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Singly Dispersed Copper Atoms with Compressive Residual Strain for Superior Photocatalytic Diluted 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
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Solar-driven diluted CO2 reduction is an alternative way to realize carbon neutrality, although promoting the photo-reactivity and selectivity in low CO2 contents remains a great challenge. Herein, an atomically dispersed Cu catalyst in a compressive strained BiOCl substrate (Cu1-BOC-CRS) is identified as a promising photocatalyst for diluted CO2 reduction reaction, capable of producing CO without any sacrificial agents or sensitizers. The single Cu atoms and the local surface strain facilitate CO2 adsorption, resulting in impressive CO formation rates of 122 and 99 μmol g-1 h-1 respectively under pure and diluted CO2 conditions. Experimental investigations revealed that the occupation of single Cu atoms in the BiOCl extends the light absorbance and charge transfer, which in turn integrates the surface CO2 capture and conversion. Moreover, the compressive strain provides an extra low-energy route towards CO2-to-CO conversion, offering valuable insights for the future design of highly efficient photocatalysts for diluted CO2 reduction.

Keywords [en]
Single atomic Cu, Strain, Diluted CO2 reduction, Photocatalysis, Energy conversion
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:su:diva-225775OAI: oai:DiVA.org:su-225775DiVA, id: diva2:1830224
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

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Zhou, ShiqiYuan, Jiayin

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