Enhanced photocatalytic phenol production from benzene on polymers with coordinatively unsaturated Fe centers

IF 4.1 3区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2024-10-29 DOI:10.1016/j.jphotochem.2024.116123

Bo Wang , Peng Li , Zongbo Xie , Zhanggao Le

{"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.

Abstract Image

查看原文本刊更多论文

在具有配位不饱和铁中心的聚合物上增强苯的光催化苯酚生产

使用低成本的铁基材料进行苯到苯酚的光催化羟基化具有重要意义，但对于苯的高效转化仍是一个巨大挑战。在此，我们报告了一种新方法，即通过简单热解苯三羧酸铁（Fe-BTC）配位聚合物，构建具有高度分散的配位不饱和（CUS）铁中心的聚合物 Fe-BTC-350。Fe-BTC-350 中的 CUS Fe 中心具有路易斯酸位点的功能，可以接受电子和羟基自由基，从而提高光催化苯酚的生成。经过优化的 Fe-BTC-350 的最佳苯酚产量为 22.7%，是 Fe-BTC 的 2.8 倍。连续反应 4 个周期后，活性没有明显下降，这表明光催化剂具有很强的稳定性。预计 CUS 过渡金属中心的构建还可用于其他光催化自由基反应。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of Photochemistry and Photobiology A-chemistry 化学-物理化学

CiteScore

7.90

自引率

7.00%

发文量

580

审稿时长

48 days

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.