纳米薄片组装的花状NiMoS催化剂制备及其加氢脱硫性能  

Preparation of Nanosheets-Assembled Flower-Like NiMoS Catalyst and Its Hydrodesulfurization Performance

作　　者：袁胜华 李唯楚 魏春金[3] 郑进保[2] 方维平[2] 伊晓东[2] 赖伟坤 YUAN Shenghua;LI Weichu;WEI Chunjin;ZHENG Jinbao;FANG Weiping;YI Xiaodong;LAI Weikun(SINOPEC(Dalian)Research Institute of Petroleum and Petrochemicals Co.,Ltd.,Dalian 116041,China;National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China;School of Science,Jimei University,Xiamen 361021,China)

机构地区：[1]中石化(大连)石油化工研究院有限公司,辽宁大连116041 [2]厦门大学化学化工学院醇醚酯化工清洁生产国家工程实验室,福建厦门361005 [3]集美大学理学院,福建厦门361021

出　　处：《石油学报（石油加工）》2023年第6期1349-1360,共12页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金项目(22172122,22072057,22172126,22172124);广西科技项目(AD17195067)资助。

摘　　要：为解决传统负载型NiMo催化剂活性位点少及加氢脱硫效率低的问题,采用简单水热硫化法制备了由纳米薄片组装的花状非负载型NiMoS催化剂,采用SEM、TEM和XRD等手段对催化剂结构与形貌进行表征,并考察不同反应条件下该催化剂的加氢脱硫反应性能。结果表明:NiMoS催化剂的花状结构由厚度约为6~12 nm的超薄纳米片组装而成,纳米薄片上MoS_(2)片层具有丰富的边缘活性位点;合成过程中,单质硫、水热时间和水热温度均影响NiMoS催化剂的纳米花状结构;在250℃、0.1 MPa氢气压力条件下,单质硫质量分数100%且在180℃水热硫化4 d所合成的花状NiMoS催化剂上噻吩的加氢脱硫转化率可达到100%,而在350℃、3.0 MPa氢气压力条件下,4,6-二甲基二苯并噻吩的加氢脱硫转化率可达到99.6%。该NiMoS纳米花非负载型催化剂的加氢脱硫反应性能优异,具有潜在的应用价值。To address the problems including few active sites and low hydrodesulfurization(HDS)activity of conventional supported NiMo catalysts,the flower-like unsupported NiMoS catalysts assembled from nanosheets were prepared using a simple hydrothermal sulfidation method,the catalyst structure and morphology were characterized by SEM,TEM and XRD,and the HDS performance of the catalysts was investigated under different reaction conditions.The results reveal that the flower-like structure of NiMoS catalyst consists of ultrathin nanosheets with a thickness of 6—12 nm,and MoS_(2) slabs on the nanosheets possess abundant edge sites.During the synthesis process,the elemental sulfur,hydrothermal temperature and time can affect the nanoflower-like structure of NiMoS catalysts.Under the conditions of 250℃and 0.1 MPa hydrogen pressure,the HDS conversion of thiophene can reach 100%over the NiMoS catalyst synthesized under the elemental sulfur mass fraction of 100%and hydrothermal sulfidation of 4 d at 180℃,while the conversion of 4,6-dimethyldibenzothiophene is 99.6%at 350℃under 3.0 MPa hydrogen pressure.The nanoflower NiMoS unsupported catalyst exhibits outstanding catalytic performance for HDS,and thus has potential application value.

关 键 词：NiMoS催化剂 水热硫化 纳米花 纳米薄片 噻吩 加氢脱硫 

分 类 号：TQ426.6[化学工程]