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Title: Can nitro groups really anchor onto TiO2? Case study of dye-to-TiO2 adsorption using azo dyes with NO2 substituents

Abstract

The nitro group has recently been suggested as a new type of anchor for dye-sensitized solar cells (DSSCs) and has shown promising optoelectronic properties. Considering the excellent electron withdrawing ability of the nitro group and wider materials selection brought about by this substituent, it is helpful to evaluate the interfacial structures and photophysics of more organic dyes where NO2 poses as the dye-to-TiO2 anchor. A computational study on a family of azo dyes bearing a nitro group is presented in this paper, where the effect of certain side groups on their optical properties is examined. Both isolated dye molecules and dye/TiO2 nanocomposites are studied via density functional theory and time-dependent density functional theory, with complementary experimental UV/vis absorption spectroscopy and photovoltaic device testing. Results demonstrate that these nitro-containing dyes prefer a monodentate anchoring mode on a TiO2 cluster. These nitro dyes reveal weak, but non-negligible, adsorption onto TiO2; yet, very low photovoltaic performance once incorporated into a DSSC device. Finally, this poor delivery of nitro groups as DSSC anchors is ostensibly inconsistent with previous findings; but is rationalized via the “auxiliary anchor” concept.

Authors:
 [1];  [2]
  1. Nanjing Univ. of Information Science and Technology (China). Dept. of Physics; Univ. of Cambridge (United Kingdom). Cavendish Lab.
  2. Univ. of Cambridge (United Kingdom). Cavendish Lab. Dept. of Chemical Engineering and Biotechnology; Argonne National Lab. (ANL), Argonne, IL (United States); STFC Rutherford Appleton Lab., Didcot (United Kingdom). ISIS Neutron and Muon Facility
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Cambridge (United Kingdom); Nanjing Univ. of Information Science and Technology (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Engineering and Physical Sciences Research Council (EPSRC); Nanjing Univ. of Information Science and Technology (China)
Contributing Org.:
STFC Rutherford Appleton Lab., Didcot (United Kingdom)
OSTI Identifier:
1352676
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 18; Journal Issue: 28; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 14 SOLAR ENERGY; Azo; DFT; Dye-sensitized solar cell; Nitro; Optoelectric material; TDDFT

Citation Formats

Zhang, Lei, and Cole, Jacqueline M. Can nitro groups really anchor onto TiO2? Case study of dye-to-TiO2 adsorption using azo dyes with NO2 substituents. United States: N. p., 2016. Web. https://doi.org/10.1039/c6cp02294d.
Zhang, Lei, & Cole, Jacqueline M. Can nitro groups really anchor onto TiO2? Case study of dye-to-TiO2 adsorption using azo dyes with NO2 substituents. United States. https://doi.org/10.1039/c6cp02294d
Zhang, Lei, and Cole, Jacqueline M. Tue . "Can nitro groups really anchor onto TiO2? Case study of dye-to-TiO2 adsorption using azo dyes with NO2 substituents". United States. https://doi.org/10.1039/c6cp02294d. https://www.osti.gov/servlets/purl/1352676.
@article{osti_1352676,
title = {Can nitro groups really anchor onto TiO2? Case study of dye-to-TiO2 adsorption using azo dyes with NO2 substituents},
author = {Zhang, Lei and Cole, Jacqueline M.},
abstractNote = {The nitro group has recently been suggested as a new type of anchor for dye-sensitized solar cells (DSSCs) and has shown promising optoelectronic properties. Considering the excellent electron withdrawing ability of the nitro group and wider materials selection brought about by this substituent, it is helpful to evaluate the interfacial structures and photophysics of more organic dyes where NO2 poses as the dye-to-TiO2 anchor. A computational study on a family of azo dyes bearing a nitro group is presented in this paper, where the effect of certain side groups on their optical properties is examined. Both isolated dye molecules and dye/TiO2 nanocomposites are studied via density functional theory and time-dependent density functional theory, with complementary experimental UV/vis absorption spectroscopy and photovoltaic device testing. Results demonstrate that these nitro-containing dyes prefer a monodentate anchoring mode on a TiO2 cluster. These nitro dyes reveal weak, but non-negligible, adsorption onto TiO2; yet, very low photovoltaic performance once incorporated into a DSSC device. Finally, this poor delivery of nitro groups as DSSC anchors is ostensibly inconsistent with previous findings; but is rationalized via the “auxiliary anchor” concept.},
doi = {10.1039/c6cp02294d},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 28,
volume = 18,
place = {United States},
year = {2016},
month = {6}
}

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