دورية أكاديمية
Tuning the reactivity of carbon surfaces with oxygen-containing functional groups.
| العنوان: | Tuning the reactivity of carbon surfaces with oxygen-containing functional groups. |
|---|---|
| المؤلفون: | Zhou J; Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA.; Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA., Yang P; Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA.; Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA., Kots PA; Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA., Cohen M; Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA., Chen Y; Pacific Northwest National Laboratory, Richland, WA, 99352, USA., Quinn CM; Department of Chemistry and Biochemistry, University of Delaware, Newark, DE, 19716, USA., de Mello MD; Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA.; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA., Anibal Boscoboinik J; Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA.; Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, 11973, USA., Shaw WJ; Pacific Northwest National Laboratory, Richland, WA, 99352, USA., Caratzoulas S; Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA., Zheng W; Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA. weiqing@udel.edu., Vlachos DG; Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA. vlachos@udel.edu.; Catalysis Center for Energy Innovation, University of Delaware, Newark, DE, 19716, USA. vlachos@udel.edu. |
| المصدر: | Nature communications [Nat Commun] 2023 Apr 21; Vol. 14 (1), pp. 2293. Date of Electronic Publication: 2023 Apr 21. |
| نوع المنشور: | Journal Article |
| اللغة: | English |
| بيانات الدورية: | Publisher: Nature Pub. Group Country of Publication: England NLM ID: 101528555 Publication Model: Electronic Cited Medium: Internet ISSN: 2041-1723 (Electronic) Linking ISSN: 20411723 NLM ISO Abbreviation: Nat Commun Subsets: PubMed not MEDLINE; MEDLINE |
| أسماء مطبوعة: | Original Publication: [London] : Nature Pub. Group |
| مستخلص: | Oxygen-containing carbons are promising supports and metal-free catalysts for many reactions. However, distinguishing the role of various oxygen functional groups and quantifying and tuning each functionality is still difficult. Here we investigate the role of Brønsted acidic oxygen-containing functional groups by synthesizing a diverse library of materials. By combining acid-catalyzed elimination probe chemistry, comprehensive surface characterizations, 15 N isotopically labeled acetonitrile adsorption coupled with magic-angle spinning nuclear magnetic resonance, machine learning, and density-functional theory calculations, we demonstrate that phenolic is the main acid site in gas-phase chemistries and unexpectedly carboxylic groups are much less acidic than phenolic groups in the graphitized mesoporous carbon due to electron density delocalization induced by the aromatic rings of graphitic carbon. The methodology can identify acidic sites in oxygenated carbon materials in solid acid catalyst-driven chemistry. (© 2023. The Author(s).) |
| References: | Phys Chem Chem Phys. 2010 May 7;12(17):4351-9. (PMID: 20407706) J Colloid Interface Sci. 2022 Aug;619:377-387. (PMID: 35398768) Nanoscale. 2020 Nov 19;12(44):22768-22777. (PMID: 33174567) J Chem Phys. 2004 Feb 1;120(5):2105-9. (PMID: 15268348) Phys Rev B Condens Matter. 1995 Feb 15;51(7):4014-4022. (PMID: 9979237) J Phys Chem C Nanomater Interfaces. 2016 Dec 22;120(50):28533-28544. (PMID: 28479940) J Phys Chem Lett. 2021 Mar 11;12(9):2413-2422. (PMID: 33661009) J Am Chem Soc. 2008 Aug 6;130(31):10369-79. (PMID: 18613662) Chemistry. 2011 Oct 4;17(41):11467-77. (PMID: 21922575) J Am Chem Soc. 2022 Feb 23;144(7):3250-3258. (PMID: 35138841) Nat Chem. 2010 Dec;2(12):1015-24. (PMID: 21107364) J Chem Phys. 2010 Apr 21;132(15):154104. (PMID: 20423165) Chem Soc Rev. 2018 Nov 12;47(22):8349-8402. (PMID: 30226518) Nat Chem. 2009 Aug;1(5):403-8. (PMID: 21378895) Nat Commun. 2023 Apr 21;14(1):2293. (PMID: 37085515) Phys Rev B Condens Matter. 1996 Oct 15;54(16):11169-11186. (PMID: 9984901) Chem Soc Rev. 2018 Apr 23;47(8):2680-2721. (PMID: 29577123) |
| معلومات مُعتمدة: | P30 GM110758 United States GM NIGMS NIH HHS |
| تواريخ الأحداث: | Date Created: 20230421 Date Completed: 20230424 Latest Revision: 20230425 |
| رمز التحديث: | 20230428 |
| مُعرف محوري في PubMed: | PMC10121666 |
| DOI: | 10.1038/s41467-023-37962-3 |
| PMID: | 37085515 |
| قاعدة البيانات: | MEDLINE |
Find this article in full text from Springer Verlag. 
Full Text Finder | تدمد: | 2041-1723 |
|---|---|
| DOI: | 10.1038/s41467-023-37962-3 |