2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO 2 Reduction

Yang, Sizhuo; Hu, Wenhui; Zhang, Xin; He, Peilei; Pattengale, Brian; Liu, Cunming; Cendejas, Melissa; Hermans, Ive; Zhang, Xiaoyi; Zhang, Jian; Huang, Jier

doi:10.1021/jacs.8b09705

Title: 2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO ₂ Reduction

Abstract

Covalent organic framework (COF) represents an emerging class of porous materials that have exhibited great potential in various applications, particularly in catalysis. Here, we report a newly designed 2D COF with incorporated Re complex, which exhibits intrinsic light absorption and charge separation (CS) properties. We show that this hybrid catalyst can efficiently reduce CO₂ to form CO under visible light illumination with high electivity (98%) and better activity than its homogeneous Re counterpart. Moreover, using advanced transient optical and X-ray absorption spectroscopy and in situ diffuse reflectance spectroscopy, we unraveled three key intermediates that are responsible for CS, the induction period, and rate limiting step in catalysis. This work not only demonstrates the potential of COFs as next generation photocatalysts for solar fuel conversion but also provide unprecedented insight into the mechanistic origins for light-driven CO₂ reduction.

Authors:

Yang, Sizhuo ^[1]; Hu, Wenhui ^[1]; Zhang, Xin ^[2]; He, Peilei ^[1];

^[1]; Liu, Cunming ^[3]; Cendejas, Melissa ^[4];

^[4];

^[3];

^[5];

^[1]

Marquette Univ., Milwaukee, WI (United States)
Univ.of Nebraska−Lincoln, Lincoln, NE (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of Wisconsin−Madison, Madison, WI (United States)
Univ.of Nebraska−Lincoln, Lincoln, NE (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Publication Date:: 2018-10-24

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

OSTI Identifier:: 1504460

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the American Chemical Society

Additional Journal Information:: Journal Volume: 140; Journal Issue: 44; Journal ID: ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Yang, Sizhuo, Hu, Wenhui, Zhang, Xin, He, Peilei, Pattengale, Brian, Liu, Cunming, Cendejas, Melissa, Hermans, Ive, Zhang, Xiaoyi, Zhang, Jian, and Huang, Jier. 2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO 2 Reduction.  United States: N. p., 2018. 
        Web.  doi:10.1021/jacs.8b09705.

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                    Yang, Sizhuo, Hu, Wenhui, Zhang, Xin, He, Peilei, Pattengale, Brian, Liu, Cunming, Cendejas, Melissa, Hermans, Ive, Zhang, Xiaoyi, Zhang, Jian, & Huang, Jier. 2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO 2 Reduction.  United States.  doi:https://doi.org/10.1021/jacs.8b09705

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                    Yang, Sizhuo, Hu, Wenhui, Zhang, Xin, He, Peilei, Pattengale, Brian, Liu, Cunming, Cendejas, Melissa, Hermans, Ive, Zhang, Xiaoyi, Zhang, Jian, and Huang, Jier. Wed .  
        "2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO 2 Reduction".  United States.  doi:https://doi.org/10.1021/jacs.8b09705.  https://www.osti.gov/servlets/purl/1504460.

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@article{osti_1504460,

  title        = {2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO 2 Reduction},

  author       = {Yang, Sizhuo and Hu, Wenhui and Zhang, Xin and He, Peilei and Pattengale, Brian and Liu, Cunming and Cendejas, Melissa and Hermans, Ive and Zhang, Xiaoyi and Zhang, Jian and Huang, Jier},

  abstractNote = {Covalent organic framework (COF) represents an emerging class of porous materials that have exhibited great potential in various applications, particularly in catalysis. Here, we report a newly designed 2D COF with incorporated Re complex, which exhibits intrinsic light absorption and charge separation (CS) properties. We show that this hybrid catalyst can efficiently reduce CO2 to form CO under visible light illumination with high electivity (98%) and better activity than its homogeneous Re counterpart. Moreover, using advanced transient optical and X-ray absorption spectroscopy and in situ diffuse reflectance spectroscopy, we unraveled three key intermediates that are responsible for CS, the induction period, and rate limiting step in catalysis. This work not only demonstrates the potential of COFs as next generation photocatalysts for solar fuel conversion but also provide unprecedented insight into the mechanistic origins for light-driven CO2 reduction.},

  doi          = {10.1021/jacs.8b09705},

  journal      = {Journal of the American Chemical Society},

  number       = 44,

  volume       = 140,

  place        = {United States},

  year         = {2018},

  month        = {10}

}

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DOI: https://doi.org/10.1021/jacs.8b09705

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Figure 2: Transient optical spectra of COF (a) and Re-COF (c) following 530 nm excitation. (b) The comparison of kinetics for ICT of COF and Re-COF. (d) The XANES spectrum of Re-COF at Re L₃-edge. The bottom panel is the difference spectrum after subtracting the laser-off spectrum from laser-on spectrummore »

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Title: 2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO 2 Reduction

Abstract

Citation Formats

Figures / Tables:

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Title: 2D Covalent Organic Frameworks as Intrinsic Photocatalysts for Visible Light-Driven CO ₂ Reduction

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