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Si-based photoelectrochemical carbon dioxide reduction for value-added chemicals

Research Project

Project/Area Number 22KF0387
Project/Area Number (Other) 22F22366 (2022)
Research Category

Grant-in-Aid for JSPS Fellows

Allocation TypeMulti-year Fund (2023)
Single-year Grants (2022)
Section外国
Review Section Basic Section 27030:Catalyst and resource chemical process-related
Research InstitutionNational Institute for Materials Science

Principal Investigator

押切 光丈  国立研究開発法人物質・材料研究機構, ナノアーキテクトニクス材料研究センター, 主幹研究員 (20354368)

Co-Investigator(Kenkyū-buntansha) LI SIJIE  国立研究開発法人物質・材料研究機構, ナノアーキテクトニクス材料研究センター, 外国人特別研究員
Project Period (FY) 2023-03-08 – 2025-03-31
Project Status Granted (Fiscal Year 2023)
Budget Amount *help
¥2,100,000 (Direct Cost: ¥2,100,000)
Fiscal Year 2024: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 2023: ¥700,000 (Direct Cost: ¥700,000)
Fiscal Year 2022: ¥400,000 (Direct Cost: ¥400,000)
Keywordsphotoelectrocatalysis / carbon dioxide reduction / silicon photocathode / photoanode / cocatalysts / surface and interface
Outline of Research at the Start

This project focus on the development of heterogeneous Si-based photocathodes (PC) for solar-driven CO2 reduction by surface/interface modification, and then assembly of photoelectrochemical (PEC) devices by coupling optimized Si-based PC and potential photoanode (PA) to complete the synergistic reaction of CO2 reduction and water oxidation to further prepare high-value chemicals.

Outline of Annual Research Achievements

In the past year, we developed a one-step method for liquid-phase in-situ growth of Ag nanoparticle cocatalysts on p-type planar Si semiconductors to fabricate photocathodes for photoelectrochemical (PEC) CO2 reduction. Directly using planar Si is beneficial to shortening the photoelectrode manufacturing process. Besides, this method can effectively control the size and distribution of the Ag nanoparticles through the Ag ion concentration and growth time. By regulating the structure and active sites of Ag cocatalysts supported on the planar Si substrates as photocathodes and evaluating their performance of reducing CO2 to syngas, the Faradaic efficiency for CO at the optimal Ag/Si photocathode is increased by 6.2 times at -0.4 V vs. RHE (reversible hydrogen electrode). This shows that the PEC CO2 reduction performance of Si-based photocathodes is closely associated with the structure and property of the cocatalyst.
Furthermore, we prepared porous nanostructured BiVO4 with n-type semiconductor properties as a potential photoanode to assist PEC CO2 reduction. In addition to analyzing the chemical composition and physical structural properties of the as-prepared BiVO4 semiconductor, we also proceed to deposit transition metal cocatalysts on the BiVO4 photoanode. By designing and optimizing the preparation parameters of the transition metal cocatalyst and the surface/interface construction between the cocatalyst and BiVO4, the photocurrent density of BiVO4 as a photoanode for water oxidation reaction has been significantly improved.

Current Status of Research Progress
Current Status of Research Progress

2: Research has progressed on the whole more than it was originally planned.

Reason

Based on the in-situ deposition and growth of Ag nanoparticles on Si under normal temperature and liquid phase conditions, we constructed a controllable Si-based photocathode for PEC CO2 reduction. By analyzing the PEC properties of Ag/Si photocathodes, it is found that the PEC CO2 reduction efficiency and selectivity are closely related to the Si surface modification and the interface structure of Si semiconductor/Ag cocatalyst. In the PEC CO2 reduction performance evaluation, the Ag/Si photocathode can increase the Faradaic efficiency for CO by 6.2 times under light irradiation. In addition, transition metal cocatalyst-modified BiVO4 photoanodes have also made progress, and the photocurrent density has been significantly improved in water oxidation performance tests. This shows that we have made smooth progress in the preparation of the Si-based photocathode and BiVO4 photoanode. It is believed that with the assistance of BiVO4 water oxidation photoanode, a Si-based photocathode can be manufactured to achieve efficient and operable PEC CO2 reduction.

Strategy for Future Research Activity

In the future, we will continue to explore the surface/interface engineering of p-type Si-based semiconductors to prepare PEC CO2 photocathodes. By matching n-type semiconductors with appropriate band structures to form p-n heterojunctions, we aim to further improve the selectivity and efficiency of CO2 reduction. In addition, we will continue to focus on the optimization of n-type BiVO4 photoanodes for water oxidation, focusing on further increasing photocurrent density and reducing onset potential. Ultimately, bias-free CO2 reduction will be constructed by combining high-performance p-type Si semiconductor photocathode and n-type BiVO4 semiconductor photoanode.

Report

(2 results)
  • 2023 Research-status Report
  • 2022 Annual Research Report
  • Research Products

    (2 results)

All 2022

All Journal Article (2 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 2 results)

  • [Journal Article] One-step construction of buried a-Si/c-Si junction photocathodes for boosting photoelectrochemical hydrogen production2022

    • Author(s)
      Sijie Li, Huiwen Lin, Gaoliang Yang, Xiaohui Ren, Shunqin Luo, Jinhua Ye
    • Journal Title

      Chemical Engineering Journal

      Volume: 455 Pages: 140898-140898

    • DOI

      10.1016/j.cej.2022.140898

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Surface/Interface Engineering of Si-Based Photocathodes for Efficient Hydrogen Evolution2022

    • Author(s)
      Sijie Li, Huiwen Lin, Shunqin Luo, Qi Wang, Jinhua Ye
    • Journal Title

      ACS Photonics

      Volume: 9 Issue: 12 Pages: 3786-3806

    • DOI

      10.1021/acsphotonics.2c00708

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Int'l Joint Research

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Published: 2022-11-17   Modified: 2024-12-25  

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