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
CO2-philic poly(ionic liquid)-assisted local enrichment strategy for enhancedelectrochemical CO2 reduction
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).ORCID iD: 0000-0003-1016-5135
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Electrochemical CO2 reduction reaction (ECO2RR) to produce valuable chemicals and fuels is a promising way to make use of excessive CO2 as one of the major green-house gases debatably responsible for climate change. The chemically inert feature of CO2 molecules makes the first-step elementary reaction with one electron reduction challenging in thermodynamics, leading to a high overpotential for this step and the overall ECO2RR as well. Herein, we reported the successful fabrication of CO2-philic PIL-modified Au model catalyst with enhanced ECO2RR performance by a local CO2 enrichment strategy. The modified gas diffusion electrode exhibited ~ 100% Faradaic efficiency for CO2-to-CO conversion (FECO) in a wide potential window of -0.2 ~ -1.0 V (versus reversible hydrogen electrode. RHE) with pure CO2 feeding, and notablymaintained the FECO > 90% even at a low CO2 concentration of 20 % vol..

Keywords [en]
electrochemical CO2 reduction, poly(ionic liquid), local environment, low-concentration CO2
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-225779OAI: oai:DiVA.org:su-225779DiVA, id: diva2:1830226
Available from: 2024-01-22 Created: 2024-01-22 Last updated: 2024-02-26Bibliographically approved
In thesis
1. Multiscale interfacial engineering of heterogeneous electrocatalysts: From structural design to mechanistic study
Open this publication in new window or tab >>Multiscale interfacial engineering of heterogeneous electrocatalysts: From structural design to mechanistic study
2024 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In a typical heterogeneous electrocatalytic reaction, for the given active sites, the electronic structure plays a determining role in electron transfer between the active sites and reactant molecules, which impacts the reaction efficiency. Besides the electronic properties of the electrocatalysts, the reaction interface at which the charge transfer occurs plays an important role in the reaction kinetics. Moreover, the accessibility of the active sites to the reactant molecules also affects the reaction efficiency. However, a well-balanced effective strategy for electronic structure optimization that improves not only the activity but also stability and cost-effectiveness is needed. Besides, a robust model specifically tailored to investigate the kinetics of the electrocatalytic reaction is required to exclude the interference of thermodynamic factors. A feasible characterization technique for probing the complex interfacial process is also required.

 

To address these remaining challenges in the three aspects above, this thesis proposed the strategies to optimize the electrocatalytic reaction processes as follows:

 

(1) Tuning the electronic structure of the active sites by engineering coordination environment and introducing strain effect. Specifically, Ni single atom was constructed to engineer the coordination environment, and the electrocatalytic performance with the tuned electronic structure was examined towards hydrazine oxidation reaction. The strain effect was created by introducing Cu single atom to BiOCl substrate, and the optimized electronic structure was investigated;

(2) Optimizing the interfacial HER kinetics targeted by proposing a specific Pt model catalyst with a channel-opening modifier. The interfacial water structure was studied by in situ surface-enhanced Raman technique, and the role of this promoting modifier was elucidated by ab initio molecular dynamic simulation;

(3) Improving the local concentration of CO2 for electrochemical CO2 reduction reaction with a poly(ionic liquid) modifier, with Au as the model catalyst and the targeted characterization techniques.

Place, publisher, year, edition, pages
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University, 2024. p. 71
Keywords
heterogeneous electrocatalysis, electronic structure, coordination environment, single-atom catalysts, strain effect, hydrogen evolution reaction kinetics, charge transfer, electrochemical CO^2 reduction, local enrichment
National Category
Materials Chemistry
Research subject
Materials Chemistry
Identifiers
urn:nbn:se:su:diva-225784 (URN)978-91-8014-647-0 (ISBN)978-91-8014-648-7 (ISBN)
Public defence
2024-03-06, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (English)
Opponent
Supervisors
Available from: 2024-02-12 Created: 2024-01-22 Last updated: 2024-02-02Bibliographically approved

Open Access in DiVA

No full text in DiVA

Authority records

Zhou, ShiqiYuan, JiayinTahavori, Elnaz

Search in DiVA

By author/editor
Zhou, ShiqiYuan, JiayinTahavori, Elnaz
By organisation
Department of Materials and Environmental Chemistry (MMK)
Materials Chemistry

Search outside of DiVA

GoogleGoogle Scholar

urn-nbn

Altmetric score

urn-nbn
Total: 31 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