期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 46, 期 66, 页码 33107-33119出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2021.07.163
关键词
Mn dopants; Ni-based catalysts; Quaternary hydrotalcites; Carbon dioxide methanation
资金
- Chinese Scholarship Council (CSC)
- Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering [2019-KF-09]
- ICES (A-STAR, Singapore)
Mn-doped NiMgAl mixed-oxide catalysts showed enhanced catalytic performance, with NiMn5-LDO delivering the best results. Mn dopants tuned the interaction between Ni and Mg(Mn)AlOx support, promoting the reduction of NiO and achieving a higher surface basicity strength.
Mn-promoted NiMgAl mixed-oxide (NiMnx-LDO, x = 0, 5, 10, 15) catalysts derived from hydrotalcite were synthesized using co-precipitation for CO2 hydrogenation to synthetic natural gas. By regulating Mn contents, NiMn5-LDO delivered the most excellent catalytic performance, being about 2 times higher than that of undoped NiMn0-LDO catalyst (TOF of NiMn5-LDO and NiMn0-LDO: 0.61 s(-1) vs 0.31 s(-1) @ 240 degrees C). Through extensive characterization, it was found that Mn dopants promoted the reduction of bulk NiO through tuning the interaction between Ni and Mg(Mn)AlOx support. A high surface ratio of Ni-0/Ni2+ was achieved over NiMn5-LDO. Furthermore, the surface basicity strength was tailored by Mn dopants. With 5 wt% of Mn, NiMn5-LDO catalyst showed a stronger medium-strength basicity and higher capacity of CO2 adsorption than others. Particularly, TOF indicates a good correlation with medium-strength basicity over NiMnx-LDO catalysts. The strong metal-support interaction originated from the hydrotalcite structure kept nickel uniformly dispersed, endowing to the improved catalytic performance. (C) 2021 Published by Elsevier Ltd on behalf of Hydrogen Energy Publications LLC.
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