CaltechAUTHORS
  A Caltech Library Service

Photoelectrochemical Behavior of a Molecular Ru-Based Water-Oxidation Catalyst Bound to TiO_2-Protected Si Photoanodes

Matheu, Roc and Moreno-Hernandez, Ivan A. and Sala, Xavier and Gray, Harry B. and Brunschwig, Bruce S. and Llobet, Antoni and Lewis, Nathan S. (2017) Photoelectrochemical Behavior of a Molecular Ru-Based Water-Oxidation Catalyst Bound to TiO_2-Protected Si Photoanodes. Journal of the American Chemical Society, 139 (33). pp. 11345-11348. ISSN 0002-7863. http://resolver.caltech.edu/CaltechAUTHORS:20170816-083201966

[img] PDF (Experimental section, additional characterization and electrochemical data) - Supplemental Material
See Usage Policy.

1582Kb

Use this Persistent URL to link to this item: http://resolver.caltech.edu/CaltechAUTHORS:20170816-083201966

Abstract

A hybrid photoanode based on a molecular water oxidation precatalyst was prepared from TiO_2-protected n- or p+-Si coated with multiwalled carbon nanotubes (CNT) and the ruthenium-based water oxidation precatalyst [Ru^(IV)(tda)(py-pyr)_2(O)], 1(O) (tda^(2–) is [2,2′:6′,2″-terpyridine]-6,6″-dicarboxylato and py-pir is 4-(pyren-1-yl)-N-(pyridin-4-ylmethyl)butanamide). The Ru complex was immobilized by π–π stacking onto CNTs that had been deposited by drop casting onto Si electrodes coated with 60 nm of amorphous TiO_2 and 20 nm of a layer of sputtered C. At pH = 7 with 3 Sun illumination, the n-Si/TiO_2/C/CNT/[1+1(O)] electrodes exhibited current densities of 1 mA cm^(–2) at 1.07 V vs NHE. The current density was maintained for >200 min at a constant potential while intermittently collecting voltammograms that indicated that over half of the Ru was still in molecular form after O_2 evolution.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/jacs.7b06800DOIArticle
http://pubs.acs.org/doi/abs/10.1021/jacs.7b06800PublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/jacs.7b06800PublisherSupporting Information
ORCID:
AuthorORCID
Matheu, Roc0000-0001-8601-5219
Moreno-Hernandez, Ivan A.0000-0001-6461-9214
Brunschwig, Bruce S.0000-0002-6135-6727
Llobet, Antoni0000-0002-6176-5272
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2017 American Chemical Society. Received: June 30, 2017; Published: August 7, 2017. The National Science Foundation under NSF Center CHE-1305124 provided support for H.B.G., I.M.H., N.S.L., B.S.B., and R.M. and for supplies at Caltech, I.M.H. was supported by a NSF Graduate Research Fellowship (Grant No. DGE-1144469). Instrumentation support was also provided by the Molecular Materials Resource Center of the Beckman Institute at California Institute of Technology. R.M., A.L., and X.S. acknowledge MINECO and FEDER (CTQ2016-80058-R, CTQ2015-64261-R, SEV 2013-0319, ENE2016-82025-REDT, CTQ2016-81923-REDC), AGAUR (2014-SGR-915), and “La Caixa” foundation. We acknowledge Dr. K. Sun for helpful discussions. The authors declare no competing financial interest.
Group:Kavli Nanoscience Institute
Funders:
Funding AgencyGrant Number
NSFCHE-1305124
NSF Graduate Research FellowshipDGE-1144469
Ministerio de Economía y Competitividad (MINECO)CTQ2016-80058-R
Ministerio de Economía y Competitividad (MINECO)CTQ2015-64261-R
Ministerio de Economía y Competitividad (MINECO)SEV 2013-0319
Ministerio de Economía y Competitividad (MINECO)ENE2016-82025-REDT
Ministerio de Economía y Competitividad (MINECO)CTQ2016-81923-REDC
Agència de Gestió d'Ajuts Universitaris i de Recerca2014-SGR-915
La Caixa FoundationUNSPECIFIED
Record Number:CaltechAUTHORS:20170816-083201966
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20170816-083201966
Official Citation:Photoelectrochemical Behavior of a Molecular Ru-Based Water-Oxidation Catalyst Bound to TiO2-Protected Si Photoanodes Roc Matheu, Ivan A. Moreno-Hernandez, Xavier Sala, Harry B. Gray, Bruce S. Brunschwig, Antoni Llobet, and Nathan S. Lewis Journal of the American Chemical Society 2017 139 (33), 11345-11348 DOI: 10.1021/jacs.7b06800
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:80464
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:16 Aug 2017 16:14
Last Modified:14 Sep 2017 17:17

Repository Staff Only: item control page