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Title: Surface and Structural Investigation of a MnO x Birnessite‐Type Water Oxidation Catalyst Formed under Photocatalytic Conditions

Abstract

Abstract Catalytically active MnO x species have been reported to form in situ from various Mn‐complexes during electrocatalytic and solution‐based water oxidation when employing cerium(IV) ammonium ammonium nitrate (CAN) oxidant as a sacrificial reagent. The full structural characterization of these oxides may be complicated by the presence of support material and lack of a pure bulk phase. For the first time, we show that highly active MnO x catalysts form without supports in situ under photocatalytic conditions. Our most active 4 MnO x catalyst (∼0.84 mmol O 2  mol Mn −1  s −1 ) forms from a Mn 4 O 4 bearing a metal–organic framework. 4 MnO x is characterized by pair distribution function analysis (PDF), Raman spectroscopy, and HR‐TEM as a disordered, layered Mn‐oxide with high surface area (216 m 2 g −1 ) and small regions of crystallinity and layer flexibility. In contrast, the S MnO x formed from Mn 2+ salt gives an amorphous species of lower surface area (80 m 2 g −1 ) and lower activity (∼0.15 mmol O 2  mol Mn −1  s −1 ). We compare these catalysts to crystalline hexagonal birnessite, which activates under the same conditions. Full deconvolution ofmore » the XPS Mn2p 3/2 core levels detects enriched Mn 3+ and Mn 2+ content on the surfaces, which indicates possible disproportionation/comproportionation surface equilibria.« less

Authors:
; ; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1786147
Grant/Contract Number:  
AC02-06CH11357; FG02-08ER46491; 434878; CHE-1213772; DGE0903675
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Name: Chemistry - A European Journal Journal Volume: 21 Journal Issue: 40; Journal ID: ISSN 0947-6539
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Deibert, Benjamin J., Zhang, Jingming, Smith, Paul F., Chapman, Karena W., Rangan, Sylvie, Banerjee, Debasis, Tan, Kui, Wang, Hao, Pasquale, Nicholas, Chen, Feng, Lee, Ki‐Bum, Dismukes, G. Charles, Chabal, Yves J., and Li, Jing. Surface and Structural Investigation of a MnO x Birnessite‐Type Water Oxidation Catalyst Formed under Photocatalytic Conditions. Germany: N. p., 2015. Web. doi:10.1002/chem.201501930.
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Deibert, Benjamin J., Zhang, Jingming, Smith, Paul F., Chapman, Karena W., Rangan, Sylvie, Banerjee, Debasis, Tan, Kui, Wang, Hao, Pasquale, Nicholas, Chen, Feng, Lee, Ki‐Bum, Dismukes, G. Charles, Chabal, Yves J., & Li, Jing. Surface and Structural Investigation of a MnO x Birnessite‐Type Water Oxidation Catalyst Formed under Photocatalytic Conditions. Germany. https://doi.org/10.1002/chem.201501930
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Deibert, Benjamin J., Zhang, Jingming, Smith, Paul F., Chapman, Karena W., Rangan, Sylvie, Banerjee, Debasis, Tan, Kui, Wang, Hao, Pasquale, Nicholas, Chen, Feng, Lee, Ki‐Bum, Dismukes, G. Charles, Chabal, Yves J., and Li, Jing. Tue . "Surface and Structural Investigation of a MnO x Birnessite‐Type Water Oxidation Catalyst Formed under Photocatalytic Conditions". Germany. https://doi.org/10.1002/chem.201501930.
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@article{osti_1786147,
title = {Surface and Structural Investigation of a MnO x Birnessite‐Type Water Oxidation Catalyst Formed under Photocatalytic Conditions},
author = {Deibert, Benjamin J. and Zhang, Jingming and Smith, Paul F. and Chapman, Karena W. and Rangan, Sylvie and Banerjee, Debasis and Tan, Kui and Wang, Hao and Pasquale, Nicholas and Chen, Feng and Lee, Ki‐Bum and Dismukes, G. Charles and Chabal, Yves J. and Li, Jing},
abstractNote = {Abstract Catalytically active MnO x species have been reported to form in situ from various Mn‐complexes during electrocatalytic and solution‐based water oxidation when employing cerium(IV) ammonium ammonium nitrate (CAN) oxidant as a sacrificial reagent. The full structural characterization of these oxides may be complicated by the presence of support material and lack of a pure bulk phase. For the first time, we show that highly active MnO x catalysts form without supports in situ under photocatalytic conditions. Our most active 4 MnO x catalyst (∼0.84 mmol O 2  mol Mn −1  s −1 ) forms from a Mn 4 O 4 bearing a metal–organic framework. 4 MnO x is characterized by pair distribution function analysis (PDF), Raman spectroscopy, and HR‐TEM as a disordered, layered Mn‐oxide with high surface area (216 m 2 g −1 ) and small regions of crystallinity and layer flexibility. In contrast, the S MnO x formed from Mn 2+ salt gives an amorphous species of lower surface area (80 m 2 g −1 ) and lower activity (∼0.15 mmol O 2  mol Mn −1  s −1 ). We compare these catalysts to crystalline hexagonal birnessite, which activates under the same conditions. Full deconvolution of the XPS Mn2p 3/2 core levels detects enriched Mn 3+ and Mn 2+ content on the surfaces, which indicates possible disproportionation/comproportionation surface equilibria.},
doi = {10.1002/chem.201501930},
journal = {Chemistry - A European Journal},
number = 40,
volume = 21,
place = {Germany},
year = {Tue Aug 11 00:00:00 EDT 2015},
month = {Tue Aug 11 00:00:00 EDT 2015}
}
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  • Kostka, Joel E.; Luther, George W.; Nealson, Kenneth H.
  • Geochimica et Cosmochimica Acta, Vol. 59, Issue 5
  • DOI: 10.1016/0016-7037(95)00007-0
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