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Title: Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis

Abstract

Utilizing solar energy to fix CO 2 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 CO 2 electrocatalytic reduction. Here, we report transition-metal atoms coordinated in a graphene shell as active centers for aqueous CO 2 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 CO 2-to-CO conversion and suppress the competing hydrogen evolution reaction dramatically. Furthermore, coupled with Li+-tuned Co 3O 4 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:
 [1];  [2];  [1];  [2];  [2];  [1];  [3];  [1];  [1];  [2];  [4];  [1];  [4];  [1];  [5];  [6];  [7];  [1]
  1. Harvard Univ., Cambridge, MA (United States)
  2. Stanford Univ., Stanford, CA (United States)
  3. Univ. of Saskatchewan, Saskatoon, SK (Canada)
  4. Fudan Univ., Shanghai (China)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  7. Harvard Univ., Cambridge, MA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1485731
Alternate Identifier(s):
OSTI ID: 1463396
Grant/Contract Number:  
AC02-76SF00515; SC0004993; 2015CB932303; 21733004; 21327901; ECS-0335765; DESC0004993
Resource Type:
Published Article
Journal Name:
Chem
Additional Journal Information:
Journal Volume: 3; Journal Issue: 6; Journal ID: ISSN 2451-9294
Publisher:
Cell Press, 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. 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, and Wang, Haotian. Thu . "Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis". United States. doi: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 = {2017},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1016/j.chempr.2017.09.014

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Cited by: 10 works
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