{"title":"通过可回收氧化还原循环利用乙醇生产乙烯的 CuCl2/FeCl3 双金属光催化剂","authors":"Shuang Xu, Mingjie Li*, Biao Zhou, Chenghao Duan, Feilin Zou, Shibing Zou, Xia Long, Guangxu Chen and Keyou Yan*, ","doi":"10.1021/acs.jpclett.4c00588","DOIUrl":null,"url":null,"abstract":"<p >Photocatalytic conversions of ethanol to valuable chemicals are significant organic synthesis reactions. Herein, we developed a CuCl<sub>2</sub>/FeCl<sub>3</sub> bimetallic photocatalyst for sustainable dehydration of ethanol to ethylene by recoverable redox cycles. The selectivity of ethylene was 98.3% for CuCl<sub>2</sub>/FeCl<sub>3</sub>, which is much higher than that of CuCl<sub>2</sub> (34.5%) and FeCl<sub>3</sub> (86.5%). Due to the ligand-to-metal charge transfer (LMCT) process involved in generating the liquid products, the CuCl<sub>2</sub>/FeCl<sub>3</sub> catalyst will be reduced to CuCl/FeCl<sub>2</sub>. Oxygen (O<sub>2</sub>) is required for the recovery of CuCl<sub>2</sub>/FeCl<sub>3</sub> to avoid exhaustion. The soluble Fe<sup>3+</sup>/Fe<sup>2+</sup> redox species deliver catalyst regeneration properties more efficiently than single metal couples, making a series of redox reactions (Cu<sup>2+</sup>/Cu<sup>+</sup>, Fe<sup>3+</sup>/Fe<sup>2+</sup>, and O<sub>2</sub>/ethanol couples) recyclable with synergistic effects. A flow reactor was designed to facilitate the continuous production of ethylene. The understanding of bimetallic synergism and consecutive reactions promotes the industrial application process of photocatalytic organic reactions.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 17","pages":"4640–4646"},"PeriodicalIF":4.6000,"publicationDate":"2024-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"CuCl2/FeCl3 Bimetallic Photocatalyst for Sustainable Ethylene Production from Ethanol via Recoverable Redox Cycles\",\"authors\":\"Shuang Xu, Mingjie Li*, Biao Zhou, Chenghao Duan, Feilin Zou, Shibing Zou, Xia Long, Guangxu Chen and Keyou Yan*, \",\"doi\":\"10.1021/acs.jpclett.4c00588\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Photocatalytic conversions of ethanol to valuable chemicals are significant organic synthesis reactions. Herein, we developed a CuCl<sub>2</sub>/FeCl<sub>3</sub> bimetallic photocatalyst for sustainable dehydration of ethanol to ethylene by recoverable redox cycles. The selectivity of ethylene was 98.3% for CuCl<sub>2</sub>/FeCl<sub>3</sub>, which is much higher than that of CuCl<sub>2</sub> (34.5%) and FeCl<sub>3</sub> (86.5%). Due to the ligand-to-metal charge transfer (LMCT) process involved in generating the liquid products, the CuCl<sub>2</sub>/FeCl<sub>3</sub> catalyst will be reduced to CuCl/FeCl<sub>2</sub>. Oxygen (O<sub>2</sub>) is required for the recovery of CuCl<sub>2</sub>/FeCl<sub>3</sub> to avoid exhaustion. The soluble Fe<sup>3+</sup>/Fe<sup>2+</sup> redox species deliver catalyst regeneration properties more efficiently than single metal couples, making a series of redox reactions (Cu<sup>2+</sup>/Cu<sup>+</sup>, Fe<sup>3+</sup>/Fe<sup>2+</sup>, and O<sub>2</sub>/ethanol couples) recyclable with synergistic effects. A flow reactor was designed to facilitate the continuous production of ethylene. The understanding of bimetallic synergism and consecutive reactions promotes the industrial application process of photocatalytic organic reactions.</p>\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"15 17\",\"pages\":\"4640–4646\"},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2024-04-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpclett.4c00588\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpclett.4c00588","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
CuCl2/FeCl3 Bimetallic Photocatalyst for Sustainable Ethylene Production from Ethanol via Recoverable Redox Cycles
Photocatalytic conversions of ethanol to valuable chemicals are significant organic synthesis reactions. Herein, we developed a CuCl2/FeCl3 bimetallic photocatalyst for sustainable dehydration of ethanol to ethylene by recoverable redox cycles. The selectivity of ethylene was 98.3% for CuCl2/FeCl3, which is much higher than that of CuCl2 (34.5%) and FeCl3 (86.5%). Due to the ligand-to-metal charge transfer (LMCT) process involved in generating the liquid products, the CuCl2/FeCl3 catalyst will be reduced to CuCl/FeCl2. Oxygen (O2) is required for the recovery of CuCl2/FeCl3 to avoid exhaustion. The soluble Fe3+/Fe2+ redox species deliver catalyst regeneration properties more efficiently than single metal couples, making a series of redox reactions (Cu2+/Cu+, Fe3+/Fe2+, and O2/ethanol couples) recyclable with synergistic effects. A flow reactor was designed to facilitate the continuous production of ethylene. The understanding of bimetallic synergism and consecutive reactions promotes the industrial application process of photocatalytic organic reactions.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.