Citation: Zhi-Feng Jiao, Ji-Xiao Zhao, Xiao-Ning Guo, Xiang-Yun Guo. Photocatalytic C-X borylation of aryl halides by hierarchical SiC nanowire-supported Pd nanoparticles[J]. Chinese Journal of Catalysis, 2020, 41(2): 357-363. doi: S1872-2067(19)63449-2
具有分级结构的SiC纳米线负载的Pd纳米颗粒光催化芳基卤化物硼化反应
本文以具有分级结构且能够响应可见光的SiC纳米线为载体,并通过液相还原法制备负载量为3 wt%的Pd/SiC催化剂.TEM照片可以看出,Pd纳米颗粒均地分散在SiC表面,平均粒径为3.7nm.UV-Vis图谱表明,SiC负载Pd以后可明显提高其对可见光的吸收.Pd/SiC在可见光(400-800nm)照射下,在30℃和常压Ar氛围下即可实现碘苯脱碘硼化,苯硼酸频哪醇酯的收率高达95%.Pd/SiC在可见光作用下,对其它碘苯类和溴苯类化合物的光催化硼化均具有较好的的普适性.在暗反应条件下,苯硼酸频哪醇酯的收率仅为5%.并且,转化率能够随着光强度的增强而增加.同时,不同的波长范围对光反应的贡献率也不同,400-450,450-500,500-550,550-600和600-800nm的光反应贡献率分别为34%,22%,16%,13%和5%,这与催化剂的紫外可见吸收光谱相一致,充分说明反应主要为光驱动反应.Pd/SiC催化剂也具有较好的可重复使用性,经过5次循环使用后,催化活性依然保持在较高的水平.
光反应和暗反应活化能的显著差别,说明二者的机理不同.理论研究发现,SiC的功函为4.0eV,低于Pd (5.12eV),当Pd负载在SiC表面时,能够形成Mott-Schottky接触,使SiC吸收可见光生成的光生电子能够迅速的传递到Pd活性位.XPS表征显示,Pd在Pd/SiC催化剂中以金属态Pd0的形式存在,并向低结合能方向移动,说明SiC中的电子向Pd迁移,增加了Pd原子周围的电子云密度.同时,光致发光光谱中,Pd/SiC位于400-550nm的特征峰与SiC相比,强度明显减弱,说明光生电子和空穴的分离效率增强.据此我们推断,光生电子迅速从SiC传递到Pd使Pd活性位表面富电子化,进而快速活化和断裂芳基卤化物中的C-I或C-Br键,有效提高催化活性.
English
Photocatalytic C-X borylation of aryl halides by hierarchical SiC nanowire-supported Pd nanoparticles
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