摘要：Mesoporous MY-xGa zeolites exhibiting both crystallized pore walls and narrowly dispersed mesopores with different Ga content were successfully synthesized. The synthesized samples were characterized by XRD, N-2 adsorption desorption isotherms, SEM, TEM, XPS, FTIR, Si-29 MAS NMR, Ga-71 MAS NMR, and Py-FTIR methods. The results show that the synthesized samples exhibit unique open channel like mesopore systems and outstanding crystallite natures; no nonframework Ga species were observed over the MY-xGa series samples, and their acidic properties can be modulated by varying the Ga/Al ratio in the initial synthesis gel. The corresponding NiMo/HMY-xGa catalysts were prepared via the incipient wetness coimpregnation method; the morphologies of the sulfide catalysts were characterized by HRTEM, and the covalent states of the active metals were characterized by XPS. The catalytic activities of the investigated catalysts for the 4,6-DMDBT HDS reaction were assessed, and the collected products were analyzed by GC and GC-MS methods. The catalyst NiMo/HMY-0.5Ga showed the highest catalytic activity due to the synergistic effect of modulated acidic properties, excellent morphology, highest sulfidation degree, and proper proportion of NiMoS phase. More importantly, 4-MDBT, DBT, and BP were observed and identified as the products of the 4,6-DMDBT HDS reaction, designated as the demethylation pathway (DM) for the 4,6-DMDBT HDS reaction. Finally, a reaction network including DDS, HYD, ISO, and DM pathways for the 4,6-DMDBT HDS reaction over catalyst NiMo/HMY-0.5Ga was proposed.

关键字：mesoporous Y zeolites 4,6-DMDBT HDS NiMoS active phase catalytic activity HDS pathway

ISSN号：2155-5435

卷、期、页：卷: 7 期: 11 页: 7665-7679

发表日期：2017-11-01

期刊分区（SCI为中科院分区）：一区

收录情况：SCIE（科学引文索引网络版）,ESI（基本科学指标数据库）,EI（工程索引）

发表期刊名称：ACS CATALYSIS

通讯作者：周文武,刘美芳,张晴,丁思佳

第一作者：魏强,周亚松

论文类型：期刊论文

论文概要：周文武,刘美芳,张晴,魏强,丁思佳,周亚松，Synthesis of NiMo Catalysts Supported on Gallium-Containing Mesoporous Y Zeolites with Different Gallium Contents and Their High Activities in the Hydrodesulfurization of 4,6-Dimethyldibenzothiophene，ACS CATALYSIS，2017，卷: 7 期: 11 页: 7665-7679

论文题目：Synthesis of NiMo Catalysts Supported on Gallium-Containing Mesoporous Y Zeolites with Different Gallium Contents and Their High Activities in the Hydrodesulfurization of 4,6-Dimethyldibenzothiophene