Enhanced Selective H2S Oxidation Performance on Mo2C-Modified g-C3N4

被引:50
作者
Lei, Chunsheng [1 ,2 ]
Zhou, Wen [1 ,2 ]
Shen, Lijuan [3 ]
Zheng, Xiaohai [3 ]
Feng, Qingguo [4 ,5 ]
Liu, Yi [2 ]
Lei, Yongpeng [2 ]
Liang, Shijing [3 ]
Zhang, Dou [2 ]
Jiang, Lilong [3 ]
Zhou, Kechao [2 ]
机构
[1] Changzhou Univ, Coll Environm & Secur Engn, 1 Gehu Rd, Changzhou 213164, Jiangsu, Peoples R China
[2] Cent S Univ, State Key Lab Powder Met, 932 South Lushan Rd, Changsha 410083, Hunan, Peoples R China
[3] Fuzhou Univ, Natl Engn Res Ctr Chem Fertilizer Catalyst, 523 Gongye Rd, Fuzhou 350002, Fujian, Peoples R China
[4] Southwest Jiaotong Univ, Minist Educ, Key Lab Adv Technol Mat, 111 North 2nd Loop Rd, Chengdu 610031, Sichuan, Peoples R China
[5] Southwest Jiaotong Univ, Inst Mat Dynam, 111 North 2nd Loop Rd, Chengdu 610031, Sichuan, Peoples R China
来源
ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2019年 / 7卷 / 19期
基金
国家重点研发计划;
关键词
molybdenum carbide; graphitic carbon nitride; hydrogen sulfide; selective oxidative desulfurization; adsorption; METAL-FREE CATALYST; DOPED CARBON NANOTUBES; HYDROGEN-EVOLUTION; EFFICIENT CATALYSTS; HIGHLY EFFICIENT; NITRIDE; CARBIDE; MO2C; NANOSHEETS; COMPOSITE;
D O I
10.1021/acssuschemeng.9b03274
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Direct catalytic selective oxidation of H2S to sulfur at low temperature has been drawing attention. Molybdenum carbide (Mo2C), in which the excess occupied orbitals provide more back-donation chances for the adsorbents' g-orbitals, shows activity in electrocatalysis, photocatalysis, thermocatalysis, etc. that are comparable to those of noble metals. This work reports for the time the use of Mo2C and Mo2C-modified g-C3N4 for catalytic selective oxidative desulfurization. The density functional theory calculation indicates that Mo2C facilitates the adsorption of H2S molecule and the HS group. Furthermore, the Mo2C-modified g-C3N4 shows a sulfur yield of as high as 99.0% at 190 degrees C, much higher than that of g-C3N4 (46.0%). The good stability of the catalyst was demonstrated by X-ray diffraction, Fourier transform infrared spectra, and so on. Remarkably, the H2S conversion of the Mo2C-modified g-C3N4 remains constant (95.0%) at 190 degrees C for as long as 30 h. As a first demonstration using carbides in selective H2S oxidation, this work provides an opportunity to develop a novel class of potential catalysts.
引用
收藏
页码:16257 / 16263
页数:13
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