Immobilization of “Capping Arene” Cobalt(II) Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation
Abstract
We report the synthesis, characterization, and electrocatalytic water oxidation activity of two cobalt complexes, (6-FP)Co(NO3)2 (1) (6-FP = 8,8'-(1,2-phenylene)diquinoline) and (5-FP)Co(NO3)2 (2) (5-FP = 1,2-bis(N-7-azaindolyl)benzene), containing “capping arene” bidentate ligands with nitrogen atom donors. The cobalt complexes 1 and 2 were supported on ordered mesoporous carbon (OMC) by π–π stacking, resulting in heterogenized cobalt materials 6-FP-Co-OMC-1 and 5-FP-Co-OMC-2, respectively, and studied for electrocatalytic water oxidation. We find that 6-FP-Co-OMC-1 exhibits an overpotential of 355 mV for a current density of 10 mA cm–2 and a turnover frequency (TOF) of ~0.53 s–1 at an overpotential of 400 mV at pH 14. 6-FP-Co-OMC-1 exhibits activity that is ~1.6 times that of 5-FP-Co-OMC-2, which gives a TOF of 0.32 s–1 at 400 mV overpotential. The structural stability of the single-atom Co site was demonstrated for 6-FP-Co-OMC-1 using X-ray absorption spectroscopy for the molecular complex supported on OMC, but slow degradation in catalyst activity can be attributed to eventual formation of Co oxide clusters. DFT computations of electrocatalytic water oxidation using the molecular complexes as models provide a description of the catalytic mechanism. These studies reveal that the mechanism for O–O bond formation involves an intermediate CoIV oxo complex that undergoes an intramolecular reductivemore »
- Authors:
-
[1];
[2];
[1];
[1];
[1];
[3];
[3];
[5];
[2];
[1];
[1]
- Univ. of Virginia, Charlottesville, VA (United States)
- California Institute of Technology (CalTech), Pasadena, CA (United States)
- Max Planck Institute for Chemical Energy Conversion, Mülheim an der Ruhr (Germany)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1856774
- Alternate Identifier(s):
- OSTI ID: 1889709
- Report Number(s):
- BNL-222885-2022-JAAM
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- SC0012704; CBET-1805022; CBET-2005250; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 24; Related Information: This article has been corrected related to duplicate figures. See https://doi.org/10.1021/acscatal.2c00122; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; cobalt; ordered mesoporous carbon; supported catalyst; electrocatalysis water; oxidation; conducting carbon
Citation Formats
Liu, Chang, Geer, Ana M., Webber, Christopher, Musgrave III, Charles B., Gu, Shunyan, Johnson, Grayson, Dickie, Diane A., Chabbra, Sonia, Schnegg, Alexander, Zhou, Hua, Sun, Cheng-Jun, Hwang, Sooyeon, Goddard III, William A., Zhang, Sen, and Gunnoe, T. Brent. Immobilization of “Capping Arene” Cobalt(II) Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation. United States: N. p., 2021.
Web. doi:10.1021/acscatal.1c04617.
Liu, Chang, Geer, Ana M., Webber, Christopher, Musgrave III, Charles B., Gu, Shunyan, Johnson, Grayson, Dickie, Diane A., Chabbra, Sonia, Schnegg, Alexander, Zhou, Hua, Sun, Cheng-Jun, Hwang, Sooyeon, Goddard III, William A., Zhang, Sen, & Gunnoe, T. Brent. Immobilization of “Capping Arene” Cobalt(II) Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation. United States. https://doi.org/10.1021/acscatal.1c04617
Liu, Chang, Geer, Ana M., Webber, Christopher, Musgrave III, Charles B., Gu, Shunyan, Johnson, Grayson, Dickie, Diane A., Chabbra, Sonia, Schnegg, Alexander, Zhou, Hua, Sun, Cheng-Jun, Hwang, Sooyeon, Goddard III, William A., Zhang, Sen, and Gunnoe, T. Brent. Thu .
"Immobilization of “Capping Arene” Cobalt(II) Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation". United States. https://doi.org/10.1021/acscatal.1c04617. https://www.osti.gov/servlets/purl/1856774.
@article{osti_1856774,
title = {Immobilization of “Capping Arene” Cobalt(II) Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation},
author = {Liu, Chang and Geer, Ana M. and Webber, Christopher and Musgrave III, Charles B. and Gu, Shunyan and Johnson, Grayson and Dickie, Diane A. and Chabbra, Sonia and Schnegg, Alexander and Zhou, Hua and Sun, Cheng-Jun and Hwang, Sooyeon and Goddard III, William A. and Zhang, Sen and Gunnoe, T. Brent},
abstractNote = {We report the synthesis, characterization, and electrocatalytic water oxidation activity of two cobalt complexes, (6-FP)Co(NO3)2 (1) (6-FP = 8,8'-(1,2-phenylene)diquinoline) and (5-FP)Co(NO3)2 (2) (5-FP = 1,2-bis(N-7-azaindolyl)benzene), containing “capping arene” bidentate ligands with nitrogen atom donors. The cobalt complexes 1 and 2 were supported on ordered mesoporous carbon (OMC) by π–π stacking, resulting in heterogenized cobalt materials 6-FP-Co-OMC-1 and 5-FP-Co-OMC-2, respectively, and studied for electrocatalytic water oxidation. We find that 6-FP-Co-OMC-1 exhibits an overpotential of 355 mV for a current density of 10 mA cm–2 and a turnover frequency (TOF) of ~0.53 s–1 at an overpotential of 400 mV at pH 14. 6-FP-Co-OMC-1 exhibits activity that is ~1.6 times that of 5-FP-Co-OMC-2, which gives a TOF of 0.32 s–1 at 400 mV overpotential. The structural stability of the single-atom Co site was demonstrated for 6-FP-Co-OMC-1 using X-ray absorption spectroscopy for the molecular complex supported on OMC, but slow degradation in catalyst activity can be attributed to eventual formation of Co oxide clusters. DFT computations of electrocatalytic water oxidation using the molecular complexes as models provide a description of the catalytic mechanism. These studies reveal that the mechanism for O–O bond formation involves an intermediate CoIV oxo complex that undergoes an intramolecular reductive O–O coupling to form a CoII–OOH species. Further, the calculations predict that the molecular 6-FP-Co structure is more active for electrocatalytic water oxidation than 5-FP-Co, which is consistent with experimental studies of 6-FP-Co-OMC-1 and 5-FP-Co-OMC-2, highlighting the possibility that the ligand structure influences the catalytic activity of the supported molecular catalysts.},
doi = {10.1021/acscatal.1c04617},
journal = {ACS Catalysis},
number = 24,
volume = 11,
place = {United States},
year = {Thu Dec 02 00:00:00 EST 2021},
month = {Thu Dec 02 00:00:00 EST 2021}
}
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