Transition-Metal Single Atoms in a Graphene Shell as Active Centers for Highly Efficient Artificial Photosynthesis
| Autor: | Chris Stokes, Haotian Wang, Yanbin Li, Kun Jiang, David C. Bell, Guangxu Chen, Ya-Wei Zhou, Jens K. Nørskov, Yongfeng Hu, Samira Siahrostami, Winfield Hill, Judith Lattimer, Wen-Bin Cai, Karen Chan, Austin Akey, Yi Cui, Mahesh K. Gangishetty, Zhiyi Lu |
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| Rok vydání: | 2017 |
| Předmět: |
General Chemical Engineering
chemistry.chemical_element 02 engineering and technology 010402 general chemistry Photochemistry 01 natural sciences Biochemistry Oxygen Artificial photosynthesis law.invention Catalysis Transition metal law Solar cell Materials Chemistry Environmental Chemistry Electrochemical reduction of carbon dioxide Chemistry Graphene Biochemistry (medical) Oxygen evolution General Chemistry 021001 nanoscience & nanotechnology 0104 chemical sciences Atomic physics 0210 nano-technology |
| Zdroj: | Chem. 3:950-960 |
| ISSN: | 2451-9294 |
| DOI: | 10.1016/j.chempr.2017.09.014 |
| Popis: | Summary 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. Coupled with Li + -tuned Co 3 O 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. |
| Databáze: | OpenAIRE |
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