TY - JOUR
T1 - Photoelectrochemical Behavior of a Molecular Ru-Based Water-Oxidation Catalyst Bound to TiO2-Protected Si Photoanodes
AU - Matheu, Roc
AU - Moreno-Hernandez, Ivan A.
AU - Sala, Xavier
AU - Gray, Harry B.
AU - Brunschwig, Bruce S.
AU - Llobet, Antoni
AU - Lewis, Nathan S.
N1 - Funding Information:
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.
PY - 2017/8/23
Y1 - 2017/8/23
N2 - A hybrid photoanode based on a molecular water oxidation precatalyst was prepared from TiO2-protected n- or p+-Si coated with multiwalled carbon nanotubes (CNT) and the ruthenium-based water oxidation precatalyst [RuIV(tda)(py-pyr)2(O)], 1(O) (tda2- 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 TiO2 and 20 nm of a layer of sputtered C. At pH = 7 with 3 Sun illumination, the n-Si/TiO2/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 O2 evolution.
AB - A hybrid photoanode based on a molecular water oxidation precatalyst was prepared from TiO2-protected n- or p+-Si coated with multiwalled carbon nanotubes (CNT) and the ruthenium-based water oxidation precatalyst [RuIV(tda)(py-pyr)2(O)], 1(O) (tda2- 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 TiO2 and 20 nm of a layer of sputtered C. At pH = 7 with 3 Sun illumination, the n-Si/TiO2/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 O2 evolution.
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U2 - 10.1021/jacs.7b06800
DO - 10.1021/jacs.7b06800
M3 - Article
C2 - 28780849
AN - SCOPUS:85028046391
VL - 139
SP - 11345
EP - 11348
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 33
ER -