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Ligand modification to stabilize the cobalt complexes for water oxidation
Shaanxi Normal Univ, Key Lab Macromol Sci Shaanxi Prov, Sch Chem & Chem Engn, Xian 710119, Shaanxi, Peoples R China.
Shaanxi Normal Univ, Key Lab Macromol Sci Shaanxi Prov, Sch Chem & Chem Engn, Xian 710119, Shaanxi, Peoples R China.
Shaanxi Normal Univ, Key Lab Macromol Sci Shaanxi Prov, Sch Chem & Chem Engn, Xian 710119, Shaanxi, Peoples R China.
Shaanxi Normal Univ, Key Lab Macromol Sci Shaanxi Prov, Sch Chem & Chem Engn, Xian 710119, Shaanxi, Peoples R China.
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2017 (English)In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 42, no 50, p. 29716-29724Article in journal (Refereed) Published
Abstract [en]

Ligand modifications with electron-withdrawing and electron-donating groups were applied to afford three novel mononuclear cobalt-based catalysts [Co(TPA-R)]2+ (TPA = tris(2-pyridylmethyl) amine; R = tri-α F, 1; R = tri-αOMe, 2; R = mono-αF, 3) for water oxidation. Characterization of the catalysts shows that steric and electronic factors play important roles in inhibiting spontaneous intermolecular dimerization of two cobalt centers, and influence the catalytic behavior. Complex 1 exhibits the best catalytic ability and stability, showing a good efficiency with TOF of 6.03 ± 0.02 mol (O2)/(mol (cat)*s) in photo-induced water oxidation experiments using Ru (bpy)3 2+ as photosensitizer and Na2S2O8 as electron acceptor. The bulky electron donating groups in 2 led to degradation of the complex and formation of CoOx particles acting as the real catalyst. Electron-withdrawing substituents on the TPA ligand can stabilize the catalyst under both electrochemical and photo-induced conditions, with the enhancement increasing with the number of the electron-withdrawing groups. © 2017 Hydrogen Energy Publications LLC.

Place, publisher, year, edition, pages
Elsevier, 2017. Vol. 42, no 50, p. 29716-29724
Keywords [en]
Water oxidation, Photo-induced, Cobalt catalyst, Ligand modification, Catalytic behavior
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-335940DOI: 10.1016/j.ijhydene.2017.10.066ISI: 000419417600009Scopus ID: 2-s2.0-85034447058OAI: oai:DiVA.org:uu-335940DiVA, id: diva2:1164373
Funder
Swedish Energy Agency, 11674-5Knut and Alice Wallenberg Foundation, 2011.0067
Note

Funding details: Shaanxi Normal University; Funding details: Energimyndigheten; Funding details: National Natural Science Foundation of China; Funding details: Knut och Alice Wallenbergs StiftelseN1 - Funding text: This work is supported by the National Natural Science Foundation of China ( 21402113 ), the Fundamental Research Funds for the Central Universities ( GK201703025 ). AT and SS gratefully acknowledge the Swedish Energy Agency ( 11674-5 ) and the Knut and Alice Wallenberg Foundation ( 2011.0067 ) for funding. We are grateful for Prof. Jing Liu at Shaanxi Normal University to provide DLS instrument. Appendix A

Available from: 2017-12-11 Created: 2017-12-11 Last updated: 2018-02-16Bibliographically approved

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Styring, StenbjörnThapper, Anders

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