Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides

A zirconium-based metal-organic framework (MOF) was successfully constructed via solvothermal assembly of a triphenylamine-based tricarboxylate ligand and Zr(IV) salt, the structure simulation of which revealed that it possesses a two-dimensional layered framework with a relatively rare dodecnuclear...

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Main Authors: Zou, Xin-Nan, Zhang, Deshan, Luan, Tian-Xiang, Li, Qiang, Li, Lei, Li, Pei-Zhou, Zhao, Yanli
Other Authors: School of Physical and Mathematical Sciences
Format: Article
Language:English
Published: 2022
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Online Access:https://hdl.handle.net/10356/160095
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1600952022-07-12T08:50:53Z Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides Zou, Xin-Nan Zhang, Deshan Luan, Tian-Xiang Li, Qiang Li, Lei Li, Pei-Zhou Zhao, Yanli School of Physical and Mathematical Sciences Science::Chemistry Aerobic Oxidation Metal-Organic Frameworks A zirconium-based metal-organic framework (MOF) was successfully constructed via solvothermal assembly of a triphenylamine-based tricarboxylate ligand and Zr(IV) salt, the structure simulation of which revealed that it possesses a two-dimensional layered framework with a relatively rare dodecnuclear Zr12 cluster as the inorganic building unit. The inherent photo-responsive property derived from the incorporated photochromic triphenylamine groups combined with its high stability makes the constructed MOF an efficient heterogeneous photocatalyst for the oxidation of sulfides, which is a fundamentally important reaction type in both environmental and pharmaceutical industries. The photocatalytic activity of the constructed MOF was first investigated under various conditions with thioanisole as a representative sulfide substrate. The MOF exhibited both high efficiency and selectivity on aerobic oxidation of thioanisole in methanol utilizing molecular oxygen in air as the oxidant under blue light irradiation for 10 h. Its high photocatalytic performance was also observed when extending the sulfide substrate to diverse thioanisole derivatives and even a sulfur-containing nerve agent simulant (2-chloroethyl ethyl sulfide). The high photocatalytic efficiency and selectivity to a broad set of sulfide substrates make the triphenylamine-incorporating zirconium-based MOF a highly promising heterogeneous photocatalyst. Ministry of Education (MOE) This work was supported by the "Qilu Young Talent Scholar" program of Shandong University and the Singapore Academic Research Fund (RT12/19). 2022-07-12T08:50:53Z 2022-07-12T08:50:53Z 2021 Journal Article Zou, X., Zhang, D., Luan, T., Li, Q., Li, L., Li, P. & Zhao, Y. (2021). Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides. ACS Applied Materials and Interfaces, 13(17), 20137-20144. https://dx.doi.org/10.1021/acsami.1c03083 1944-8244 https://hdl.handle.net/10356/160095 10.1021/acsami.1c03083 33886272 2-s2.0-85106143445 17 13 20137 20144 en RT12/19 ACS Applied Materials and Interfaces © 2021 American Chemical Society. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Chemistry
Aerobic Oxidation
Metal-Organic Frameworks
spellingShingle Science::Chemistry
Aerobic Oxidation
Metal-Organic Frameworks
Zou, Xin-Nan
Zhang, Deshan
Luan, Tian-Xiang
Li, Qiang
Li, Lei
Li, Pei-Zhou
Zhao, Yanli
Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides
description A zirconium-based metal-organic framework (MOF) was successfully constructed via solvothermal assembly of a triphenylamine-based tricarboxylate ligand and Zr(IV) salt, the structure simulation of which revealed that it possesses a two-dimensional layered framework with a relatively rare dodecnuclear Zr12 cluster as the inorganic building unit. The inherent photo-responsive property derived from the incorporated photochromic triphenylamine groups combined with its high stability makes the constructed MOF an efficient heterogeneous photocatalyst for the oxidation of sulfides, which is a fundamentally important reaction type in both environmental and pharmaceutical industries. The photocatalytic activity of the constructed MOF was first investigated under various conditions with thioanisole as a representative sulfide substrate. The MOF exhibited both high efficiency and selectivity on aerobic oxidation of thioanisole in methanol utilizing molecular oxygen in air as the oxidant under blue light irradiation for 10 h. Its high photocatalytic performance was also observed when extending the sulfide substrate to diverse thioanisole derivatives and even a sulfur-containing nerve agent simulant (2-chloroethyl ethyl sulfide). The high photocatalytic efficiency and selectivity to a broad set of sulfide substrates make the triphenylamine-incorporating zirconium-based MOF a highly promising heterogeneous photocatalyst.
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Zou, Xin-Nan
Zhang, Deshan
Luan, Tian-Xiang
Li, Qiang
Li, Lei
Li, Pei-Zhou
Zhao, Yanli
format Article
author Zou, Xin-Nan
Zhang, Deshan
Luan, Tian-Xiang
Li, Qiang
Li, Lei
Li, Pei-Zhou
Zhao, Yanli
author_sort Zou, Xin-Nan
title Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides
title_short Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides
title_full Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides
title_fullStr Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides
title_full_unstemmed Incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides
title_sort incorporating photochromic triphenylamine into a zirconium-organic framework for highly effective photocatalytic aerobic oxidation of sulfides
publishDate 2022
url https://hdl.handle.net/10356/160095
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