Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-01-25 , DOI: 10.1016/j.apcatb.2020.118686
Hao Huang , Xu-Sheng Wang , Davin Philo , Fumihiko Ichihara , Hui Song , Yunxiang Li , Dan Li , Teng Qiu , Shengyao Wang , Jinhua Ye
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The fixation of atmospheric dinitrogen to ammonia is one of the most essential processes for sustaining life. Since the N≡N bond in dinitrogen is one of the strongest bonds in chemistry, it remains a grand challenge to develop efficient catalysts for fixation of N2 under ambient conditions. Herein we report for the first time on visible-light-assisted photocatalytic nitrogen fixation by metal organic framework material at room temperature and pressure. The Ti3+ species induced by electron transfer from ligand-to-metal charge transfer process provide active sites for N2 reduction. Furthermore, visible-light-assisted photocatalytic N2 fixation is achieved by ligands functionalization which extend the light harvesting of the MOF to visible region. The integration of Ti sites and amine-functionalized linkers in NH2-MIL-125 (Ti) shows the highest visible light photocatalysis efficiency in a rate of 12.3 μmol g-1 h-1. This Ti MOF system therefore shows a potential as a new design of combining light-harvesting and catalytic components in a single solid platform for green NH3 production.
中文翻译:
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走向可见光辅助的光催化固氮:具有功能性配体的钛金属有机骨架
大气中二氮固定为氨是维持生命的最重要过程之一。由于二氮中的N≡N键是化学中最强的键之一,因此开发在环境条件下固定N 2的高效催化剂仍然是一项艰巨的挑战。本文我们首次报道了在室温和压力下金属有机骨架材料对可见光辅助光催化固氮的作用。由配体到金属的电荷转移过程中的电子转移引起的Ti 3+物种为N 2还原提供了活性位点。此外,可见光辅助的光催化N 2固定是通过配体功能化实现的,该功能化将MOF的光捕获范围扩展到了可见区域。在NH 2 -MIL-125(Ti)中Ti位点和胺官能化连接基的整合显示出最高的可见光光催化效率,速率为12.3μmolg -1 h -1。因此,该Ti MOF系统显示了一种将光收集和催化成分结合在单个固态平台上以生产绿色NH 3的新设计的潜力。