Ändra sökning
RefereraExporteraLänk till posten
Permanent länk

Direktlänk
Referera
Referensformat
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Annat format
Fler format
Språk
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Annat språk
Fler språk
Utmatningsformat
  • html
  • text
  • asciidoc
  • rtf
CO2-philic poly(ionic liquid)-assisted local enrichment strategy for enhancedelectrochemical CO2 reduction
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).ORCID-id: 0000-0003-1016-5135
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
(Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
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..

Nyckelord [en]
electrochemical CO2 reduction, poly(ionic liquid), local environment, low-concentration CO2
Nationell ämneskategori
Materialkemi
Identifikatorer
URN: urn:nbn:se:su:diva-225779OAI: oai:DiVA.org:su-225779DiVA, id: diva2:1830226
Tillgänglig från: 2024-01-22 Skapad: 2024-01-22 Senast uppdaterad: 2024-02-26Bibliografiskt granskad
Ingår i avhandling
1. Multiscale interfacial engineering of heterogeneous electrocatalysts: From structural design to mechanistic study
Öppna denna publikation i ny flik eller fönster >>Multiscale interfacial engineering of heterogeneous electrocatalysts: From structural design to mechanistic study
2024 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
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.

Ort, förlag, år, upplaga, sidor
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University, 2024. s. 71
Nyckelord
heterogeneous electrocatalysis, electronic structure, coordination environment, single-atom catalysts, strain effect, hydrogen evolution reaction kinetics, charge transfer, electrochemical CO^2 reduction, local enrichment
Nationell ämneskategori
Materialkemi
Forskningsämne
materialkemi
Identifikatorer
urn:nbn:se:su:diva-225784 (URN)978-91-8014-647-0 (ISBN)978-91-8014-648-7 (ISBN)
Disputation
2024-03-06, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 13:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2024-02-12 Skapad: 2024-01-22 Senast uppdaterad: 2024-02-02Bibliografiskt granskad

Open Access i DiVA

Fulltext saknas i DiVA

Person

Zhou, ShiqiYuan, JiayinTahavori, Elnaz

Sök vidare i DiVA

Av författaren/redaktören
Zhou, ShiqiYuan, JiayinTahavori, Elnaz
Av organisationen
Institutionen för material- och miljökemi (MMK)
Materialkemi

Sök vidare utanför DiVA

GoogleGoogle Scholar

urn-nbn

Altmetricpoäng

urn-nbn
Totalt: 42 träffar
RefereraExporteraLänk till posten
Permanent länk

Direktlänk
Referera
Referensformat
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Annat format
Fler format
Språk
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Annat språk
Fler språk
Utmatningsformat
  • html
  • text
  • asciidoc
  • rtf