Visible-light-switched electron transfer over single porphyrin-metal atom center for highly selective electroreduction of carbon dioxide
External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO 2 reduction by mimicking the structure of...
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| Published in | Nature communications Vol. 10; no. 1; pp. 3844 - 10 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
26.08.2019
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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| Abstract | External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO
2
reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h
−1
at −1.1 V and CO Faradaic efficiency (FE) of 94.2% at −0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center.
The light field effect can improve performance in electrocatalytic processes, but is not fully understood. Here the authors design a photo-coupled electrocatalyst using a porphyrin ligand as a photosensitizer and a coordinated metal as a catalytically active site for carbon dioxide reduction. |
|---|---|
| AbstractList | External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO2 reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h−1 at −1.1 V and CO Faradaic efficiency (FE) of 94.2% at −0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center. External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO 2 reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h −1 at −1.1 V and CO Faradaic efficiency (FE) of 94.2% at −0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center. The light field effect can improve performance in electrocatalytic processes, but is not fully understood. Here the authors design a photo-coupled electrocatalyst using a porphyrin ligand as a photosensitizer and a coordinated metal as a catalytically active site for carbon dioxide reduction. External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO2 reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h-1 at -1.1 V and CO Faradaic efficiency (FE) of 94.2% at -0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center.External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO2 reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h-1 at -1.1 V and CO Faradaic efficiency (FE) of 94.2% at -0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center. External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h at -1.1 V and CO Faradaic efficiency (FE) of 94.2% at -0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center. The light field effect can improve performance in electrocatalytic processes, but is not fully understood. Here the authors design a photo-coupled electrocatalyst using a porphyrin ligand as a photosensitizer and a coordinated metal as a catalytically active site for carbon dioxide reduction. External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO 2 reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h −1 at −1.1 V and CO Faradaic efficiency (FE) of 94.2% at −0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center. |
| ArticleNumber | 3844 |
| Author | Liu, Xiaozhi Zuo, Shouwei Gu, Lin Yang, Deren Wang, Dong He, Ting Yu, Hongde Yang, Haozhou Wang, Xun Li, Haoyi Ni, Bing |
| Author_xml | – sequence: 1 givenname: Deren orcidid: 0000-0002-2133-8612 surname: Yang fullname: Yang, Deren organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University – sequence: 2 givenname: Hongde surname: Yu fullname: Yu, Hongde organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University – sequence: 3 givenname: Ting orcidid: 0000-0001-8308-8738 surname: He fullname: He, Ting organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University – sequence: 4 givenname: Shouwei orcidid: 0000-0001-8936-4668 surname: Zuo fullname: Zuo, Shouwei organization: Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences – sequence: 5 givenname: Xiaozhi orcidid: 0000-0001-8647-8694 surname: Liu fullname: Liu, Xiaozhi organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences – sequence: 6 givenname: Haozhou surname: Yang fullname: Yang, Haozhou organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University – sequence: 7 givenname: Bing orcidid: 0000-0001-9657-6933 surname: Ni fullname: Ni, Bing organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University – sequence: 8 givenname: Haoyi orcidid: 0000-0002-0723-8068 surname: Li fullname: Li, Haoyi organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University – sequence: 9 givenname: Lin surname: Gu fullname: Gu, Lin organization: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences – sequence: 10 givenname: Dong orcidid: 0000-0002-0594-0515 surname: Wang fullname: Wang, Dong organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University – sequence: 11 givenname: Xun orcidid: 0000-0002-8066-4450 surname: Wang fullname: Wang, Xun email: wangxun@mail.tsinghua.edu.cn organization: Key Lab of Organic Optoelectronics and Molecular Engineering, Department of Chemistry, Tsinghua University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31451689$$D View this record in MEDLINE/PubMed |
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| Snippet | External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic... The light field effect can improve performance in electrocatalytic processes, but is not fully understood. Here the authors design a photo-coupled... |
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| SubjectTerms | 147/137 147/143 147/28 639/301 639/638 639/925 Carbon dioxide Catalysis Catalysts Chlorophyll Copper Efficiency Electrocatalysts Electron transfer Energy Energy gap Gold Humanities and Social Sciences Ligands Light Light effects Microscopy Mimicry multidisciplinary Nanoparticles Oxidation Physics Science Science (multidisciplinary) Wavelet transforms |
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| Title | Visible-light-switched electron transfer over single porphyrin-metal atom center for highly selective electroreduction of carbon dioxide |
| URI | https://link.springer.com/article/10.1038/s41467-019-11817-2 https://www.ncbi.nlm.nih.gov/pubmed/31451689 https://www.proquest.com/docview/2280471244 https://www.proquest.com/docview/2281108898 https://pubmed.ncbi.nlm.nih.gov/PMC6710284 https://doaj.org/article/85ed472523964a36808bb40593cf373a |
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