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Electrocatalytic water oxidation using (bpy)₂Co-based precursors

Holland, Ryan Lynn and Tubbs, Holly M. and McKeown, Bradley Aaron and Nielsen, Robert J. and Goddard, William Andrew and Gunnoe, T. Brent (2019) Electrocatalytic water oxidation using (bpy)₂Co-based precursors. In: 258th ACS National Meeting & Exposition, 25-29 August 2019, San Diego, CA.

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As an earth-abundant and inexpensive first-row transition metal, cobalt is a good candidate for the development of water oxidn. catalysts. The (bpy) ₂Co (bpy = 2,2'-bipyridine) mol. motif offers stable and functional electrocatalytic water oxidn., while substituents on the bipyridyl group offer a ready means for attachment to materials. Data are consistent with the Co(II) complex (bpy) ₂Co(NO3)₂ (1-H) serving as an active and robust catalyst in neutral aq. conditions with a catalytic potential (E_(cat)) of 1.3 V vs NHE at a scan rate of 20 mV s⁻¹ in 0.1 M phosphate buffer and an estd. turnover frequency of 40 s⁻¹. A series of (Ybpy)₂CoX₂ complexes (Ybpy = 4,4'-disubstituted bpy ligands with Y = NH₂ or NO₂; X = NO₃ or Cl) were synthesized and tested for electrocatalytic water oxidn. to det. the effect of electron-withdrawing and electrondonating substituents on electrocatalytic activity. Addnl., the diamino-substituted complex (4,4'-NH2bpy)₂Co(NO3)₂ (1-NH₂) serves as an avenue of approach for the functionalization of carbon-based material supports and the development of heterogeneous water oxidn. catalysts. Complex 1-NH₂ was utilized to append the (bpy)₂Co motif to carbon-materials derived from the hydrothermal carbonization (HTC) of monosaccharide starting materials via diazotization. Alternatively, addn. of 4,4'-divinyl-2,2'-bipyridine during the HTC synthesis provided a carbon material with pre-ligated coordination sites, which allowed for direct metalation with simple metal salts such as CoCl₂.bul.6H₂O or CoNO₃.bul.6H₂O.

Item Type:Conference or Workshop Item (Paper)
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URLURL TypeDescription Website
Nielsen, Robert J.0000-0002-7962-0186
Goddard, William Andrew0000-0003-0097-5716
Gunnoe, T. Brent0000-0001-5714-3887
Additional Information:© 2019 American Chemical Society.
Record Number:CaltechAUTHORS:20200430-073830291
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:102914
Deposited By: Tony Diaz
Deposited On:30 Apr 2020 15:40
Last Modified:30 Apr 2020 15:40

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