期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 292, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120167
关键词
Nitrogenase-inspired; Metal-organic frameworks; Zr-Hf bimetallic clusters; Functional ligands; Photocatalytic nitrogen fixation
资金
- National Natural Science Foundation of China [21621004]
- Program of Introducing Talents of Discipline to Universities [BP0618007]
- Natural Science Foundation ofTianjin City [18JCYBJC21000]
Inspired by nitrogenase, a metal-organic framework (MOF) photocatalyst, U(Zr-Hf)-X, was designed with bimetallic Zr-Hf nodes and functional ligands for efficient nitrogen fixation under visible-light. The optimized photocatalyst showed a high nitrogen fixation rate under visible-light, demonstrating the potential for visible-light-driven nitrogen fixation catalysts through a rational design approach.
Inspired by nitrogenase, we designed a kind of metal-organic framework (MOF) photocatalysts, U(Zr-Hf)-X, composed of bimetallic Zr-Hf nodes and different functional ligands. In the Zr-Hf bimetallic cluster, the Zr species serves as the active site of nitrogen fixation, while the Hf species acts as electron buffer tank to optimize electron transfer and utilization. In the organic ligands, the light absorption and utilization of MOFs is improved via introducing target functional groups to efficiently generate electrons. Notably, the organic ligand containing two thiol groups (-SH) can extend the absorption edge to the visible region. The optimal U(0.5Hf)-2SH (metal nodes: 0.5Zr: 0.5Hf; linkers: TPA-2SH) photocatalyst exhibits nitrogen fixation rate up to 116.1 mu mol g-1 h-1 under visible-light, attributed to the ligand-to-metal-to-metal electron transfer (LMMET) pathway and Zr-based pi-backbonding mechanism. Our nitrogenase-inspired strategy establishes a novel paradigm for rational design of visible-light-driven nitrogen fixation catalysts.
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