Sohaib Hameed , Wengang Liu , Zhounan Yu , Jifeng Pang , Wenhao Luo , Aiqin Wang
{"title":"在铁单原子催化剂上将 5-羟甲基糠醛无碱有氧氧化为 2,5-呋喃二羧酸†。","authors":"Sohaib Hameed , Wengang Liu , Zhounan Yu , Jifeng Pang , Wenhao Luo , Aiqin Wang","doi":"10.1039/d4gc01777c","DOIUrl":null,"url":null,"abstract":"<div><p>2,5-Furandicarboxylic acid (FDCA) is one of the most promising biodegradable substitutes for fossil-derived terephthalic acid (PTA) and adipic acid. The production of FDCA from biomass-derived 5-hydroxymethylfurfural (HMF) is significant and has attracted great attention. However, the major challenge lies in the development of a non-precious metal-based catalyst system without employing a homogeneous base. Herein, we successfully prepared an atomically dispersed Fe–N–C/γ-Al<sub>2</sub>O<sub>3</sub> catalyst, which affords superior catalytic performance in terms of activity and stability with a FDCA yield of 99.8% and reusability of five recycle times in the catalytic oxidation of HMF to FDCA under base-free mild conditions. Based on controlled experiments and complementary characterization studies, we found that the atomically dispersed medium-spin Fe–N<sub>5</sub> active sites together with the surface acidic/basic sites of alumina synergistically enhanced the catalytic activity and selectivity towards FDCA under base-free conditions. Our process eliminates the employment of expensive oxidants and corrosive bases, leading to economic and green biomass transformations.</p></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.3000,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over a Fe single-atom catalyst†\",\"authors\":\"Sohaib Hameed , Wengang Liu , Zhounan Yu , Jifeng Pang , Wenhao Luo , Aiqin Wang\",\"doi\":\"10.1039/d4gc01777c\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>2,5-Furandicarboxylic acid (FDCA) is one of the most promising biodegradable substitutes for fossil-derived terephthalic acid (PTA) and adipic acid. The production of FDCA from biomass-derived 5-hydroxymethylfurfural (HMF) is significant and has attracted great attention. However, the major challenge lies in the development of a non-precious metal-based catalyst system without employing a homogeneous base. Herein, we successfully prepared an atomically dispersed Fe–N–C/γ-Al<sub>2</sub>O<sub>3</sub> catalyst, which affords superior catalytic performance in terms of activity and stability with a FDCA yield of 99.8% and reusability of five recycle times in the catalytic oxidation of HMF to FDCA under base-free mild conditions. Based on controlled experiments and complementary characterization studies, we found that the atomically dispersed medium-spin Fe–N<sub>5</sub> active sites together with the surface acidic/basic sites of alumina synergistically enhanced the catalytic activity and selectivity towards FDCA under base-free conditions. Our process eliminates the employment of expensive oxidants and corrosive bases, leading to economic and green biomass transformations.</p></div>\",\"PeriodicalId\":78,\"journal\":{\"name\":\"Green Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.3000,\"publicationDate\":\"2024-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Green Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/org/science/article/pii/S1463926224005958\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Green Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/org/science/article/pii/S1463926224005958","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid over a Fe single-atom catalyst†
2,5-Furandicarboxylic acid (FDCA) is one of the most promising biodegradable substitutes for fossil-derived terephthalic acid (PTA) and adipic acid. The production of FDCA from biomass-derived 5-hydroxymethylfurfural (HMF) is significant and has attracted great attention. However, the major challenge lies in the development of a non-precious metal-based catalyst system without employing a homogeneous base. Herein, we successfully prepared an atomically dispersed Fe–N–C/γ-Al2O3 catalyst, which affords superior catalytic performance in terms of activity and stability with a FDCA yield of 99.8% and reusability of five recycle times in the catalytic oxidation of HMF to FDCA under base-free mild conditions. Based on controlled experiments and complementary characterization studies, we found that the atomically dispersed medium-spin Fe–N5 active sites together with the surface acidic/basic sites of alumina synergistically enhanced the catalytic activity and selectivity towards FDCA under base-free conditions. Our process eliminates the employment of expensive oxidants and corrosive bases, leading to economic and green biomass transformations.
期刊介绍:
Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.