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dc.contributor.authorWang, Qing Nan
dc.contributor.authorWeng, Xue Fei
dc.contributor.authorZhou, Bai Chuan
dc.contributor.authorLv, Shao Pei
dc.contributor.authorMiao, Shu
dc.contributor.authorZhang, Daliang
dc.contributor.authorHan, Yu
dc.contributor.authorScott, Susannah L.
dc.contributor.authorSchüth, Ferdi
dc.contributor.authorLu, An Hui
dc.date.accessioned2019-09-11T13:38:00Z
dc.date.available2019-09-11T13:38:00Z
dc.date.issued2019-07-02
dc.identifier.citationWang, Q.-N., Weng, X.-F., Zhou, B.-C., Lv, S.-P., Miao, S., Zhang, D., … Lu, A.-H. (2019). Direct, Selective Production of Aromatic Alcohols from Ethanol Using a Tailored Bifunctional Cobalt–Hydroxyapatite Catalyst. ACS Catalysis, 9(8), 7204–7216. doi:10.1021/acscatal.9b02566
dc.identifier.doi10.1021/acscatal.9b02566
dc.identifier.urihttp://hdl.handle.net/10754/656733
dc.description.abstractAromatic alcohols are essential components of many solvents, coatings, plasticizers, fine chemicals, and pharmaceuticals. Traditional manufacturing processes involving the oxidation of petroleum-derived aromatic hydrocarbons suffer from low selectivity due to facile overoxidation reactions which produce aromatic aldehydes, acids, and esters. Here we report a Co-containing hydroxyapatite (HAP) catalyst that converts ethanol directly to methylbenzyl alcohols (MB-OH, predominantly 2-MB-OH) at 325 °C. The dehydrogenation of ethanol to acetaldehyde, which is catalyzed by Co2+, has the highest reaction barrier. Acetaldehyde undergoes rapid, HAP-catalyzed condensation and forms the key intermediate, 2-butenal, which yields aromatic aldehydes through self-condensation and then MB-OH via hydrogenation. In the presence of Co2+, 2-butenal is selectively hydrogenated to 2-butenol. This reaction does not hinder aromatization because cross-coupling between 2-butenal and 2-butenol leads directly to MB-OH without passing through MBâ•O. Using these insights a dual-bed catalyst configuration was designed for use in a single reactor to improve the aromatic alcohol selectivity. Its successful use supports the proposed reaction mechanism.
dc.description.sponsorshipWe thank Prof. Mingshu Chen and Dr. Ding Ding (Xiamen University, China) for their assistance with XPS, LEIS, and CO-FTIR measurements. This work was supported by a Joint Sino-German Research Project (21761132011), the State Key Program of the National Natural Science Foundation of China (21733002), and the Cheung Kong Scholars Program of China (T2015036).
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttp://pubs.acs.org/doi/10.1021/acscatal.9b02566
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/10.1021/acscatal.9b02566.
dc.subjectethanol
dc.subjectaromatic alcohols
dc.subjectcobalt−hydroxyapatite
dc.subjectdehydrogenation
dc.subjectdehydrocyclization
dc.titleDirect, Selective Production of Aromatic Alcohols from Ethanol Using a Tailored Bifunctional Cobalt-Hydroxyapatite Catalyst
dc.typeArticle
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Center
dc.contributor.departmentChemical Science Program
dc.contributor.departmentElectron Microscopy
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratory
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalACS Catalysis
dc.rights.embargodate2020-08-02
dc.eprint.versionPost-print
dc.contributor.institutionState Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, People's Republic of China
dc.contributor.institutionDalian National Laboratory of Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, People's Republic of China
dc.contributor.institutionDepartment of Chemical Engineering, University of California, Santa Barbara, California 93106, United States
dc.contributor.institutionMax-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, D-45470 Mülheim an der Ruhr, Germany
kaust.personZhang, Daliang
kaust.personHan, Yu
dc.date.published-online2019-07-02
dc.date.published-print2019-08-02


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