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 »
- Authors:
-
- Northeastern Univ., Shenyang (China); National Center for Nanoscience and Technology, Beijing (China)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- National Center for Nanoscience and Technology, Beijing (China)
- Wuhan Univ. of Technology, Wuhan (China)
- 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.
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
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.
@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}
}
Web of Science
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