Highly active Au/δ-MoC and Au/β-Mo2C catalysts for the low-temperature water gas shift reaction: effects of the carbide metal/carbon ratio on the catalyst performance

Posada-Pérez, Sergio; Gutiérrez, Ramón A.; Zuo, Zhijun; Ramírez, Pedro J.; Viñes, Francesc; Liu, Ping; Illas, Francesc; Rodriguez, José A.

doi:10.1039/C7CY00639J

Title: Highly active Au/δ-MoC and Au/β-Mo₂C catalysts for the low-temperature water gas shift reaction: effects of the carbide metal/carbon ratio on the catalyst performance

Journal Article · Mon May 08 00:00:00 EDT 2017 · Catalysis Science and Technology

DOI:https://doi.org/10.1039/C7CY00639J· OSTI ID:1425081

Posada-Pérez, Sergio ^[1]; Gutiérrez, Ramón A. ^[2]; Zuo, Zhijun ^[3]; Ramírez, Pedro J. ^[2];

^[1]; Liu, Ping ^[4];

^[1];

^[4]

Univ. of Barcelona (Spain). Dept. of Materials Science and Physical Chemistry. Inst. of Theoretical and Computational Chemistry
Central Univ. of Venezuela, Caracas (Venezuela)
Taiyuan Univ. of Technology (China). Key Lab. of Coal Science and Technology of Ministry of Education and Shanxi Province
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.

In this paper, the water gas shift (WGS) reaction catalyzed by orthorhombic β-Mo₂C and cubic δ-MoC surfaces with and without Au clusters supported thereon has been studied by means of a combination of sophisticated experiments and state-of-the-art computational modeling. Experiments evidence the importance of the metal/carbon ratio on the performance of these systems, where Au/δ-MoC is presented as a suitable catalyst for WGS at low temperatures owing to its high activity, selectivity (only CO₂ and H₂ are detected), and stability (oxycarbides are not observed). Periodic density functional theory-based calculations show that the supported Au clusters and the Au/δ-MoC interface do not take part directly in water dissociation but their presence is crucial to switch the reaction mechanism, drastically decreasing the effect of the reverse WGS reaction and favoring the WGS products desorption, thus leading to an increase in CO₂ and H₂ production. Finally, the present results clearly display the importance of the Mo/C ratio and the synergy with the admetal clusters in tuning the activity and selectivity of the carbide substrate.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States); Univ. of Barcelona (Spain); Taiyuan Univ. of Technology (China)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Ministry of Economy and Competitiveness (MINECO) (Spain); European Regional Development Fund (FEDER); Government of Catalonia; European Union (EU); National High Technology Research and Development Program of China

Grant/Contract Number:: SC0012704; CTQ2015-64618-R; CTQ2012-30751; RYC-2012-10129; 2014SGR97; XRQTC; 676580; 2013AA051201

OSTI ID:: 1425081

Report Number(s):: BNL-203250-2018-JAAM; TRN: US1802036

Journal Information:: Catalysis Science and Technology, Vol. 7, Issue 22; ISSN 2044-4753

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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