摘要：Extensive efforts have been devoting to remove sulfur from transportation fuels to protect the environment. Here we present the synthesis of highly efficient hydrodesulfurization (HDS) catalysts by loading Co/Mo sulfides on various carbon modified gamma-Al2O3 substrates. The synthetic strategy features facile sequential impregnation and pyrolysis process. The morphology, surface property, and pore structure of the catalysts were characterized by various techniques, and the catalytic performance were evaluated by a fixed-bed hydrodesulfurization unit. The optimized CoMo/NPC@gamma-Al2O3 showed superior dibenzothiophene (DBT) removal rates (99%) and kHDS value (5.12 x 10(-7) mol g(-1) s(-1)) than those of CoMo@gamma-Al2O3 at a relatively low temperature of 280 C, revealing the effective modulation of carbon backbone. This remarkable HDS activity originated from the high sulfidation degree as well as electron-rich Mo species, which was attributed to the electron donating effect by N, P co-doping in the carbon skeleton. In addition, after the carbon modification, the decreased acid sites in gamma-Al2O3 support and the electron-rich Mo sulfide resulted in a high selectivity of direct desulphurization (DDS) pathway over hydrogenation (HYD), leading to significant hydrogen energy economy. The density functional theory (DFT) calculations confirmed that the electron-donating effect of NPC enhanced the dispersion of Mo species and weakened the Mo-O/Mo-S bonds, creating more active sites. This work provides an effective strategy for rational design and synthesis of highly-efficient HDS catalysts in practical industrial application.

关键字：N, P co-doping; Electron transfer; Hydrodesulfurization; CoMoS catalyst

ISSN号：0016-2361

卷、期、页：卷: 322

发表日期：2022-08-15

影响因子：6.608900

期刊分区（SCI为中科院分区）：二区

收录情况：SCIE（科学引文索引网络版）

发表期刊名称：FUEL

通讯作者：张革,徐朱松,孙思远,许崇,马广

第一作者：杨帆,车赛,杨旺,魏强,李永峰

论文类型：期刊论文

论文概要：张革,杨帆,徐朱松,车赛,孙思远,许崇,马广,杨旺,魏强,李永峰，Electronic structure regulation of CoMoS catalysts by N, P co-doped carbon modification for effective hydrodesulfurization，FUEL，2022，卷: 322

论文题目：Electronic structure regulation of CoMoS catalysts by N, P co-doped carbon modification for effective hydrodesulfurization