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Promotional effect of Cu and influence of surface NiCu alloy for enhanced H2 yields from CH4 decomposition over Cu modified Ni supported on MCM-41 catalyst Naresh Gutta, Vijay Kumar Velisoju, Anjaneyulu Chatla, Venu Boosa, James Tardio, Jim Patel, and Venugopal Akula Energy Fuels, Just Accepted Manuscript • DOI: 10.1021/acs.energyfuels.7b03363 • Publication Date (Web): 13 Feb 2018 Downloaded from http://pubs.acs.org on February 14, 2018
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Energy & Fuels
Optimized composition of 50wt%Ni-10wt%Cu supported on MCM-41 demonstrated highest H2 yields and the CH4 decomposition activities were correlated with surface Ni-Cu alloy. 242x79mm (96 x 96 DPI)
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Promotional effect of Cu and influence of surface Ni-Cu alloy for enhanced H2 yields from CH4 decomposition over Cu modified Ni supported on MCM-41 catalyst Naresh Gutta,1,2 Vijay Kumar Velisoju,1 Anjaneyulu Chatla,1 Venu Boosa,1 James Tardio,2 Jim Patel,3 and Venugopal Akula1,* 1
Catalysis Laboratory, Inorganic and Physical Chemistry Division, CSIR – Indian Institute of
Chemical Technology, Hyderabad-500 007, Telangana, India;
[email protected] 2
Centre for Advanced Materials & Industrial Chemistry (CAMIC), School of Sciences, RMIT
University, GPO BOX 2476, Melbourne – 3001, Australia 3
CSIRO Energy, 71 Normanby Rd, Clayton North, Victoria 3169, Australia.
Abstract Catalysts based on MCM-41 decorated with 35-70 nm diameter Ni particles was tested for the production of hydrogen by catalytic decomposition of methane (CDM). About 122 Nm3 (molNi)-1 hydrogen yield was achieved over a catalyst comprised of optimised Ni loading of 50 wt% Ni/MCM-41. The H2 yield increased dramatically to 204 Nm3 (molNi)-1, up on modification with 10 wt% Cu. Presence of Cu, in contact to Ni, appeared to reduce the sintering and coking of the active Ni sites, which enhanced the longevity of the catalyst. Raman analysis of the catalysts recovered after CDM experiments revealed that doping of Cu to Ni/MCM-41, enhanced the graphitic carbon deposition over the catalyst. All the samples (Ni and Ni-Cu modified MCM-41) were characterized by H2 chemisorption, SEM/TEM, XPS, XRD, H2-TPR, N2O titration and Raman spectroscopy to examine the bulk and surface properties of the catalysts.
Keywords: CH4, CDM, MCM-41, Ni-Cu alloy, pure H2, CNT
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1. Introduction Hydrogen is currently being considered as a large-scale carrier for renewable energy. However, H2 is principally produced from natural gas,1-5 and conventional CH4 reforming technologies must incorporate costly carbon capture and sequestration technologies (CCS) if COx (CO and CO2) emissions are to be minimised. One alternative to the oxy reforming of natural gas, that holds potential for low CO2 emissions and produces pure H2 suitable for fuel cell applications (
