Non-Bonding Interaction of Neighboring Fe and Ni Single-Atom Pairs on MOF-Derived N-Doped Carbon for Enhanced CO 2 Electroreduction

作者：Long Jiao, Juntong Zhu, Yan Zhang, Weijie Yang, Siyuan Zhou, Aowen Li, Chenfan Xie, Xusheng Zheng, Wu Zhou, Shu‐Hong Yu, Hai‐Long Jiang · 发表于：Journal of the American Chemical Society · 年份：2021 · DOI：10.1021/jacs.1c08050 · 被引用次数：658 · 研究领域：CO2 Reduction Techniques and Catalysts、Electrocatalysts for Energy Conversion、Covalent Organic Framework Applications

Single-atom catalysts (SACs), featuring high atom utilization, have captured widespread interests in diverse applications. However, the single-atom sites in SACs are generally recognized as independent units and the interplay of adjacent sites is largely overlooked. Herein, by the direct pyrolysis of MOFs assembled with Fe and Ni-doped ZnO nanoparticles, a novel Fe 1 –Ni 1 –N–C catalyst, with neighboring Fe and Ni single-atom pairs decorated on nitrogen-doped carbon support, has been precisely constructed. Thanks to the synergism of neighboring Fe and Ni single-atom pairs, Fe 1 –Ni 1 –N–C presents significantly boosted performances for electrocatalytic reduction of CO 2, far surpassing Fe 1 –N–C and Ni 1 –N–C with separate Fe or Ni single atoms. Additionally, the Fe 1 –Ni 1 –N–C also exhibits superior performance with excellent CO selectivity and durability in Zn-CO 2 battery. Theoretical simulations reveal that, in Fe 1 –Ni 1 –N–C, single Fe atoms can be highly activated by adjacent single-atom Ni via non-bonding interaction, significantly facilitating the formation of COOH* intermediate and thereby accelerating the overall CO 2 reduction. This work supplies a general strategy to construct single-atom catalysts containing multiple metal species and reveals the vital importance of the communitive effect between adjacent single atoms toward improved catalysis.