Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis
Abstract
Utilizing solar energy to fix CO2 with water into chemical fuels and oxygen, a mimic process of photosynthesis in nature, is becoming increasingly important but still challenged by low selectivity and activity, especially in CO2 electrocatalytic reduction. Here, we report transition-metal atoms coordinated in a graphene shell as active centers for aqueous CO2 reduction to CO with high faradic efficiencies over 90% under significant currents up to ~60 mA/mg. We employed three-dimensional atom probe tomography to directly identify the single Ni atomic sites in graphene vacancies. Theoretical simulations suggest that compared with metallic Ni, the Ni atomic sites present different electronic structures that facilitate CO2-to-CO conversion and suppress the competing hydrogen evolution reaction dramatically. Furthermore, coupled with Li+-tuned Co3O4 oxygen evolution catalyst and powered by a triple-junction solar cell, our artificial photosynthesis system achieves a peak solar-to-CO efficiency of 12.7% by using earth-abundant transition-metal electrocatalysts in a pH-equal system.
- Authors:
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1485731
- Alternate Identifier(s):
- OSTI ID: 1463396
- Grant/Contract Number:
- DESC0004993; AC02-76SF00515; SC0004993; 2015CB932303; 21733004; 21327901; ECS-0335765
- Resource Type:
- Published Article
- Journal Name:
- Chem
- Additional Journal Information:
- Journal Name: Chem Journal Volume: 3 Journal Issue: 6; Journal ID: ISSN 2451-9294
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; artificial photosynthesis; renewable energy; single-atom catalysis; transition metals; nickel single atoms; graphene; carbon dioxide reduction; oxygen evolution reaction; solar-to-fuel conversion; three-dimensional atom probe tomography
Citation Formats
Jiang, Kun, Siahrostami, Samira, Akey, Austin J., Li, Yanbin, Lu, Zhiyi, Lattimer, Judith, Hu, Yongfeng, Stokes, Chris, Gangishetty, Mahesh, Chen, Guangxu, Zhou, Yawei, Hill, Winfield, Cai, Wen-Bin, Bell, David, Chan, Karen, Nørskov, Jens K., Cui, Yi, and Wang, Haotian. Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis. United States: N. p., 2017.
Web. doi:10.1016/j.chempr.2017.09.014.
Jiang, Kun, Siahrostami, Samira, Akey, Austin J., Li, Yanbin, Lu, Zhiyi, Lattimer, Judith, Hu, Yongfeng, Stokes, Chris, Gangishetty, Mahesh, Chen, Guangxu, Zhou, Yawei, Hill, Winfield, Cai, Wen-Bin, Bell, David, Chan, Karen, Nørskov, Jens K., Cui, Yi, & Wang, Haotian. Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis. United States. https://doi.org/10.1016/j.chempr.2017.09.014
Jiang, Kun, Siahrostami, Samira, Akey, Austin J., Li, Yanbin, Lu, Zhiyi, Lattimer, Judith, Hu, Yongfeng, Stokes, Chris, Gangishetty, Mahesh, Chen, Guangxu, Zhou, Yawei, Hill, Winfield, Cai, Wen-Bin, Bell, David, Chan, Karen, Nørskov, Jens K., Cui, Yi, and Wang, Haotian. Fri .
"Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis". United States. https://doi.org/10.1016/j.chempr.2017.09.014.
@article{osti_1485731,
title = {Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis},
author = {Jiang, Kun and Siahrostami, Samira and Akey, Austin J. and Li, Yanbin and Lu, Zhiyi and Lattimer, Judith and Hu, Yongfeng and Stokes, Chris and Gangishetty, Mahesh and Chen, Guangxu and Zhou, Yawei and Hill, Winfield and Cai, Wen-Bin and Bell, David and Chan, Karen and Nørskov, Jens K. and Cui, Yi and Wang, Haotian},
abstractNote = {Utilizing solar energy to fix CO2 with water into chemical fuels and oxygen, a mimic process of photosynthesis in nature, is becoming increasingly important but still challenged by low selectivity and activity, especially in CO2 electrocatalytic reduction. Here, we report transition-metal atoms coordinated in a graphene shell as active centers for aqueous CO2 reduction to CO with high faradic efficiencies over 90% under significant currents up to ~60 mA/mg. We employed three-dimensional atom probe tomography to directly identify the single Ni atomic sites in graphene vacancies. Theoretical simulations suggest that compared with metallic Ni, the Ni atomic sites present different electronic structures that facilitate CO2-to-CO conversion and suppress the competing hydrogen evolution reaction dramatically. Furthermore, coupled with Li+-tuned Co3O4 oxygen evolution catalyst and powered by a triple-junction solar cell, our artificial photosynthesis system achieves a peak solar-to-CO efficiency of 12.7% by using earth-abundant transition-metal electrocatalysts in a pH-equal system.},
doi = {10.1016/j.chempr.2017.09.014},
journal = {Chem},
number = 6,
volume = 3,
place = {United States},
year = {Fri Dec 01 00:00:00 EST 2017},
month = {Fri Dec 01 00:00:00 EST 2017}
}
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https://doi.org/10.1016/j.chempr.2017.09.014
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