U.S. Department of EnergyOffice of Scientific and Technical Information
Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen
Abstract
A bio-inspired O2 sensitive nickel catalyst dispersed in a hydrophobic and redox-silent polymer matrix shows enhanced stability for catalytic H2 oxidation as well as O2 tolerance. A simple but efficient electrode design separates the catalyst into two different reaction layers to promote different reactivity on the catalyst. (1) close to the electrode surface, the catalyst can directly exchange electrons with the electrode and generate current from H2 oxidation; and (2) at the outer film boundary, the electrolyte exposed layer is electrically isolated from the electrode, which enables the H2 reduced Ni-complex to convert O2 to H2O and thus provides protection to the O2-sensitive inner reaction layer. This strategy solves one of the biggest limitations of these otherwise outstanding catalysts and could be used to protect other similar catalysts whose wider application is currently limited by sensitivity towards oxygen.
- Authors:
-
[2];
[2];
[1]
- Max Planck Inst. for Chemical Energy Conversion, Ruhr (Germany)
- Univ. Bochum (Germany)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1424831
- Report Number(s):
- PNNL-SA-129794
Journal ID: ISSN 2041-1723; KC0302010
- Grant/Contract Number:
- AC05-76RL01830
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE
Citation Formats
Oughli, Alaa A., Ruff, Adrian, Boralugodage, Nilusha Priyadarshani, Rodríguez-Maciá, Patricia, Plumeré, Nicolas, Lubitz, Wolfgang, Shaw, Wendy J., Schuhmann, Wolfgang, and Rüdiger, Olaf. Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-03011-7.
Oughli, Alaa A., Ruff, Adrian, Boralugodage, Nilusha Priyadarshani, Rodríguez-Maciá, Patricia, Plumeré, Nicolas, Lubitz, Wolfgang, Shaw, Wendy J., Schuhmann, Wolfgang, & Rüdiger, Olaf. Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen. United States. https://doi.org/10.1038/s41467-018-03011-7
Oughli, Alaa A., Ruff, Adrian, Boralugodage, Nilusha Priyadarshani, Rodríguez-Maciá, Patricia, Plumeré, Nicolas, Lubitz, Wolfgang, Shaw, Wendy J., Schuhmann, Wolfgang, and Rüdiger, Olaf. 2018.
"Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen". United States. https://doi.org/10.1038/s41467-018-03011-7. https://www.osti.gov/servlets/purl/1424831.
@article{osti_1424831,
title = {Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen},
author = {Oughli, Alaa A. and Ruff, Adrian and Boralugodage, Nilusha Priyadarshani and Rodríguez-Maciá, Patricia and Plumeré, Nicolas and Lubitz, Wolfgang and Shaw, Wendy J. and Schuhmann, Wolfgang and Rüdiger, Olaf},
abstractNote = {A bio-inspired O2 sensitive nickel catalyst dispersed in a hydrophobic and redox-silent polymer matrix shows enhanced stability for catalytic H2 oxidation as well as O2 tolerance. A simple but efficient electrode design separates the catalyst into two different reaction layers to promote different reactivity on the catalyst. (1) close to the electrode surface, the catalyst can directly exchange electrons with the electrode and generate current from H2 oxidation; and (2) at the outer film boundary, the electrolyte exposed layer is electrically isolated from the electrode, which enables the H2 reduced Ni-complex to convert O2 to H2O and thus provides protection to the O2-sensitive inner reaction layer. This strategy solves one of the biggest limitations of these otherwise outstanding catalysts and could be used to protect other similar catalysts whose wider application is currently limited by sensitivity towards oxygen.},
doi = {10.1038/s41467-018-03011-7},
url = {https://www.osti.gov/biblio/1424831},
journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 9,
place = {United States},
year = {Wed Feb 28 00:00:00 EST 2018},
month = {Wed Feb 28 00:00:00 EST 2018}
}
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Carbon-Nanotube-Supported Bio-Inspired Nickel Catalyst and Its Integration in Hybrid Hydrogen/Air Fuel Cells
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Clean Donor Oxidation Enhances the H 2 Evolution Activity of a Carbon Quantum Dot–Molecular Catalyst Photosystem
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Arginine-Containing Ligands Enhance H 2 Oxidation Catalyst Performance
journal, May 2014
- Dutta, Arnab; Roberts, John A. S.; Shaw, Wendy J.
- Angewandte Chemie International Edition, Vol. 53, Issue 25
Direct Comparison of the Performance of a Bio-inspired Synthetic Nickel Catalyst and a [NiFe]-Hydrogenase, Both Covalently Attached to Electrodes
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- Rodriguez-Maciá, Patricia; Dutta, Arnab; Lubitz, Wolfgang
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A Redox Hydrogel Protects the O 2 -Sensitive [FeFe]-Hydrogenase from Chlamydomonas reinhardtii from Oxidative Damage
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- Angewandte Chemie International Edition, Vol. 54, Issue 42
Carbon-Nanotube-Supported Bio-Inspired Nickel Catalyst and Its Integration in Hybrid Hydrogen/Air Fuel Cells
journal, January 2017
- Gentil, Solène; Lalaoui, Noémie; Dutta, Arnab
- Angewandte Chemie International Edition, Vol. 56, Issue 7
The Role of a Dipeptide Outer-Coordination Sphere on H 2 -Production Catalysts: Influence on Catalytic Rates and Electron Transfer
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- Reback, Matthew L.; Ginovska-Pangovska, Bojana; Ho, Ming-Hsun
- Chemistry - A European Journal, Vol. 19, Issue 6
Covalent Attachment of the Water-insoluble Ni(P Cy 2 N Phe 2 ) 2 Electrocatalyst to Electrodes Showing Reversible Catalysis in Aqueous Solution
journal, October 2016
- Rodríguez-Maciá, Patricia; Priyadarshani, Nilusha; Dutta, Arnab
- Electroanalysis, Vol. 28, Issue 10
Wiring of the aldehyde oxidoreductase PaoABC to electrode surfaces via entrapment in low potential phenothiazine-modified redox polymers
journal, June 2016
- Pinyou, Piyanut; Ruff, Adrian; Pöller, Sascha
- Bioelectrochemistry, Vol. 109
Achieving Reversible H 2 /H + Interconversion at Room Temperature with Enzyme-Inspired Molecular Complexes: A Mechanistic Study
journal, August 2016
- Priyadarshani, Nilusha; Dutta, Arnab; Ginovska, Bojana
- ACS Catalysis, Vol. 6, Issue 9
Protection and Reactivation of the [NiFeSe] Hydrogenase from Desulfovibrio vulgaris Hildenborough under Oxidative Conditions
journal, April 2017
- Ruff, Adrian; Szczesny, Julian; Zacarias, Sónia
- ACS Energy Letters, Vol. 2, Issue 5
Hydrogenases
journal, March 2014
- Lubitz, Wolfgang; Ogata, Hideaki; Rüdiger, Olaf
- Chemical Reviews, Vol. 114, Issue 8
Development of Molecular Electrocatalysts for Energy Storage
journal, February 2014
- DuBois, Daniel L.
- Inorganic Chemistry, Vol. 53, Issue 8
Hydrogen Oxidation and Production Using Nickel-Based Molecular Catalysts with Positioned Proton Relays
journal, January 2006
- Wilson, Aaron D.; Newell, Rachel H.; McNevin, Michael J.
- Journal of the American Chemical Society, Vol. 128, Issue 1
Mechanism of Protection of Catalysts Supported in Redox Hydrogel Films
journal, April 2015
- Fourmond, Vincent; Stapf, Stefanie; Li, Huaiguang
- Journal of the American Chemical Society, Vol. 137, Issue 16
Biomimetic assembly and activation of [FeFe]-hydrogenases
journal, June 2013
- Berggren, G.; Adamska, A.; Lambertz, C.
- Nature, Vol. 499, Issue 7456
Reduction of oxygen catalyzed by nickel diphosphine complexes with positioned pendant amines
journal, January 2010
- Yang, Jenny Y.; Bullock, R. Morris; Dougherty, William G.
- Dalton Transactions, Vol. 39, Issue 12
Energy and environment policy case for a global project on artificial photosynthesis
journal, January 2013
- Faunce, Thomas A.; Lubitz, Wolfgang; Rutherford, A. W. (Bill)
- Energy & Environmental Science, Vol. 6, Issue 3
Oxygen-tolerant proton reduction catalysis: much O 2 about nothing?
journal, January 2015
- Wakerley, David W.; Reisner, Erwin
- Energy & Environmental Science, Vol. 8, Issue 8
Powering the planet: Chemical challenges in solar energy utilization
journal, October 2006
- Lewis, N. S.; Nocera, D. G.
- Proceedings of the National Academy of Sciences, Vol. 103, Issue 43, p. 15729-15735
Chemical approaches to artificial photosynthesis
journal, September 2012
- Concepcion, J. J.; House, R. L.; Papanikolas, J. M.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 39
Amino acid modified Ni catalyst exhibits reversible H 2 oxidation/production over a broad pH range at elevated temperatures
journal, November 2014
- Dutta, Arnab; DuBois, Daniel L.; Roberts, John A. S.
- Proceedings of the National Academy of Sciences, Vol. 111, Issue 46
A Synthetic Nickel Electrocatalyst with a Turnover Frequency Above 100,000 s-1 for H2 Production
journal, August 2011
- Helm, M. L.; Stewart, M. P.; Bullock, R. M.
- Science, Vol. 333, Issue 6044, p. 863-866
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