{"title":"增强无金属供体-受体共轭光催化剂的内电场以实现四环素的高效光催化降解和二氧化碳还原","authors":"Guangyu Wu, Geng Li, Yonggong Tang, Guoyu Tai, Yuwei Pan, Jiangang Han, Weinan Xing","doi":"10.1021/acs.langmuir.4c03632","DOIUrl":null,"url":null,"abstract":"<p><p>Constructing alternating donor-acceptor (D-A) units within g-C<sub>3</sub>N<sub>4</sub> represents an effective strategy for enhancing photocatalytic performance through improved charge carrier separation while concurrently addressing energy shortages and facilitating wastewater remediation. Here, a series of D-A-type conjugated photocatalysts (CNBTC-X) are prepared using g-C<sub>3</sub>N<sub>4</sub> as an acceptor unit and different masses of 5-bromo-2-thiophenecarboxaldehyde (BTC) as a donor unit by a one-step thermal polymerization. CNBTC-50 presents higher photocatalytic properties for CO<sub>2</sub> reduction coupled with tetracycline (TC) removal than those of g-C<sub>3</sub>N<sub>4</sub>, CNBTC-10, CNBTC-30, and CNBTC-70. The introduction of the unique electron-donor-acceptor structure effectively drives the separation and transfer of photoinduced carriers while reducing the internal carrier transfer hindrance. Photocatalytic experiments reveal that the CNBTC-50 photocatalyst achieves up to 94.6% TC removal under visible light irradiation conditions. Compared with that of the pristine g-C<sub>3</sub>N<sub>4</sub>, the photocatalytic degradation reaction rate constant of CNBTC-50 is significantly increased by about 3.87 times. The study examines the influence of various reaction parameters on degradation activity, including catalyst concentration, pH, and TC concentration. Additionally, LC-MS is utilized to perform a comprehensive analysis of the intermediates and pathways involved in TC degradation. Furthermore, CNBTC-50 demonstrates remarkable photocatalytic CO<sub>2</sub> reduction activity, achieving rates of 20.83 μmol g<sup>-1</sup> h<sup>-1</sup> (CO) and 9.36 μmol g<sup>-1</sup> h<sup>-1</sup> (CH<sub>4</sub>), which are 10.68 and 5.98 times more efficient than those of g-C<sub>3</sub>N<sub>4</sub>, respectively. This work aims to offer valuable guidance for the rational design of nonmetal D-A-structured catalysts and effectively integrates reaction systems to couple CO<sub>2</sub> reduction with antibiotic removal.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":" ","pages":""},"PeriodicalIF":3.7000,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing Internal Electric Field of Metal-Free Donor-Acceptor Conjugated Photocatalysts for Efficient Photocatalytic Degradation of Tetracycline and CO<sub>2</sub> Reduction.\",\"authors\":\"Guangyu Wu, Geng Li, Yonggong Tang, Guoyu Tai, Yuwei Pan, Jiangang Han, Weinan Xing\",\"doi\":\"10.1021/acs.langmuir.4c03632\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Constructing alternating donor-acceptor (D-A) units within g-C<sub>3</sub>N<sub>4</sub> represents an effective strategy for enhancing photocatalytic performance through improved charge carrier separation while concurrently addressing energy shortages and facilitating wastewater remediation. Here, a series of D-A-type conjugated photocatalysts (CNBTC-X) are prepared using g-C<sub>3</sub>N<sub>4</sub> as an acceptor unit and different masses of 5-bromo-2-thiophenecarboxaldehyde (BTC) as a donor unit by a one-step thermal polymerization. CNBTC-50 presents higher photocatalytic properties for CO<sub>2</sub> reduction coupled with tetracycline (TC) removal than those of g-C<sub>3</sub>N<sub>4</sub>, CNBTC-10, CNBTC-30, and CNBTC-70. The introduction of the unique electron-donor-acceptor structure effectively drives the separation and transfer of photoinduced carriers while reducing the internal carrier transfer hindrance. Photocatalytic experiments reveal that the CNBTC-50 photocatalyst achieves up to 94.6% TC removal under visible light irradiation conditions. Compared with that of the pristine g-C<sub>3</sub>N<sub>4</sub>, the photocatalytic degradation reaction rate constant of CNBTC-50 is significantly increased by about 3.87 times. The study examines the influence of various reaction parameters on degradation activity, including catalyst concentration, pH, and TC concentration. Additionally, LC-MS is utilized to perform a comprehensive analysis of the intermediates and pathways involved in TC degradation. Furthermore, CNBTC-50 demonstrates remarkable photocatalytic CO<sub>2</sub> reduction activity, achieving rates of 20.83 μmol g<sup>-1</sup> h<sup>-1</sup> (CO) and 9.36 μmol g<sup>-1</sup> h<sup>-1</sup> (CH<sub>4</sub>), which are 10.68 and 5.98 times more efficient than those of g-C<sub>3</sub>N<sub>4</sub>, respectively. This work aims to offer valuable guidance for the rational design of nonmetal D-A-structured catalysts and effectively integrates reaction systems to couple CO<sub>2</sub> reduction with antibiotic removal.</p>\",\"PeriodicalId\":50,\"journal\":{\"name\":\"Langmuir\",\"volume\":\" \",\"pages\":\"\"},\"PeriodicalIF\":3.7000,\"publicationDate\":\"2024-11-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Langmuir\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.langmuir.4c03632\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Langmuir","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.langmuir.4c03632","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Enhancing Internal Electric Field of Metal-Free Donor-Acceptor Conjugated Photocatalysts for Efficient Photocatalytic Degradation of Tetracycline and CO2 Reduction.
Constructing alternating donor-acceptor (D-A) units within g-C3N4 represents an effective strategy for enhancing photocatalytic performance through improved charge carrier separation while concurrently addressing energy shortages and facilitating wastewater remediation. Here, a series of D-A-type conjugated photocatalysts (CNBTC-X) are prepared using g-C3N4 as an acceptor unit and different masses of 5-bromo-2-thiophenecarboxaldehyde (BTC) as a donor unit by a one-step thermal polymerization. CNBTC-50 presents higher photocatalytic properties for CO2 reduction coupled with tetracycline (TC) removal than those of g-C3N4, CNBTC-10, CNBTC-30, and CNBTC-70. The introduction of the unique electron-donor-acceptor structure effectively drives the separation and transfer of photoinduced carriers while reducing the internal carrier transfer hindrance. Photocatalytic experiments reveal that the CNBTC-50 photocatalyst achieves up to 94.6% TC removal under visible light irradiation conditions. Compared with that of the pristine g-C3N4, the photocatalytic degradation reaction rate constant of CNBTC-50 is significantly increased by about 3.87 times. The study examines the influence of various reaction parameters on degradation activity, including catalyst concentration, pH, and TC concentration. Additionally, LC-MS is utilized to perform a comprehensive analysis of the intermediates and pathways involved in TC degradation. Furthermore, CNBTC-50 demonstrates remarkable photocatalytic CO2 reduction activity, achieving rates of 20.83 μmol g-1 h-1 (CO) and 9.36 μmol g-1 h-1 (CH4), which are 10.68 and 5.98 times more efficient than those of g-C3N4, respectively. This work aims to offer valuable guidance for the rational design of nonmetal D-A-structured catalysts and effectively integrates reaction systems to couple CO2 reduction with antibiotic removal.
期刊介绍:
Langmuir is an interdisciplinary journal publishing articles in the following subject categories:
Colloids: surfactants and self-assembly, dispersions, emulsions, foams
Interfaces: adsorption, reactions, films, forces
Biological Interfaces: biocolloids, biomolecular and biomimetic materials
Materials: nano- and mesostructured materials, polymers, gels, liquid crystals
Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry
Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals
However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do?
Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*.
This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).