In-situ combination of CeO2-Au/SnO2 with g-C3N4 nanotubes as superior tubular catalysts for synergistically boosting the nitroaromatic reduction

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Jiasheng Fang, Ming Chen, Xusheng Wang, Zhenting Huang, Shuo Zhao, Peng Wang, Qing Li, Guangfu Liao
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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.

Abstract Image

CeO2-Au/SnO2与g-C3N4纳米管原位结合,作为协同促进硝基芳烃还原的优良管状催化剂
将g-C3N4纳米管(CNTs)与纳米尺寸的金属氧化物集成在一起,制造出高度结构化的复合材料,使得创新设计的高效au负载催化剂能够用于环境修复应用。在这里,我们报道了一种管状核壳催化剂CNTs@CeO2-Au/SnO2,它通过Sn2+介导的界面策略进行工程设计,能够静电吸附和原位还原金纳米粒子(NPs),然后与ceo2修饰的碳纳米管精确集成。该催化剂在硝基芳香族污染物还原方面表现优异,对4-硝基苯酚(4-NP)和4-硝基苯胺(4-NA)的去除反应速率常数分别为2.286 min−1和2.226 min−1,转换频率(TOF)分别为29.07 min−1和69.43 min−1,优于对照材料和先前的同类材料。该催化剂不仅能显著还原4-NP和4-NA异构体,还能还原复杂废水中的混合硝基芳烃和染料,证明了该催化剂的实用性。该催化剂被证明具有优异的可重复使用性,在连续五个循环中保持可靠的催化活性和结构稳健性。机理揭示了亚稳Au- h中间体和CeO2、Au/SnO2和CNTs之间的三元电子协同作用在降低活化能以驱动非自发的吸热还原途径中的关键作用。这项工作建立了多功能催化结构的蓝图,利用界面工程和电子转移调制来解决复杂的环境矩阵。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
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.
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