Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Electrochemical Denitrification and Oxidative Dehydrogenation of Ethylbenzene over N-doped Mesoporous Carbon: Atomic Level Understanding of Catalytic Activity by N-15 NMR Spectroscopy
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Show others and affiliations
Number of Authors: 102020 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 32, no 17, p. 7263-7273Article in journal (Refereed) Published
Abstract [en]

Spherical mesoporous carbon (with a particle size in the range of 40−75 μm) was synthesized by nanoreplication of a hard silica template using sucrose as the carbon precursor. The mesoporous carbon with BET surface areas higher than 1200 m2/g was doped with N by a treatment in an aqueous solution of nitric acid and/or in a flow of gaseous ammonia. The highest N content (3.2 wt % of N in bulk) was obtained when both modification methods were combined. Complementary physicochemical characterization techniques, including scanning electron microscopy (SEM), low-temperature N2 adsorption, powder X-ray diffraction (XRD), and Raman spectroscopy revealed the morphology, structure, and textural properties of the synthesized N-loaded carbon materials. For the identification of the detailed chemical structure on the surface of the carbons, 1H, 13C, and 15N solid-state nuclear magnetic resonance (NMR) measurements were performed, and the data were supported by chemical shift calculations with accurate quantum chemistry methods and X-ray photoelectron spectroscopic (XPS) analyses. All NMR experiments were performed at natural isotope abundance. The verified experimental data clearly showed that after the introduction of the N-containing moieties by the combined methods of treatment, a high concentration of pyridinic N at the edge, and pyrrolic N being external to the edge, was achieved for the mesoporous carbon. The distributed N surface species promoted the catalytic activity in the oxidative dehydrogenation of ethylbenzene to styrene but did not significantly influence the efficiency of the carbon materials in the electrochemical reduction of nitrate ions.

Place, publisher, year, edition, pages
2020. Vol. 32, no 17, p. 7263-7273
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:su:diva-186423DOI: 10.1021/acs.chemmater.0c01666ISI: 000569075300016OAI: oai:DiVA.org:su-186423DiVA, id: diva2:1492961
Available from: 2020-11-04 Created: 2020-11-04 Last updated: 2023-01-19Bibliographically approved
In thesis
1. Biomass-derived nanoscopic catalysts for water treatment: Structure-property relationship investigation
Open this publication in new window or tab >>Biomass-derived nanoscopic catalysts for water treatment: Structure-property relationship investigation
2023 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Green Chemistry has received widespread interest due to its capacity to meet environmental and economic objectives. The Twelve Principles were proposed to better perform Green Chemistry and have become the guideline for solving many environmental issues. Water contamination has become a major global challenge in the 21st century. Millions of people die from diseases caused by drinking contaminated water. Nitrate, metal ions and dye are the most frequent contaminants. Nitrate in drinking water, after ingestion, is reduced to nitrite by the gastrointestinal tract and threatens human health. Dye-polluted water is usually nonbiodegradable and poisonous: the main criticism is that it is harmful to human health and hampers the photosynthesis rate of aquatic life. Metal ions generally lead to biological and physiological complications when they bind to cellular macromolecules. Therefore, efficient and eco-friendly purification technology is pressing to provide solutions for water purification. 

This thesis is set out to investigate the electro-/photo- catalytical water purification techniques using different catalysts. Efficient nitrate electrochemical reduction was achieved by using NDC materials, and the active sites were determined with the help of a comprehensive solid-state NMR supported by theoretical calculation and DFT calculations. Furthermore, the photochemical dye degradation was performed using cellulose-based hybrid bio-inorganic catalysts. The intentional maintenance of the surface functional groups on cellulose-based materials can promote dye degradation performance and, most importantly, achieve simultaneous removal of heavy metal ions aside from photo dye degradation. Additionally, this thesis proposed two possible synthesis strategies to obtain electro-/photo- catalysts using cellulose-based materials as renewable resources. The Twelve Principles of Green Chemistry guided the optimization of the synthesis route and raw material selectivity. Notably, the low-temperature synthesis of hybrid photocatalysts maintained the surface functional groups and preserved the kinetic mechanism of contaminants' adsorption on bio-substrate.  This research is likely to contribute to a deeper understanding of renewable materials with green synthesis methods for catalysts targeting water contamination treatment.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm University, 2023. p. 70
Keywords
green chemistry, water purification, electrochemistry, photochemistry, biomass material, structure-property relationship
National Category
Inorganic Chemistry
Research subject
Inorganic Chemistry
Identifiers
urn:nbn:se:su:diva-213988 (URN)978-91-8014-168-0 (ISBN)978-91-8014-169-7 (ISBN)
Public defence
2023-03-31, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B Stockholm and digitally via Zoom, public link is available at the department website, Stockholm, 09:00 (English)
Opponent
Supervisors
Available from: 2023-03-08 Created: 2023-01-19 Last updated: 2023-04-05Bibliographically approved

Open Access in DiVA

No full text in DiVA

Other links

Publisher's full text

Authority records

Chen, JianhongJaworski, AleksanderAleksis, RihardsPell, Andrew J.Hedin, NiklasSlabon, Adam

Search in DiVA

By author/editor
Chen, JianhongJaworski, AleksanderAleksis, RihardsPell, Andrew J.Hedin, NiklasSlabon, Adam
By organisation
Department of Materials and Environmental Chemistry (MMK)
In the same journal
Chemistry of Materials
Chemical Sciences

Search outside of DiVA

GoogleGoogle Scholar

doi
urn-nbn

Altmetric score

doi
urn-nbn
Total: 41 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf