Electronic Modulation of the Interaction between Fe Single Atoms and WO 2.72– x for Photocatalytic N 2 Reduction

作者：Biao Hu, Binghao Wang, Lang Chen, Zhangjun Bai, Wei Zhou, Jun‐Kang Guo, Sheng Shen, Ting‐Liang Xie, Chak‐Tong Au, Lilong Jiang, Shuang‐Feng Yin · 发表于：ACS Catalysis · 年份：2022 · DOI：10.1021/acscatal.2c03367 · 被引用次数：78 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Covalent Organic Framework Applications

In the design of photocatalysts for ammonia synthesis, the construction of effective nitrogen (N 2 ) adsorption and activation sites is critical. Herein, Fe single atoms were effectively fixed on the surfaces of WO 2.72– x nanowires. Electronic interactions between single Fe atoms and WO 2.72– x resulted in a d -band center shift toward the Fermi level and thus enhancement of N 2 bonding with the catalyst surface. The studies of differential charge density and electron localization reveal that there is enhanced electron transfer from Fe-SA/WO 2.72– x to the adsorbed N 2, signifying that Fe single atoms are active centers for N 2 activation. Benefiting from electronic interactions, the optimized catalyst shows a NH 4 + generation rate of 186.5 μmol g –1 h –1 during photocatalytic N 2 reduction.