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Title: Organic pollutant photodecomposition by Ag/KNbO3 nanocomposites: A combined experimental and theoretical study

Abstract

In this study, Ag nanoparticles supported on well-defined perovskite orthorhombic KNbO3 nanowires are synthesized via facile photoreduction and systematically characterized by XRD, Raman, DRUV–vis, XPS, PL, TEM, HRTEM, and HAADF-STEM. The photoreactivity of Ag/KNbO3 nanocomposites as a function of Ag contents (0.4–2.8 wt %) is assessed toward aqueous rhodamine B degradation under UV- and visible-light, respectively. It is found that the UV-induced photoreactivity initially increases and then decreases with increasing Ag contents. At an optimal Ag content (ca. 1.7 wt %), the greatest photoreactivity is achieved under UV light, with the photocatalytic reaction rate of 1.7 wt % Ag/KNbO3 exceeding that of pristine KNbO3 by a factor of ca. 13. In contrast, visible light-induced photoreactivity monotonically increases with increasing Ag contents in the range of 0.4–2.8 wt %. On the basis of the detected active species and intermediate products in the photocatalytic processes, conjugated structure cleavage and N-deethylation are revealed to be the respective predominant pathway under UV and visible-light illumination. To gain an insight into the observed photoreactivity, the electronic properties of Ag/KNbO3 have been investigated using spin-polarized DFT calculations. Herein, Ag extended adlayers (1–4 ML) on the slab models of KNbO3 (101) are employed to mimic large supportedmore » Ag nanoparticles. A Bader analysis of the electron density shows a small net charge transfer (ca. 0.1 e) from KNbO3 to Ag. The electron localization function of Ag/KNbO3 (101) illustrates that Ag adlayers with thickness larger than 2 ML are essentially metallic, and weak polarization occurs at the interface. In addition, the metallic Ag adlayers generate a continuum of Ag bandgap states, which play a key role in determining different Ag content-dependent behavior between UV and visible-light illumination.« less

Authors:
 [1];  [2];  [3];  [2];  [4];  [5];  [3];  [3]
+ Show Author Affiliations
  1. Northeastern Univ., Shenyang (China); National Center for Nanoscience and Technology, Beijing (China)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. National Center for Nanoscience and Technology, Beijing (China)
  4. Wuhan Univ. of Technology, Wuhan (China)
  5. Northeastern Univ., Shenyang (China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1247985
Report Number(s):
BNL-112078-2016-JA
Journal ID: ISSN 1932-7447; R&D Project: CO009; KC0302010
Grant/Contract Number:  
SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 120; Journal Issue: 5; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nanocomposites; localized surface plasmon resonance; photocatalysis; potassium niobate; silver

Citation Formats

Zhang, Tingting, Liu, Ping, Lei, Wanying, Rodriguez, J. A., Yu, Jiaguo, Qi, Yang, Liu, Gang, and Liu, Minghua. Organic pollutant photodecomposition by Ag/KNbO3 nanocomposites: A combined experimental and theoretical study. United States: N. p., 2016. Web. doi:10.1021/acs.jpcc.5b11297.
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Zhang, Tingting, Liu, Ping, Lei, Wanying, Rodriguez, J. A., Yu, Jiaguo, Qi, Yang, Liu, Gang, & Liu, Minghua. Organic pollutant photodecomposition by Ag/KNbO3 nanocomposites: A combined experimental and theoretical study. United States. https://doi.org/10.1021/acs.jpcc.5b11297
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Zhang, Tingting, Liu, Ping, Lei, Wanying, Rodriguez, J. A., Yu, Jiaguo, Qi, Yang, Liu, Gang, and Liu, Minghua. Tue . "Organic pollutant photodecomposition by Ag/KNbO3 nanocomposites: A combined experimental and theoretical study". United States. https://doi.org/10.1021/acs.jpcc.5b11297. https://www.osti.gov/servlets/purl/1247985.
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@article{osti_1247985,
title = {Organic pollutant photodecomposition by Ag/KNbO3 nanocomposites: A combined experimental and theoretical study},
author = {Zhang, Tingting and Liu, Ping and Lei, Wanying and Rodriguez, J. A. and Yu, Jiaguo and Qi, Yang and Liu, Gang and Liu, Minghua},
abstractNote = {In this study, Ag nanoparticles supported on well-defined perovskite orthorhombic KNbO3 nanowires are synthesized via facile photoreduction and systematically characterized by XRD, Raman, DRUV–vis, XPS, PL, TEM, HRTEM, and HAADF-STEM. The photoreactivity of Ag/KNbO3 nanocomposites as a function of Ag contents (0.4–2.8 wt %) is assessed toward aqueous rhodamine B degradation under UV- and visible-light, respectively. It is found that the UV-induced photoreactivity initially increases and then decreases with increasing Ag contents. At an optimal Ag content (ca. 1.7 wt %), the greatest photoreactivity is achieved under UV light, with the photocatalytic reaction rate of 1.7 wt % Ag/KNbO3 exceeding that of pristine KNbO3 by a factor of ca. 13. In contrast, visible light-induced photoreactivity monotonically increases with increasing Ag contents in the range of 0.4–2.8 wt %. On the basis of the detected active species and intermediate products in the photocatalytic processes, conjugated structure cleavage and N-deethylation are revealed to be the respective predominant pathway under UV and visible-light illumination. To gain an insight into the observed photoreactivity, the electronic properties of Ag/KNbO3 have been investigated using spin-polarized DFT calculations. Herein, Ag extended adlayers (1–4 ML) on the slab models of KNbO3 (101) are employed to mimic large supported Ag nanoparticles. A Bader analysis of the electron density shows a small net charge transfer (ca. 0.1 e) from KNbO3 to Ag. The electron localization function of Ag/KNbO3 (101) illustrates that Ag adlayers with thickness larger than 2 ML are essentially metallic, and weak polarization occurs at the interface. In addition, the metallic Ag adlayers generate a continuum of Ag bandgap states, which play a key role in determining different Ag content-dependent behavior between UV and visible-light illumination.},
doi = {10.1021/acs.jpcc.5b11297},
journal = {Journal of Physical Chemistry. C},
number = 5,
volume = 120,
place = {United States},
year = {Tue Jan 12 00:00:00 EST 2016},
month = {Tue Jan 12 00:00:00 EST 2016}
}
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