{"title":"Enhanced photocatalytic phenol production from benzene on polymers with coordinatively unsaturated Fe centers","authors":"Bo Wang , Peng Li , Zongbo Xie , Zhanggao Le","doi":"10.1016/j.jphotochem.2024.116123","DOIUrl":null,"url":null,"abstract":"<div><div>The photocatalytic hydroxylation of benzene to phenol using low-cost Fe-based materials is of great significance but remains a great challenge for the conversion of benzene in an efficient manner. Here we report a novel method to construct polymeric Fe-BTC-350 with highly dispersed coordinatively unsaturated (CUS) Fe centers by a simple pyrolysis of iron benzene tricarboxylic acid (Fe-BTC) coordination polymer. The CUS Fe centers in Fe-BTC-350 function as Lewis acid sites to accept both electrons and hydroxyl radicals, thus enhancing photocatalytic phenol generation. An optimal phenol yield of 22.7 % has been achieved over optimized Fe-BTC-350 which is 2.8 times that of the Fe-BTC. No evident decay in the activity was found after 4 cycles of consecutive reactions, indicating the robust stability of the photocatalyst. It is expected that the construction of CUS transition metal centers can also be utilized for other photocatalytic radical reactions.</div></div>","PeriodicalId":16782,"journal":{"name":"Journal of Photochemistry and Photobiology A-chemistry","volume":"460 ","pages":"Article 116123"},"PeriodicalIF":4.1000,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Photochemistry and Photobiology A-chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1010603024006671","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The photocatalytic hydroxylation of benzene to phenol using low-cost Fe-based materials is of great significance but remains a great challenge for the conversion of benzene in an efficient manner. Here we report a novel method to construct polymeric Fe-BTC-350 with highly dispersed coordinatively unsaturated (CUS) Fe centers by a simple pyrolysis of iron benzene tricarboxylic acid (Fe-BTC) coordination polymer. The CUS Fe centers in Fe-BTC-350 function as Lewis acid sites to accept both electrons and hydroxyl radicals, thus enhancing photocatalytic phenol generation. An optimal phenol yield of 22.7 % has been achieved over optimized Fe-BTC-350 which is 2.8 times that of the Fe-BTC. No evident decay in the activity was found after 4 cycles of consecutive reactions, indicating the robust stability of the photocatalyst. It is expected that the construction of CUS transition metal centers can also be utilized for other photocatalytic radical reactions.
期刊介绍：
JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds.
All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor).
The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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