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

被引:51
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
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
相关论文
共 62 条
[1]   Nitrogen-doped carbon nanotube spheres as metal-free catalysts for the partial oxidation of H2S [J].
Ba, Housseinou ;
Cuong Duong-Viet ;
Liu, Yuefeng ;
Nhut, Jean-Mario ;
Granger, Pascal ;
Ledoux, Marc J. ;
Cuong Pham-Huu .
COMPTES RENDUS CHIMIE, 2016, 19 (10) :1303-1309
[2]   XPS investigation of preferential sputtering of S from MoS2 and determination of MoSx stoichiometry from Mo and S peak positions [J].
Baker, MA ;
Gilmore, R ;
Lenardi, C ;
Gissler, W .
APPLIED SURFACE SCIENCE, 1999, 150 (1-4) :255-262
[3]   Enhanced visible-light photocatalytic activity of g-C3N4/TiO2 films [J].
Boonprakob, Natkritta ;
Wetchakun, Natda ;
Phanichphant, Sukon ;
Waxler, David ;
Sherrell, Peter ;
Nattestad, Andrew ;
Chen, Jun ;
Inceesungvorn, Burapat .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2014, 417 :402-409
[4]   Low temperature desulfurization on Co-doped α-FeOOH: Tailoring the phase composition and creating the defects [J].
Cao, Yanning ;
Shen, Lijuan ;
Hu, Xiaoli ;
Du, Zhongjie ;
Jiang, Lilong .
CHEMICAL ENGINEERING JOURNAL, 2016, 306 :124-130
[5]   Preparation and catalytic activity of active carbon-supported Mo2C nanoparticles [J].
Celzard, A ;
Marêché, JF ;
Furdin, G ;
Fierro, V ;
Sayag, C ;
Pielaszek, J .
GREEN CHEMISTRY, 2005, 7 (11) :784-792
[6]   Pomegranate-like N,P-Doped Mo2C@C Nanospheres as Highly Active Electrocatalysts for Alkaline Hydrogen Evolution [J].
Chen, Yu-Yun ;
Zhang, Yun ;
Jiang, Wen-Jie ;
Zhang, Xing ;
Dai, Zhihui ;
Wan, Li-Jun ;
Hu, Jin-Song .
ACS NANO, 2016, 10 (09) :8851-8860
[7]   N-doped defective carbon with trace Co for efficient rechargeable liquid electrolyte-/all-solid-state Zn-air batteries [J].
Chen, Zhiyan ;
Wang, Qichen ;
Zhang, Xiaobin ;
Lei, Yongpeng ;
Hu, Wei ;
Luo, Yao ;
Wang, Yaobing .
SCIENCE BULLETIN, 2018, 63 (09) :548-555
[8]   Nitrogen-Doped Carbon Nanotubes as a Highly Active Metal-Free Catalyst for Selective Oxidation [J].
Chizari, Kambiz ;
Deneuve, Adrien ;
Ersen, Ovidiu ;
Florea, Ileana ;
Liu, Yu ;
Edouard, David ;
Janowska, Izabela ;
Begin, Dominique ;
Cuong Pham-Huu .
CHEMSUSCHEM, 2012, 5 (01) :102-108
[9]   Metal-free activation of H2O2 by g-C3N4 under visible light irradiation for the degradation of organic pollutants [J].
Cui, Yanjuan ;
Ding, Zhengxin ;
Liu, Ping ;
Antonietti, Markus ;
Fu, Xianzhi ;
Wang, Xinchen .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2012, 14 (04) :1455-1462
[10]   Carbon nanotubes containing oxygenated decorating defects as metal-free catalyst for selective oxidation of H2S [J].
Cuong Duong-Viet ;
Liu, Yuefeng ;
Ba, Housseinou ;
Lai Truong-Phuoc ;
Baaziz, Walid ;
Lam Nguyen-Dinh ;
Nhut, Jean-Mario ;
Cuong Pham-Huu .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2016, 191 :29-41