Tailoring supported palladium sulfide catalysts through H2-assisted sulfidation with H2S
作者:Wei Xu、Jun Ni、Qunfeng Zhang、Feng Feng、Yizhi Xiang、Xiaonian Li
DOI:10.1039/c3ta12277h
日期:——
Supported palladium sulfide catalysts are of great interest in selective hydrogenation reactions. In this work, “Pd4S”, “Pd3S”, “Pd16S7” and “PdS” supported on activated carbon were selectively synthesized by tailoring the H2-assisted sulfidation of Pd/C with H2S at 150–750 °C, and were characterized by means of XRD, XPS, TEM, HRTEM, EDS, BET and H2-TPR techniques. The results indicated that the sulfidation atmosphere, the sulfidation temperature and the metal–support interaction all played important roles in determining the crystal structure and composition of the PdxSy/C catalysts, which in turn gave different catalytic performances in the synthesis of N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine (6PPD) by the reductive N-alkylation of aromatic amines. PdS/C showed the highest selectivity (>97%) and stability among all the PdxSy/C catalysts.
负载型硫化钯催化剂在选择性加氢反应中具有重要意义。在这项工作中,通过在150-750℃下用H2S对Pd/C进行H2辅助硫化,选择性地合成了负载在活性炭上的“Pd4S”、“Pd3S”、“Pd16S7”和“PdS”,其特征在于:采用 XRD、XPS、TEM、HRTEM、EDS、BET 和 H2-TPR 技术。结果表明,硫化气氛、硫化温度和金属-载体相互作用都对PdxSy/C催化剂的晶体结构和组成起重要作用,从而在N-(1通过芳香胺的还原性 N-烷基化得到 ,3-二甲基丁基)-N'-苯基-对苯二胺 (6PPD)。在所有 PdxSy/C 催化剂中,PdS/C 显示出最高的选择性(>97%)和稳定性。