Effect of sulfur–carbon interaction on sulfur poisoning of Ni/Al2O3 catalysts for hydrogenation. (9th March 2017)

• Record Type: Journal Article
• Authors: Feng, Junpeng; Liu, Jinjia; Tang, Mingxing; Zhou, Ligong; Zhang, Xiaoyin; Wen, Xiaodong; Ge, Hui; Li, Debao; Li, Xuekuan
• Is Part Of: International journal of hydrogen energy. Volume 42:Number 10(2017)
• Page Start: 6727
• Page End: 6737
• Publication Date: 2017-03-09
• Subjects: Hydrogenation -- Sulfur poisoning -- Ni catalyst -- Carbon–sulfur -- Dissociation; Hydrogen as fuel -- Periodicals; Hydrogène (Combustible) -- Périodiques; Hydrogen as fuel; Periodicals; 665.81
• DOI: 10.1016/j.ijhydene.2017.01.125
• Languages: English
• ISSNs: 0360-3199

Abstract

Abstract: The poisoning effects of two types of carbon-containing sulfides (CS2 and CH3 SSCH3 ) on Ni/Al2 O3 catalysts for the hydrogenation of benzene and cyclohexene were systematically investigated via experiments and DFT calculations. The toxicity of CH3 SSCH3 is two and three times greater than that of CS2 for the hydrogenation of cyclohexene and benzene, respectively. The characterization and DFT results reveal that CH3 SSCH3 dissociates easily during hydrogenation and releases CH4, allowing sulfur atoms to poison the Ni sites. However, the presence of CS2 in the hydrogenation step slows the decline in the catalytic performance, because of resistance to the direct dissociation of the strong CS bond of CS2 . The chemisorbed CS2 molecules and their incomplete dissociation weaken the strength of NiS bond and decrease the poisoning effect of sulfur. The poisoning processes of two sulfides are also discussed following a DFT study. This work opens up promising possibilities for the industrial study of S-poisoning resistance in supported Ni catalysts. Graphical abstract: Highlights: CH3 SSCH3 dissociates easily and releases CH4, allowing sulfur to poison Ni atoms. CS2 molecules can stably chemisorb on Ni surface and undergo part dissociation. CS interaction weakens NiS bond and decreases the S-poisoning effect on Ni sites.