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The High-Temperature Acidity Paradox of Oxidized Carbon: An in situ DRIFTS Study
Herold, Felix1,2; Oefner, Niklas1; Zakgeym, Dina3; Drochner, Alfons1; Qi, Wei4; Etzold, Bastian J. M.1
Corresponding AuthorEtzold, Bastian J. M.(bastian.etzold@tu-darmstadt.de)
2022-01-10
Source PublicationCHEMCATCHEM
ISSN1867-3880
Pages13
AbstractUntil now, oxygen functionalized carbon materials were not considered to exhibit significant acidity at high temperatures, since carboxylic acids, the most prominent acidic functionality, are prone to decarboxylation at temperatures exceeding 250 degrees C. Paradoxically, we could show that oxidized carbon materials can act as highly active high-temperature solid acid catalysts in the dehydration of methanol at 300 degrees C, showing an attractive selectivity to dimethyl ether (DME) of up to 92 % at a conversion of 47 %. Building on a tailor-made carbon model material, we developed a strategy to utilize in situ DRIFT spectroscopy for the analysis of carbon surface species under process conditions, which until now proofed to be highly challenging due to the high intrinsic absorbance of carbon. By correlating the catalytic behavior with a comprehensive in situ DRIFTS study and extensive post mortem analysis we could attribute the high-temperature acidity of oxidized carbons to the interaction of thermally stable carboxylic anhydrides and lactones with nucleophilic constituents of the reaction atmosphere e. g. methanol and H2O. Dynamic equilibria of surface oxides depending on reaction atmosphere and temperature were observed, and a methyl ester, formed by methanolysis of anhydrides and lactones, was identified as key intermediate for DME generation on oxidized carbon catalysts.
Keywordacid base catalysis carbon materials carbon surface chemistry heterogeneous catalysis in situ spectroscopy
Funding OrganizationDeutsche Bundesstiftung Umwelt (DBU) ; Career Bridging Grant from Technical University of Darmstadt ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) ; NSFC of China ; Natural Science Foundation of Liaoning Province of China ; Projekt DEAL
DOI10.1002/cctc.202101586
Indexed BySCI
Language英语
Funding ProjectDeutsche Bundesstiftung Umwelt (DBU) ; Career Bridging Grant from Technical University of Darmstadt ; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)[ET-101/13-1] ; NSFC of China[22072163] ; NSFC of China[21761132010] ; Natural Science Foundation of Liaoning Province of China[2020-YQ-02] ; Projekt DEAL
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000741472500001
PublisherWILEY-V C H VERLAG GMBH
Citation statistics
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/173738
Collection中国科学院金属研究所
Corresponding AuthorEtzold, Bastian J. M.
Affiliation1.Tech Univ Darmstadt, Ernst Berl Inst Tech & Makromolekulare Chem, Dept Chem, Alarich Weiss Str 8, D-64287 Darmstadt, Germany
2.Norwegian Univ Sci & Technol, Dept Chem Engn, Sem Saelandsvei 4, N-7491 Trondheim, Norway
3.Forschungszentrum Julich, Helmholtz Inst Erlangen Nurnberg Renewable Energy, Egerlandstr 3, D-91058 Erlangen, Germany
4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Wenhua Rd 72, Shenyang 110016, Peoples R China
Recommended Citation
GB/T 7714
Herold, Felix,Oefner, Niklas,Zakgeym, Dina,et al. The High-Temperature Acidity Paradox of Oxidized Carbon: An in situ DRIFTS Study[J]. CHEMCATCHEM,2022:13.
APA Herold, Felix,Oefner, Niklas,Zakgeym, Dina,Drochner, Alfons,Qi, Wei,&Etzold, Bastian J. M..(2022).The High-Temperature Acidity Paradox of Oxidized Carbon: An in situ DRIFTS Study.CHEMCATCHEM,13.
MLA Herold, Felix,et al."The High-Temperature Acidity Paradox of Oxidized Carbon: An in situ DRIFTS Study".CHEMCATCHEM (2022):13.
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