Runzi Cao , Heng Shao , Xinjie Wang , Jian Wang , Enxiang Shang , Yang Li
{"title":"Nb2O5/GCN异质结催化剂光催化可降解PBAT制备高附加值燃料:性能与机理","authors":"Runzi Cao , Heng Shao , Xinjie Wang , Jian Wang , Enxiang Shang , Yang Li","doi":"10.1016/j.cclet.2025.111029","DOIUrl":null,"url":null,"abstract":"<div><div>Photocatalysis holds great promise for the conversion of plastic waste into valuable chemicals. However, the conversion efficiency is constrained by the poor carriers' separation efficiency over the single component photocatalyst. Herein, we synthesized a novel type Ⅱ Nb<sub>2</sub>O<sub>5</sub>/GCN heterojunction to investigate its efficiency in the photocatalytic upcycling of polybutylene adipate/terephthalate (PBAT) microplastics (MPs) into acids and alcohols under visible light irradiation (100 mW/cm2). The findings indicate that the charge transfer within the type Ⅱ Nb<sub>2</sub>O<sub>5</sub>/GCN occurs from the conduction band of GCN to the conduction band of Nb<sub>2</sub>O<sub>5</sub>, thereby enhancing the separation efficiency of carriers Notably, the rates of ethanol and acetic acid generation from 1.5 mg/mL PBAT MPs treated with the 60 %Nb<sub>2</sub>O<sub>5</sub>/GCN photocatalyst were 21.8-fold and 1.8-fold higher, respectively, compared to those by Nb<sub>2</sub>O<sub>5</sub> alone. Density functional theory calculations demonstrate that the hydroxyl radicals (<sup>•</sup>OH) produced by the Nb<sub>2</sub>O<sub>5</sub>/GCN heterojunction cleaves the ester bond (O<img>C=O) of PBAT MP into the monomer. These monomers are subsequently converted into acids and alcohols through various reactions, including C<img>C bond cleavage, hydrodeoxygenation, and C<img>C bond coupling. This study highlights the effectiveness of heterojunction photocatalyst in converting PBAT MPs into valuable chemicals, thus significantly promoting advancements in bioplastics recycling.</div></div>","PeriodicalId":10088,"journal":{"name":"Chinese Chemical Letters","volume":"36 7","pages":"Article 111029"},"PeriodicalIF":9.4000,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Photocatalytic production of high-value-added fuels from biodegradable PBAT by Nb2O5/GCN heterojunction catalyst: Performance and mechanism\",\"authors\":\"Runzi Cao , Heng Shao , Xinjie Wang , Jian Wang , Enxiang Shang , Yang Li\",\"doi\":\"10.1016/j.cclet.2025.111029\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Photocatalysis holds great promise for the conversion of plastic waste into valuable chemicals. However, the conversion efficiency is constrained by the poor carriers' separation efficiency over the single component photocatalyst. Herein, we synthesized a novel type Ⅱ Nb<sub>2</sub>O<sub>5</sub>/GCN heterojunction to investigate its efficiency in the photocatalytic upcycling of polybutylene adipate/terephthalate (PBAT) microplastics (MPs) into acids and alcohols under visible light irradiation (100 mW/cm2). The findings indicate that the charge transfer within the type Ⅱ Nb<sub>2</sub>O<sub>5</sub>/GCN occurs from the conduction band of GCN to the conduction band of Nb<sub>2</sub>O<sub>5</sub>, thereby enhancing the separation efficiency of carriers Notably, the rates of ethanol and acetic acid generation from 1.5 mg/mL PBAT MPs treated with the 60 %Nb<sub>2</sub>O<sub>5</sub>/GCN photocatalyst were 21.8-fold and 1.8-fold higher, respectively, compared to those by Nb<sub>2</sub>O<sub>5</sub> alone. Density functional theory calculations demonstrate that the hydroxyl radicals (<sup>•</sup>OH) produced by the Nb<sub>2</sub>O<sub>5</sub>/GCN heterojunction cleaves the ester bond (O<img>C=O) of PBAT MP into the monomer. These monomers are subsequently converted into acids and alcohols through various reactions, including C<img>C bond cleavage, hydrodeoxygenation, and C<img>C bond coupling. This study highlights the effectiveness of heterojunction photocatalyst in converting PBAT MPs into valuable chemicals, thus significantly promoting advancements in bioplastics recycling.</div></div>\",\"PeriodicalId\":10088,\"journal\":{\"name\":\"Chinese Chemical Letters\",\"volume\":\"36 7\",\"pages\":\"Article 111029\"},\"PeriodicalIF\":9.4000,\"publicationDate\":\"2025-03-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Chemical Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1001841725002153\",\"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":"Chinese Chemical Letters","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1001841725002153","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Photocatalytic production of high-value-added fuels from biodegradable PBAT by Nb2O5/GCN heterojunction catalyst: Performance and mechanism
Photocatalysis holds great promise for the conversion of plastic waste into valuable chemicals. However, the conversion efficiency is constrained by the poor carriers' separation efficiency over the single component photocatalyst. Herein, we synthesized a novel type Ⅱ Nb2O5/GCN heterojunction to investigate its efficiency in the photocatalytic upcycling of polybutylene adipate/terephthalate (PBAT) microplastics (MPs) into acids and alcohols under visible light irradiation (100 mW/cm2). The findings indicate that the charge transfer within the type Ⅱ Nb2O5/GCN occurs from the conduction band of GCN to the conduction band of Nb2O5, thereby enhancing the separation efficiency of carriers Notably, the rates of ethanol and acetic acid generation from 1.5 mg/mL PBAT MPs treated with the 60 %Nb2O5/GCN photocatalyst were 21.8-fold and 1.8-fold higher, respectively, compared to those by Nb2O5 alone. Density functional theory calculations demonstrate that the hydroxyl radicals (•OH) produced by the Nb2O5/GCN heterojunction cleaves the ester bond (OC=O) of PBAT MP into the monomer. These monomers are subsequently converted into acids and alcohols through various reactions, including CC bond cleavage, hydrodeoxygenation, and CC bond coupling. This study highlights the effectiveness of heterojunction photocatalyst in converting PBAT MPs into valuable chemicals, thus significantly promoting advancements in bioplastics recycling.
期刊介绍:
Chinese Chemical Letters (CCL) (ISSN 1001-8417) was founded in July 1990. The journal publishes preliminary accounts in the whole field of chemistry, including inorganic chemistry, organic chemistry, analytical chemistry, physical chemistry, polymer chemistry, applied chemistry, etc.Chinese Chemical Letters does not accept articles previously published or scheduled to be published. To verify originality, your article may be checked by the originality detection service CrossCheck.