Photoactive Ag(I)-based coordination polymer as a potential semiconductor for photocatalytic water splitting and environmental remediation: experimental and theoretical approach

Mandal, Subrata, Nanavati, Sachin P. ORCID: https://orcid.org/0000-0002-5525-4329, Willock, David J. ORCID: https://orcid.org/0000-0002-8893-1090 and Ananthakrishnan, Rajakumar 2019. Photoactive Ag(I)-based coordination polymer as a potential semiconductor for photocatalytic water splitting and environmental remediation: experimental and theoretical approach. Journal of Physical Chemistry C 123 (39) , pp. 23940-23950. 10.1021/acs.jpcc.9b04957

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Abstract

Metal–organic frameworks or metal coordination polymers (CPs) with controlled structure on the micro/nanoscale have attracted intense interest for potential applications in a wide variety of fields, such as energy storage and conversion, chemical and biological sensing, and catalysis. Here, we report a new class of photocatalytic material, Ag(I)-based nano-micro-structured coordination polymer (Ag(I)-CP), which offers performance at a level competitive with known semiconductors in photocatalytic water oxidation and oxidation of organic compounds, such as dye/organic pollutants present in contaminated water. The coordination polymer was synthesized by a wet-chemical route and has been characterized using powder X-ray diffraction, X-ray photoelectron spectroscopy, and electron microscopy. The Ag(I)-CP has notable semiconducting characteristics and charge transfer ability due to ligand-centered charge transfer in combination with metal-to-ligand charge transfer (Ag–O cluster to ligand center), as established from experimental absorption, luminescence, and photoelectrochemical measurements alongside density functional theory calculations. Notably, Ag(I)-CP exhibits a highly reactive valance band potential +3.40 V vs NHE, composed of hybridized state of O 2p and C 2p through the organic linker and Ag 4d; this acts as an active center for the generation of reactive oxygen species, i.e., hydroxyl radical and h+ under photocatalytic conditions. Consequently, the photogenerated species facilitate effective oxidations of water and organic contaminants such as tartrazine, rhodamine B, and 2,4-dichlorophenol under UV light irradiation. Furthermore, our results suggest that the Ag(I)-CP could be used as a promising material for the development of heterostructure for a variety of photoassisted redox catalysis reactions.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Advanced Research Computing @ Cardiff (ARCCA) Chemistry
Publisher:	American Chemical Society
ISSN:	1932-7447
Date of First Compliant Deposit:	1 October 2019
Date of Acceptance:	28 August 2019
Last Modified:	06 Nov 2023 21:13
URI:	https://orca.cardiff.ac.uk/id/eprint/125824

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