nitrogen-doped carbon layers (FeSA-FeC/NC). The FeSA-FeC/NC electrocatalyst demonstrates outstanding ORR performance in alkaline electrolytes, achieving a high half-wave potential (E = 0.902 V), 4e ORR selectivity, and robust methanol tolerance. The exceptional ORR catalytic performance is credited to the relatively substantial specific surface area and the optimal arrangement of active sites, including atomically dispersed Fe-N sites and synergistic FeC clusters. In situ spectroelectrochemical characterization and theoretical calculations verify that FeC clusters disrupt the symmetric electronic structure of Fe-N, optimizing 3d orbitals of Fe centers, thereby accelerating O─O bond cleavage in *OOH to boost ORR activity. Furthermore, a zinc-air battery constructed with FeSA-FeC/NC demonstrates excellent potential in energy storage application, yielding a maximum power density of 151.3 mW cm and robust cycling durability surpassing that of commercial Pt/C catalysts. This study establishes a cost-effective route for producing metal-based carbon electrocatalysts with exceptional performance using environmentally friendly raw materials.
对于像金属空气电池这样的能量转换装置而言，设计基于过渡金属的氧还原反应（ORR）电催化剂，使其具有成本效益且高效，至关重要但也具有挑战性。在这项工作中，我们提出了一种具有成本效益的策略，用于制备由封装在氮掺杂碳层中的单原子铁位点和FeC簇组成的催化剂（FeSA-FeC/NC）。FeSA-FeC/NC电催化剂在碱性电解质中表现出出色的ORR性能，实现了高半波电位（E = 0.902 V）、4e ORR选择性和强大的甲醇耐受性。这种优异的ORR催化性能归因于相对较大的比表面积和活性位点的最佳排列，包括原子分散的Fe-N位点和协同作用的FeC簇。原位光谱电化学表征和理论计算证实，FeC簇破坏了Fe-N的对称电子结构，优化了Fe中心的3d轨道，从而加速了*OOH中O─O键的断裂，提高了ORR活性。此外，用FeSA-FeC/NC构建的锌空气电池在储能应用中表现出优异的潜力，产生的最大功率密度为151.3 mW cm，并且具有超过商业Pt/C催化剂的强大循环耐久性。这项研究建立了一条使用环保原料生产具有优异性能的金属基碳电催化剂的经济有效途径。
