State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, School of Chemistry and Chemical Engineering, Ningxia University, Yinchuan, Ningxia 750021, China.
State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, School of Chemistry and Chemical Engineering, Ningxia University, Yinchuan, Ningxia 750021, China.
J Colloid Interface Sci. 2023 Sep 15;646:547-554. doi: 10.1016/j.jcis.2023.05.069. Epub 2023 May 15.
The polyoxometalates (POMs) have been shown to be highly effective as reactive sites for photocatalytic nitrogen fixation reactions. However, the effect of POMs regulation on catalytic performance has not been reported yet. Herein, a series of composites (SiWM@MIL-101(Cr) (M = Fe, Co, V, Mo) and D-SiWMo@MIL-101(Cr), D, Disordered) were obtained by regulating transition metal compositions and arrangement in the POMs. The ammonia production rate of SiWMo@MIL-101(Cr) is much higher than that of other composites, reaching 185.67 μmol·h·g in N without sacrificial agents. The structural characterization of composites reveals that the increase of the electron cloud density of W atom in composites is the key to improve the photocatalytic performance. In this paper, the microchemical environment of POMs was regulated by transition metal doping method, thereby promoting the efficiency of photocatalytic ammonia synthesis for the composites, which provides new insights into the design of POM-based photocatalysts with high catalytic activity.
多金属氧酸盐（POMs）已被证明是高效的光催化固氮反应反应活性位。然而，目前尚未有关于 POMs 调节对催化性能影响的报道。在此，通过调节 POMs 中过渡金属组成和排列，得到了一系列复合材料（SiWM@MIL-101(Cr)（M=Fe、Co、V、Mo）和 D-SiWMo@MIL-101(Cr)、D、无序）。SiWMo@MIL-101(Cr) 的氨生成速率远高于其他复合材料，在没有牺牲剂的情况下达到 185.67μmol·h·g。复合材料的结构表征表明，复合材料中 W 原子的电子云密度增加是提高光催化性能的关键。本文通过过渡金属掺杂方法调节 POMs 的微化学环境，从而提高了复合材料的光催化氨合成效率，为设计具有高催化活性的基于 POM 的光催化剂提供了新的思路。
