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dc.contributor.authorLi, Jing
dc.contributor.authorZhou, Yanan
dc.contributor.authorXiao, Xin
dc.contributor.authorWang, Wei
dc.contributor.authorWang, Ning
dc.contributor.authorQian, Weizhong
dc.contributor.authorChu, Wei
dc.date.accessioned2018-11-12T11:49:46Z
dc.date.available2018-11-12T11:49:46Z
dc.date.issued2018-11-06
dc.identifier.citationLi J, Zhou Y, Xiao X, Wang W, Wang N, et al. (2018) Regulation of Ni-CNT Interaction on Mn Promoted Nickel Nanocatalysts Supported on Oxygenated CNTs for CO2 Selective Hydrogenation. ACS Applied Materials & Interfaces. Available: http://dx.doi.org/10.1021/acsami.8b04220.
dc.identifier.issn1944-8244
dc.identifier.issn1944-8252
dc.identifier.doi10.1021/acsami.8b04220
dc.identifier.urihttp://hdl.handle.net/10754/629857
dc.description.abstractMn promoted Ni nanoparticles (NPs) supported on oxygen-functionalized carbon nanotubes (CNTs) was synthesized for CO2 hydrogenation to methane. This novel metal-carbon catalytic system was characterized by both experimental and computational studies. An anomalous metal-support interaction mode (i.e. a higher temperature would lead to a weakened Ni-CNT interaction) was observed. Deep investigation confirmed that surface oxygen groups (SOGs) on CNTs played a key role in tuning the Ni-CNT interaction. We proposed that high calcination temperature would firstly lead to the decomposition of SOGs (> 400 oC), then causing a loss of anchoring sites and the anchoring effect of SOGs on Ni NPs, thus cutting off the connection between interfacial Ni atoms and CNT body, so resulting in the migration and coalescence of fine flat Ni NPs into larger sphere ones at 550 oC (geometric effect). Density functional calculation (DFT) study clarified this kind of anchoring effect stemmed from the formation of covalent bonding between interfacial Ni atom and C or O elements of SOGs, causing electrons transferred from Ni atoms to CNT support because of the intrinsic electronegativity of -COOH (electronic effect). Besides, Mn promotion notably boost the activity compared with unpromoted catalysts, which was irrelevant with the size effect but the enhanced CO2 adsorption and conversion according to the result of CO2-TPD and transient response experiment. The optimized NiMn350 catalyst endowed with Mn promotion and robust Ni-CNT interaction, showed both high activity and sintering resistance more than 140-hour. Our findings paved the way to reasonably design the metal-carbon catalyst with both high activity and stability.
dc.description.sponsorshipThis work was supported by the National Natural Science Foundation of China (21506111, 21476145); The National project of 2016YFA0200102 and the Beijing key project of Z161100002116012. We thank Dr. Z. L. Guo, and Dr. J. Deng for their useful discussion and helps.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/acsami.8b04220
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acsami.8b04220.
dc.subjectMetal-support interaction
dc.subjectMn promoter
dc.subjectCO2 hydrogenation
dc.subjectCarbon nanotube
dc.subjectmethanation
dc.titleRegulation of Ni-CNT Interaction on Mn Promoted Nickel Nanocatalysts Supported on Oxygenated CNTs for CO2 Selective Hydrogenation
dc.typeArticle
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalACS Applied Materials & Interfaces
dc.eprint.versionPost-print
dc.contributor.institutionBeijing Key Laboratory of Green Chemical Reaction Engineering and Technology, \nDepartment of Chemical Engineering, Tsinghua University, Beijing 100084, China
dc.contributor.institutionDepartment of Chemical Engineering, Sichuan University, pChengdu 610065, China
dc.contributor.institutionICPEES, UMR 7515 CNRS-University of Strasbourg (UdS), 25, rue Becquerel, 67087 Strasbourg Cedex 02, France
kaust.personWang, Ning
refterms.dateFOA2018-11-12T12:07:05Z
dc.date.published-online2018-11-06
dc.date.published-print2018-12-05


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