Hierarchal Porous Graphene-Structured Electrocatalysts with Fe–N5 Active Sites Modified with Fe Clusters for Enhanced Performance Toward Oxygen Reduction Reaction
Hierarchal Porous Graphene-Structured Electrocatalysts with Fe–N5 Active Sites Modified with Fe Clusters for Enhanced Performance Toward Oxygen Reduction Reaction
复制标题
具有 Fe-N5 活性位点的分级多孔石墨烯结构电催化剂，经 Fe 团簇修饰，可增强氧还原反应的性能
DOI：
10.1021/acsami.2c10947
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Yao Wang
中科院分区：
文献类型：
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作者：
Liqiu Liu;Yifei Liao;Sizhe Yue;Chaoling Wu;Yungui Chen;Haijiao Xie;Yao Wang
活性中心周围的局部配位环境对M-N-C催化剂的本征活性有重要影响。本文分别以Fe3+-SCN-和NaHCO3为金属前驱体和造孔剂，成功地制备了具有Fe团簇修饰的Fe-N5活性中心的多孔石墨烯。各种表征技术和理论计算证实了伴随着Fe团簇的独特的Fe-N5构型和改善的ORR活性。得益于这些孔，成功地构建了质量和电子转移通道，使更多的活性中心可以访问，并促进了ORR过程。结果表明，所制备的催化剂具有良好的ORR活性，半波电位为0.89V，选择性相当，稳定性较好。此外，以该材料为正极催化剂的国产锌空气电池的最大功率密度为0.205 W/cm~2，显示了CsA-Fe-N-C催化剂替代贵重铂催化剂的潜力。
The local coordination environment around the active centers has a major impact on tuning the intrinsic activity of M–N–C catalysts. Herein, a porous graphene with Fe–N5active sites modified with Fe clusters is successfully fabricated by using Fe3+-SCN–and NaHCO3as the metal precursor and pore-forming agent, respectively. The unique Fe–N5configuration accompanying Fe clusters and the improved ORR activity are confirmed by various characterization techniques and theoretical calculations. Benefiting from the pores, mass and electron transfer channels are successfully constructed, making more active sites accessible and facilitating the ORR process. As a consequence, the as-prepared catalyst has an excellent ORR activity with a half-wave potential of 0.89 V, comparable selectivity, and superior stability. In addition, a homemade primary zinc–air battery using this material as the cathode catalyst has a maximum power density of 0.205 W/cm2, revealing the potential of the as-constructed CSA-Fe–N–C catalyst to replace precious Pt catalysts.