TY - JOUR
T1 - Monometallic Carbonyl-Derived CeO 2 -Supported Rh and Co Bicomponent Catalysts for CO-Free, High-Yield H 2 Generation from Low-Temperature Ethanol Steam Reforming
AU - Huang, Lin
AU - Choong, Catherine
AU - Chen, Luwei
AU - Wang, Zhan
AU - Zhong, Ziyi
AU - Campos-Cuerva, Carlos
AU - Lin, Jianyi
PY - 2013/1
Y1 - 2013/1
N2 - CeO 2 -supported Rh and Co bicomponent catalysts derived from monometallic carbonyls and prepared from metal nitrates for low-temperature ethanol steam reforming (ESR) have been studied by catalytic testing using a multi-channel reactor, temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), H 2 chemisorption, transmission electron microscopy-energy dispersive X-ray analysis (TEM-EDX), powder X-ray diffraction (PXRD) and IR spectroscopy. Reaction product analysis shows that low-temperature ESR proceeds mainly through 1)adsorbed oxametallacycle decarbonylation (OD) and acetaldehyde steam reforming (ASR) on Rh/CeO 2 , 2)ethanol dehydrogenation to acetaldehyde, ASR, and water-gas shift (WGS) on Co/CeO 2 , and 3)OD, ASR, and WGS on (Rh+Co)/CeO 2 . The addition of Co to Rh/CeO 2 results in decreased catalytic selectivity towards CO and CH 4 . The carbonyl-derived (Rh+Co)/CeO 2 displays marked advantage over the nitrate-prepared catalyst, leading to CO-free H 2 generation with H 2 yields as high as 4.3molH2molC2H5OH -1 at temperatures as low as 300°C. Combined studies by TPR, XPS, H 2 chemisorption, and TEM-EDX suggest significant interaction between the Rh and Co atoms in carbonyl-derived (Rh+Co)/CeO 2 , in contrast to nitrate-prepared catalysts, which is assumed to promote efficient WGS during the ESR process. Catalyst deactivation, possibly as a result of catalyst sintering, metal oxidation, and coke deposition during ESR, is discussed in terms of TPR, XPS, TGA, TEM, and PXRD. A WGS-ESR bilayered catalyst system of Rh/CeO 2 -(Rh+Co)/CeO 2 is successfully applied to the CO-free and high-yield production of H 2 from low-temperature ESR.
AB - CeO 2 -supported Rh and Co bicomponent catalysts derived from monometallic carbonyls and prepared from metal nitrates for low-temperature ethanol steam reforming (ESR) have been studied by catalytic testing using a multi-channel reactor, temperature-programmed reduction (TPR), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), H 2 chemisorption, transmission electron microscopy-energy dispersive X-ray analysis (TEM-EDX), powder X-ray diffraction (PXRD) and IR spectroscopy. Reaction product analysis shows that low-temperature ESR proceeds mainly through 1)adsorbed oxametallacycle decarbonylation (OD) and acetaldehyde steam reforming (ASR) on Rh/CeO 2 , 2)ethanol dehydrogenation to acetaldehyde, ASR, and water-gas shift (WGS) on Co/CeO 2 , and 3)OD, ASR, and WGS on (Rh+Co)/CeO 2 . The addition of Co to Rh/CeO 2 results in decreased catalytic selectivity towards CO and CH 4 . The carbonyl-derived (Rh+Co)/CeO 2 displays marked advantage over the nitrate-prepared catalyst, leading to CO-free H 2 generation with H 2 yields as high as 4.3molH2molC2H5OH -1 at temperatures as low as 300°C. Combined studies by TPR, XPS, H 2 chemisorption, and TEM-EDX suggest significant interaction between the Rh and Co atoms in carbonyl-derived (Rh+Co)/CeO 2 , in contrast to nitrate-prepared catalysts, which is assumed to promote efficient WGS during the ESR process. Catalyst deactivation, possibly as a result of catalyst sintering, metal oxidation, and coke deposition during ESR, is discussed in terms of TPR, XPS, TGA, TEM, and PXRD. A WGS-ESR bilayered catalyst system of Rh/CeO 2 -(Rh+Co)/CeO 2 is successfully applied to the CO-free and high-yield production of H 2 from low-temperature ESR.
KW - Cerium
KW - Cobalt
KW - Rhodium
KW - Supported catalysts
UR - http://www.scopus.com/inward/record.url?scp=84871641096&partnerID=8YFLogxK
U2 - 10.1002/cctc.201200452
DO - 10.1002/cctc.201200452
M3 - 文章
AN - SCOPUS:84871641096
SN - 1867-3880
VL - 5
SP - 220
EP - 234
JO - ChemCatChem
JF - ChemCatChem
IS - 1
ER -