Dry Reforming of Ethane and Butane with CO2 over PtNi/CeO2 Bimetallic Catalysts

Yan, Binhang; Yang, Xiaofang; Yao, Siyu; Wan, Jie; Myint, MyatNoeZin; Gomez, Elaine; Xie, Zhenhua; Kattel, Shyam; Xu, Wenqian; Chen, Jingguang G.

doi:10.1021/acscatal.6b02176

Title: Dry Reforming of Ethane and Butane with CO₂ over PtNi/CeO₂ Bimetallic Catalysts

Journal Article · Wed Sep 21 00:00:00 EDT 2016 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.6b02176· OSTI ID:1342631

Yan, Binhang ^[1]; Yang, Xiaofang ^[2]; Yao, Siyu ^[2]; Wan, Jie ^[3]; Myint, MyatNoeZin ^[4]; Gomez, Elaine ^[4]; Xie, Zhenhua ^[4]; Kattel, Shyam ^[2]; Xu, Wenqian ^[2]; Chen, Jingguang G. ^[5]

Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Tsinghua Univ., Beijing (China). Dept. of Chemical Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
Tsinghua Univ., Beijing (China). College of Materials Science and Engineering
Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering

Dry reforming is a potential process to convert CO₂ and light alkanes into syngas (H₂ and CO), which can be subsequently transformed to chemicals and fuels. Here in this work, PtNi bimetallic catalysts have been investigated for dry reforming of ethane and butane using both model surfaces and supported powder catalysts. The PtNi bimetallic catalyst shows an improvement in both activity and stability as compared to the corresponding monometallic catalysts. The formation of PtNi alloy and the partial reduction of Ce⁴⁺ to Ce³⁺ under reaction conditions are demonstrated by in-situ Ambient Pressure X-ray Photoemission Spectroscopy (AP-XPS), X-ray Diffraction (XRD) and X-ray Absorption Fine Structure (XAFS) measurements. A Pt-rich bimetallic surface is revealed by Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) following CO adsorption. Combined in-situ experimental results and Density Functional Theory (DFT) calculations suggest that the Pt-rich PtNi bimetallic surface structure would weaken the binding of surface oxygenates/carbon species and reduce the activation energy for C-C bond scission, leading to an enhanced dry reforming activity.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; AC02-98CH10886; FG02-05ER15688; AC02-05CH11231

OSTI ID:: 1342631

Report Number(s):: BNL-113425-2017-JA; R&D Project: CO035; KC0302010; TRN: US1701623

Journal Information:: ACS Catalysis, Vol. 6, Issue 11; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 84 works

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Effect of Oxide Support on Catalytic Performance of FeNi‐based Catalysts for CO ₂ ‐assisted Oxidative Dehydrogenation of Ethane Yan, Binhang; Yao, Siyu; Chen, Jingguang G. ChemCatChem, Vol. 12, Issue 2 https://doi.org/10.1002/cctc.201901585	journal	November 2019
The effects of bimetallic interactions for CO ₂ ‐assisted oxidative dehydrogenation and dry reforming of propane Gomez, Elaine; Xie, Zhenhua; Chen, Jingguang G. AIChE Journal, Vol. 65, Issue 8 https://doi.org/10.1002/aic.16670	journal	June 2019
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Combining CO2 reduction with propane oxidative dehydrogenation over bimetallic catalysts Gomez, Elaine; Kattel, Shyam; Yan, Binhang Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03793-w	journal	April 2018
Active sites for tandem reactions of CO ₂ reduction and ethane dehydrogenation Yan, Binhang; Yao, Siyu; Kattel, Shyam Proceedings of the National Academy of Sciences, Vol. 115, Issue 33 https://doi.org/10.1073/pnas.1806950115	journal	July 2018
Net reduction of CO2 via its thermocatalytic and electrocatalytic transformation reactions in standard and hybrid processes Tackett, Brian M.; Gomez, Elaine; Chen, Jingguang G. Nature Catalysis, Vol. 2, Issue 5 https://doi.org/10.1038/s41929-019-0266-y	journal	April 2019
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
dry reforming
bimetallic catalyst
synthesis gas
ethane
butane
CO2

Title: Dry Reforming of Ethane and Butane with CO2 over PtNi/CeO2 Bimetallic Catalysts

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Title: Dry Reforming of Ethane and Butane with CO₂ over PtNi/CeO₂ Bimetallic Catalysts