{"title":"还原氧化石墨烯包覆g-C3N4/SnO2异质结构中界面载流子动力学的揭示及其增强吸附和阳光驱动光催化作用。","authors":"Shalu Gupta, and , Rakesh Kumar*, ","doi":"10.1021/acs.langmuir.5c01341","DOIUrl":null,"url":null,"abstract":"<p >This work demonstrates the engineering of an rGO-wrapped g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> ternary heterojunction-based photocatalyst via a one-step in situ hydrothermal technique. The well-positioned CB edge of g-C<sub>3</sub>N<sub>4</sub> and the VB of SnO<sub>2</sub> create a type-II heterojunction, making g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> a promising photocatalyst for efficient redox reactions. Further, the incorporation of rGO, with its high specific surface area, significantly enhances the density of active site availability of the resulting ternary rGO/g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> heterostructure. The reduced band gap and formation of the multiple heterojunctions improve the separation and migration efficiency of photogenerated charge carriers, making the rGO/g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> heterojunction highly effective for removing a diverse category of pollutants. A small dose of 0.3 mg/mL of the ternary heterostructure degrades 99.3% of RhB dye under the exposure of simulated solar light for 40 min. Remarkably, the ternary heterostructure exhibits exceptional photodegradation efficiency for a mixture of dyes (MB + RhB + MO) with a high concentration of 30 mg/L, achieving removal rates of 99.99%, 71.4%, and 71%, respectively, within 40 min of irradiation. Moreover, first- and second-order in addition to the intraparticle diffusion models were used to determine the rate constants and equilibrium adsorption capacities of the rGO/g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> heterostructure, uncovering the underlying adsorption mechanisms. To comprehend the mechanistic intricacies underlying photocatalysis, a charge transfer process at the multiple interfaces has been thoroughly discussed using the experimentally determined values of work function and band edge positions from ultraviolet photoelectron spectroscopy and Mott–Schottky analysis, respectively. Eventually, the scavenger’s study affirms that the photogenerated e<sup>–</sup>–h<sup>+</sup> pairs, superoxide anion, and hydroxyl free radicals all play an active role in the photodegradation process.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":"41 25","pages":"16160–16179"},"PeriodicalIF":3.9000,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unveiling of Interfacial Charge Carrier Dynamics in rGO Wrapped g-C3N4/SnO2 Heterostructure for Enhanced Adsorption and Sunlight-Driven Photocatalysis\",\"authors\":\"Shalu Gupta, and , Rakesh Kumar*, \",\"doi\":\"10.1021/acs.langmuir.5c01341\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >This work demonstrates the engineering of an rGO-wrapped g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> ternary heterojunction-based photocatalyst via a one-step in situ hydrothermal technique. The well-positioned CB edge of g-C<sub>3</sub>N<sub>4</sub> and the VB of SnO<sub>2</sub> create a type-II heterojunction, making g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> a promising photocatalyst for efficient redox reactions. Further, the incorporation of rGO, with its high specific surface area, significantly enhances the density of active site availability of the resulting ternary rGO/g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> heterostructure. The reduced band gap and formation of the multiple heterojunctions improve the separation and migration efficiency of photogenerated charge carriers, making the rGO/g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> heterojunction highly effective for removing a diverse category of pollutants. A small dose of 0.3 mg/mL of the ternary heterostructure degrades 99.3% of RhB dye under the exposure of simulated solar light for 40 min. Remarkably, the ternary heterostructure exhibits exceptional photodegradation efficiency for a mixture of dyes (MB + RhB + MO) with a high concentration of 30 mg/L, achieving removal rates of 99.99%, 71.4%, and 71%, respectively, within 40 min of irradiation. Moreover, first- and second-order in addition to the intraparticle diffusion models were used to determine the rate constants and equilibrium adsorption capacities of the rGO/g-C<sub>3</sub>N<sub>4</sub>/SnO<sub>2</sub> heterostructure, uncovering the underlying adsorption mechanisms. To comprehend the mechanistic intricacies underlying photocatalysis, a charge transfer process at the multiple interfaces has been thoroughly discussed using the experimentally determined values of work function and band edge positions from ultraviolet photoelectron spectroscopy and Mott–Schottky analysis, respectively. Eventually, the scavenger’s study affirms that the photogenerated e<sup>–</sup>–h<sup>+</sup> pairs, superoxide anion, and hydroxyl free radicals all play an active role in the photodegradation process.</p>\",\"PeriodicalId\":50,\"journal\":{\"name\":\"Langmuir\",\"volume\":\"41 25\",\"pages\":\"16160–16179\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-06-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Langmuir\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.langmuir.5c01341\",\"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://pubs.acs.org/doi/10.1021/acs.langmuir.5c01341","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Unveiling of Interfacial Charge Carrier Dynamics in rGO Wrapped g-C3N4/SnO2 Heterostructure for Enhanced Adsorption and Sunlight-Driven Photocatalysis
This work demonstrates the engineering of an rGO-wrapped g-C3N4/SnO2 ternary heterojunction-based photocatalyst via a one-step in situ hydrothermal technique. The well-positioned CB edge of g-C3N4 and the VB of SnO2 create a type-II heterojunction, making g-C3N4/SnO2 a promising photocatalyst for efficient redox reactions. Further, the incorporation of rGO, with its high specific surface area, significantly enhances the density of active site availability of the resulting ternary rGO/g-C3N4/SnO2 heterostructure. The reduced band gap and formation of the multiple heterojunctions improve the separation and migration efficiency of photogenerated charge carriers, making the rGO/g-C3N4/SnO2 heterojunction highly effective for removing a diverse category of pollutants. A small dose of 0.3 mg/mL of the ternary heterostructure degrades 99.3% of RhB dye under the exposure of simulated solar light for 40 min. Remarkably, the ternary heterostructure exhibits exceptional photodegradation efficiency for a mixture of dyes (MB + RhB + MO) with a high concentration of 30 mg/L, achieving removal rates of 99.99%, 71.4%, and 71%, respectively, within 40 min of irradiation. Moreover, first- and second-order in addition to the intraparticle diffusion models were used to determine the rate constants and equilibrium adsorption capacities of the rGO/g-C3N4/SnO2 heterostructure, uncovering the underlying adsorption mechanisms. To comprehend the mechanistic intricacies underlying photocatalysis, a charge transfer process at the multiple interfaces has been thoroughly discussed using the experimentally determined values of work function and band edge positions from ultraviolet photoelectron spectroscopy and Mott–Schottky analysis, respectively. Eventually, the scavenger’s study affirms that the photogenerated e––h+ pairs, superoxide anion, and hydroxyl free radicals all play an active role in the photodegradation process.
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).