{"title":"In-situ combination of CeO2-Au/SnO2 with g-C3N4 nanotubes as superior tubular catalysts for synergistically boosting the nitroaromatic reduction","authors":"Jiasheng Fang, Ming Chen, Xusheng Wang, Zhenting Huang, Shuo Zhao, Peng Wang, Qing Li, Guangfu Liao","doi":"10.1016/j.cej.2025.164208","DOIUrl":null,"url":null,"abstract":"Integrating g-C<sub>3</sub>N<sub>4</sub> nanotubes (CNTs) with nano-sized metal oxides to fabricate highly structured composites enables the innovative design of efficient Au-supported catalysts in environmental remediation applications. Here, we report a tubular core–shell catalyst, CNTs@CeO<sub>2</sub>-Au/SnO<sub>2</sub>, engineered through a Sn<sup>2+</sup>-mediated interfacial strategy enabling electrostatic adsorption and in-situ reduction of Au nanoparticles (NPs), followed by precise integration with CeO<sub>2</sub>-decorated CNTs. The catalyst achieved exceptional performance in nitroaromatic pollutant reduction, exhibiting reaction rate constants of 2.286 min<sup>−1</sup> and 2.226 min<sup>−1</sup> with turnover frequencies (TOF) of 29.07 min<sup>−1</sup> and 69.43 min<sup>−1</sup> for 4-nitrophenol (4-NP) and 4-nitroaniline (4-NA) removals, respectively, surpassing control materials and prior counterparts. The catalyst’s practical versatility was demonstrated through its remarkable reduction of not only 4-NP and 4-NA isomers but also mixed nitroaromatics and dyes in complex wastewater. The catalyst proved excellent reusability, sustaining reliable catalytic activity and structural robustness across five consecutive cycles. Mechanistic insights revealed the critical role of metastable Au-H intermediates and a ternary electronic synergy between CeO<sub>2</sub>, Au/SnO<sub>2</sub> and CNTs in lowering activation energy to drive otherwise non-spontaneous, endothermic reduction pathways. This work established a blueprint for multifunctional catalytic architectures leveraging interfacial engineering and electron-transfer modulation to address complex environmental matrices.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"98 1","pages":""},"PeriodicalIF":13.3000,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2025.164208","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Integrating g-C3N4 nanotubes (CNTs) with nano-sized metal oxides to fabricate highly structured composites enables the innovative design of efficient Au-supported catalysts in environmental remediation applications. Here, we report a tubular core–shell catalyst, CNTs@CeO2-Au/SnO2, engineered through a Sn2+-mediated interfacial strategy enabling electrostatic adsorption and in-situ reduction of Au nanoparticles (NPs), followed by precise integration with CeO2-decorated CNTs. The catalyst achieved exceptional performance in nitroaromatic pollutant reduction, exhibiting reaction rate constants of 2.286 min−1 and 2.226 min−1 with turnover frequencies (TOF) of 29.07 min−1 and 69.43 min−1 for 4-nitrophenol (4-NP) and 4-nitroaniline (4-NA) removals, respectively, surpassing control materials and prior counterparts. The catalyst’s practical versatility was demonstrated through its remarkable reduction of not only 4-NP and 4-NA isomers but also mixed nitroaromatics and dyes in complex wastewater. The catalyst proved excellent reusability, sustaining reliable catalytic activity and structural robustness across five consecutive cycles. Mechanistic insights revealed the critical role of metastable Au-H intermediates and a ternary electronic synergy between CeO2, Au/SnO2 and CNTs in lowering activation energy to drive otherwise non-spontaneous, endothermic reduction pathways. This work established a blueprint for multifunctional catalytic architectures leveraging interfacial engineering and electron-transfer modulation to address complex environmental matrices.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.