SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Xin Liu,Peng Xu,Qi Fu,Runhan Li,Chenxi He,Wenxuan Yao,Lei Wang,Shiqi Xie,Zhiyi Xie,Jingwei Ma,Qiulai He,John C. Crittenden
Zero-valent copper activated peroxymonosulfate (ZVC/PMS) system was widely used to degrade refractory contaminants due to being highly effective. However, the low reactivity and easy dismutation of cuprous species (Cu(I)) in acid condition limited its efficiency. In our study, ZVC coupled with ferrous ion (Fe(II)) promoted PMS to degrade orange II. Multiple oxidants including Cu(III), OH and SO 4 − made main contribution on orange II degradation in the Fe(II)/ZVC/PMS system. In the Fe(II)/ZVC/PMS system, ZVC generated Cu(I) by H + corrosion and PMS oxidation, and Cu(I) reacted with oxygen producing hydrogen peroxide. Then, Fe(II) and Cu(I) catalyzed hydrogen peroxide and PMS to generate Cu(III), OH and SO 4 − , and thereinto Fe(III) was reduced to Fe(II) by ZVC and Cu(I). In the Fe(II)/ZVC/PMS system, water matrix including humic acid, sulfate and nitrate had no significant impact on orange II degradation, while chloride restrained the degradation of orange II. The Fe(II)/ZVC/PMS system exhibited great degradation for orange II in tap water, lake water and well water. Additionally, the Fe(II)/ZVC/PMS system degraded more than 90% of methyl orange, rhodamine B, acetaminophen, ibuprofen, propranolol and diclofenac. Through adjusting the final reaction solution to pH 8.5 and subsiding, the discharge of total copper met the II-level environmental quality standards for surface water in China (1 mg/L). Hence, the study provided a promising method to induce PMS for enhanced degradation of contaminants.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Yangke Long,Jian Dai,Shiyin Zhao,Shixin Huang,Zuotai Zhang
Practical implementation of periodate-based advanced oxidation processes for environmental remediation largely relies on the development of cost-effective and high-performance activators. Surface atomic engineering toward these activators is desirable but it remains challenging to realize improved activation properties. Here, a surface atomic engineering strategy used to obtain a novel hybrid activator, namely cobalt-coordinated nitrogen-doped graphitic carbon nanosheet-enwrapped cobalt nanoparticles (denoted as Co@NC-rGO), from a sandwich-architectured metal–organic framework/graphene oxide composite is reported. This activator exhibits prominent periodate activation properties toward pollutant degradation , surpassing previously reported transition-metal-based activators. Importantly, the activator shows good stability, magnetic reusability, and the potential for application in a complex water matrix. Density functional theory modeling implies that the strong activation capability of Co@NC-rGO is related to its surface atomic structure for which the embedded cobalt nanoparticles with abundant interfacial Co–N coordinations display modified electronic configurations on the active centers and benefit periodate adsorption. Quenching experiments and electrochemical measurements showed that the system could oxidize organics through a dominant nonradical pathway. Additionally, a lower concentration of cobalt leaching was observed for the Co@NC-rGO/periodate system than for its Co@NC-rGO/persulfate counterpart. Our work provides a pathway toward engineering surface atomic structures in hybrid activators for efficient periodate activation.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 32
·17366-17379
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IF 12.732
Junjie Zhang,Wenran Gao,Yamei Yue,Wei Wang,Fatang Tan,Xinyun Wang,Xueliang Qiao,Po Keung Wong
Herein, biactive centers of Fe0-anchored graphitic N-rich graphene (Fe-GNG) were constructed via coordination and hydrogen bonding assemblies followed by calcination. The obtained Fe-GNG exhibited excellent peroxymonosulfate (PMS) activation ability to degrade diverse organic pollutants, accompanied by very low activation energy. Electron paramagnetic resonance and quenching experiments indicated that ˙OH and 1O2 were the predominant reactive species responsible for organics degradation, and were generated from PMS activation mainly at Fe0 and graphitic N sites, respectively. The degradation process had wide pH (2.2–10.3) and temperature (5–45 °C) application ranges, and a high tolerance to common matrix species, which enabled application to natural water systems. Furthermore, the magnetic Fe-GNG catalyst exhibited high stability and reusability, still degrading over 90% organics after five runs. This work provides a feasible strategy to construct multiple active sites for PMS activation, and clarifies the synergistic effect of metal and carbonaceous materials in radical and nonradical activation processes.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
·
IF 9.028
Jingyi Lin,Qin Dai,He Zhao,Hongbin Cao,Tianyu Wang,Guangwei Wang,Chuncheng Chen
Photoinduced interfacial release of volatile organic compounds (VOCs) from surfactants receives emerging concerns. Here, we investigate the photoreaction of 1-nonanol (NOL) as a model surfactant at the air–water interface, especially for the important role of 1O2 in the formation of VOCs. The production of VOCs is real-time quantitated. The results indicate that the oxygen content apparently affects the total yields of VOCs during the photoreaction of interfacial NOL. The photoactivity of NOL is about 8 times higher under air than that under nitrogen, which is mainly attributed to the generation of 1O2. Additionally, the production of VOCs increased by about 4 times with the existence of the air–water interface. Quenching experiments of 1O2 also illustrate the contribution of 1O2 to VOC formation, which could reach more than 95% during photoirradiation of NOL. Furthermore, density functional theory calculations show that 1O2 generated via energy transfer of photosensitizers can abstract two hydrogen atoms from a fatty alcohol molecule. The energy barrier of this reaction is 72.3 kJ/mol, and its reaction rate coefficient is about 2.742 s–1 M–1. 1O2 significantly promotes photoinduced oxidation of fatty alcohols and VOC formation through hydrogen abstraction, which provides a new insight into the interfacial photoreaction.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Tao Xiao,Peijian Yan,Kaijie Li,Caoping Yang,Hongbo Yu,Junyou Wang,Hongfeng Yin,Shenghu Zhou
Hollow mesoporous nanoreactors with encaged functional nanoparticles are promising heterogeneous catalysts due to the advantages related to their hollow cavities. In this study, we employ metal ion-bound polymer micelles to synthesize PtSn alloy nanoparticle-encaged hollow mesoporous nanoreactors (PtSn@HMSNs), which contain ∼4 nm PtSn alloy NPs located in ∼13 nm hollow cavities and relatively large (∼9 nm) mesoporous channels in silica shells. Relative to monometallic Pt@HMSNs and supported Pt1Sn0.3/SiO2, Pt1Sn0.3@HMSNs exhibit greatly enhanced activity and selectivity for hydrogenation of furfural to furfuryl alcohol. At 1.0 MPa H2, 100 °C, and a furfural/Pt molar ratio of 1884:1, 97.5% of furfuryl alcohol yield was achieved in 5.0 h. The dramatically promoted catalytic performance of Pt1Sn0.3@HMSNs can be assigned to the confinement effect that the location of active NPs inside hollow cavities increases the collision rates between reactants and active NPs to promote catalytic activity, as well as the synergistic effect between Pt and Sn.
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Materials Research Express
·
2021
·Vol. 8
·期 4
·045308
·
IF 1.62
Hao Luo,Kai Jin,Jie Tao,Hao Wang
It is difficult to synergistically improve the self-healing and mechanical properties of self-healing epoxy resin system based on Diels-Alder (DA) reversible covalent bond due to its different compositions. In this study, a method combining molecular dynamics (MD) simulation and back propagation (BP) neural network was employed to achieve a balance between self-healing property and mechanical property. In addition, self-healing and mechanical properties were predicted and the influence of different compositions of the system on these properties was investigated by the BP neural network. It was found that the DA bond formed by the furan group of furfuryl glycidyl ether (FGE) and the maleimide group of bismaleimide (BMI) was of great importance for self-healing property, and that diglycidyl ether of bisphenol-A (DGEBA) with a mass fraction of 25%–48% could improve the tensile property of the system. Finally, a self-healing epoxy resin system with superior comprehensive properties was designed through the proposed method under four indexes of Young's modulus (E), self-healing efficiency (η), Ultimate Tensile Strength (UTS), and glass transition temperature (Tg).
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Jinping Liang,Ling Fu
Persulfate-based advanced oxidation process (PS-AOP) is a promising technology for in-depth wastewater treatment. Here, Co 3 O 4 quantum dots (QDs) decorated hierarchical C@Co 3 O 4 (C@Co 3 O 4 -Q5) was prepared by a facile route. The crystalline structure, micrograph and chemical composition of C@Co 3 O 4 -Q5 were characterized by XRD, SEM, TEM and XPS. Taking Rhodamine B (RhB) as a model contaminant, the influences of process parameters on the degradation performance were evaluated. Detailed reaction kinetics investigation indicated that, at elevated temperatures higher than 30 °C, RhB degradation rate approximately follows this expression: r = 1.022 × 1 0 7 e x p ( - 47850 / R T ) [ R h B ] [ P M S ] 0.36 , whereas the real energies for catalytic activation ( Eac ) and heat activation ( Eah ) were 16.231 kJ·mol −1 and 31.62 kJ·mol −1 , respectively. Reactive oxygen species (ROS) quenching experiments and EPR tests suggested that not the general held radical SO 4 − but the downstream OH and the nonradical ROS 1 O 2 co-contribute to RhB mineralization. Meanwhile, PMS activation mechanisms referring to OH and 1 O 2 generation were elaborated based on XPS discussion. It was revealed that Co 3 O 4 quantum dots and oxygen functional groups and/or oxygen defects on carbon surface cooperate to generate ROS. Additionally, 5 successive cycles confirmed C@Co 3 O 4 -Q5′s high stability and reusability. These findings provided new insights into carbon-loaded QDs catalysts for PMS-mediated micropollutants removal.
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CATALYSIS LETTERS
·
2021
·Vol. 151
·期 9
·2513-2526
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IF 3.186
Cui Kai,Qian Wei,Shao Zhengjiang,Zhao Xiuge,Gong Honghui,Wei Xinjia,Wang Jiajia,Chen Manyu,Cao Xiaoming,Hou Zhenshan
Furfural (FFR) is one of the most important biomass-derived chemicals. Its large-scale availability calls for the exploration of new transformation methods for further valorization. Herein, we demonstrate that Ru nanoparticles (Ru NPs)-supported on a sulfonated carbon layer coated SBA-15 can be employed as an efficient bi-functional catalyst for one step conversion of FFR into 1,4-pentanediol (1,4-PeDO). The optimum bi-functional catalyst can afford the full the conversion of FFR and 86% selectivity to 1,4-PeDO. The catalysts have been characterized thoroughly by using a complementary combination of powder X-ray diffraction, N 2 adsorption–desorption, scanning/transmission electron microscopy, Fourier transform infrared spectroscopy, elemental analysis, and X-ray photoelectron spectroscopy. The characterization revealed that acidic groups (–SO 3 H) have been introduced on the surface of the carbon layer coated SBA-15 support after sulfonation with 98% H 2 SO 4 and the surface acidity can be tuned facilely by the sulfonating time. Meantime, Ru(0) sites was highly dispersed via an impregnation and sequential reduction and directly adjacent to the surface –SO 3 H group. There existed an electronic interaction between Ru(0) sites and sulfonic groups, in which the electronic transfer from sulfonic sites to Ru(0) sites occurred. Brönsted acid sites (–SO 3 H) have a significant influence on the FFR conversion and the selectivity to 1,4-PeDO. The ordered mesoporous structure, the appropriate density of acid sites and the electron-rich Ru(0) sites accounted for the the excellent performance of the catalyst for an efficient production of 1,4-PeDO from FFR. Graphic Abstract
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GREEN CHEMISTRY
·
2021
·Vol. 23
·期 4
·1772-1781
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IF 10.182
Jiale Ye,Songqi Ma,Binbo Wang,Qingming Chen,Kaifeng Huang,Xiwei Xu,Qiong Li,Sheng Wang,Na Lu,Jin Zhu
The lignin derivative ferulic acid was directly functionalized to diepoxy which could be co-cross-linked with furfuryl alcohol-derived monoepoxy to achieve high-performance bio-based thermosets. The development of high-performance bio-based epoxy as a sustainable alternative to fossil-sourced bisphenol A epoxy has great significance. In this work, ferulic acid-based diepoxy (FAE) was facilely synthesized through a direct reaction with epichlorohydrin. After cross-linking, its thermal and mechanical properties are comparable with or even higher than those of bisphenol A epoxy. The carbon–carbon double bond in the framework of the FAE was also exploited to further upgrade its properties via the Diels–Alder reaction with a synthesized glycidyl ether of furfuryl alcohol (GEFA). The chemical structures of FAE and GEFA, curing kinetics, and the Diels–Alder reaction were characterized in detail. The glass transition temperature of FAE-GEFA systems reached ∼250 °C. This work provides a simple way to achieve high-performance thermosets from ferulic acid, and also offers a promising sustainable alternative to bisphenol A epoxy.
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POLYMERS FOR ADVANCED TECHNOLOGIES
·
2020
·Vol. 32
·期 3
·1239-1250
·
IF 2.578
Shanjun Ding,Jun Zhang,Lin Zhou,Yunjun Luo
Polymer composites with self-healing ability are highly desired for applications in advanced modern devices. Here, we report on self-healing polymer composites consisting of silver deposited-carbon nanotubes hybrid nanoparticles (CNT-Ag) as fillers and self-healable polyurethane (DAPU) as a matrix based on thermally reversible Diels-Alder reaction. The results indicated that as the hybrid filler loading is 1 wt%, the composites not only obtained a high-strength (~15.97 MPa) and high healing efficiency (~90.1%) by increasing filler loading after healing, but also enhance thermal conductivity (~1.65 Wm −1 K −1 ) and obviously shorten its healing progress in comparison with other composites in the case of the same healing time. Given that Ag_NPs deposited on the surfaces of the CNTs act as bridges to link the adjacent CNTs and reduce interfacial thermal resistance, which can effectively explain the reasons for the obtained high mechanical strength and healing efficiency and promoting healing progress in the polymer composites. This work may offer a novel strategy for balancing relation between mechanical property, healing ability and healing progress in the field of self-healing materials application.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Dahu Ding,Liang Zhou,Fuxing Kang,Shengjiong Yang,Rongzhi Chen,Tianming Cai,Xiaoguang Duan,Shaobin Wang
Biochar is a promising candidate for the adsorptive removal of organic/inorganic pollutants, yet its role in metal-free catalyzed advanced oxidation processes still remains ambiguous. In this work, five biochar samples (PPBKx, where x represents the pyrolysis temperature) were prepared by using metal-enriched phytoremediation plant residue as the feedstock. Notably, PPBK exhibited a high specific surface area (as high as 1090.7 m2 g–1) and outstanding adsorption capacity toward ciprofloxacin (CIP, as much as 1.51 ± 0.19 mmol g–1). By introducing peroxymonosulfate (PMS, 5 mM) as the chemical oxidant, over 2 mmol g–1 CIP was synergistically adsorbed and oxidized within 30 min although PMS itself could not oxidize CIP efficiently, suggesting the formation of reactive oxidative species. Theoretical calculations revealed that PMS anions preferentially adsorbed on the activated C atoms adjacent to the graphitic N dopant, where the carbon matrix served as the electron donor, instead of as an electron mediator. The adsorbed PMS possessed a smaller molecular orbital energy gap, indicating that it was much easier to be activated than free PMS anions. Surface-bound reactive species were elucidated to be the dominant contributor through chemical quenching experiments and electrochemical characterizations. The catalytic activity of PPBK700 could be greatly retained in repeated oxidations because of the stable N species, which serve as the active catalytic sites, while the CIP adsorption was greatly deteriorated because of the diminishing active adsorption sites (carbon matrix edge) caused by the partial oxidation of PMS. This work not only provides a facile and low-cost approach for the synthesis of functional biochar toward environmental remediation but also deepens the understanding of biochar-catalyzed PMS activation and nonradical oxidation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
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IF 7.489
Yang Zhao,Di Wu,Ying Chen,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Carbon materials are effective catalysts to activate peroxymonosulfate (PMS) for organic pollutant degradation. Both nitrogen doping and structural defects could enhance their catalytic performance for PMS activation. In this study, nitrogen-doped graphene (NG) is first synthesized by the calcination of graphene oxide (GO) with ammonium nitrate (NH 4 NO 3 ). The obtained NG is then annealed further at a higher temperature under a N 2 atmosphere to remove partially doped N atoms and create new structural defects. The obtained defective nitrogen-doped graphene (D-NG) can activate PMS for bisphenol A (BPA) degradation more effectively. Different annealing temperatures from 850 to 1150 °C are investigated, and D-NG synthesized at 1050 °C exhibits the highest activity. The enhanced catalytic performance is proposed to originate from the synergistic effect between doped N atoms and created structural defects. According to radical quenching, electron paramagnetic resonance (EPR), and electrochemical results, both radical and nonradical pathways are present during PMS activation, and the nonradical pathway plays the dominant role. This study provides a facile method for metal-free catalyst synthesis, which also enriches the synergistic mechanism between doped N and structural defects and thus should have great potential in wastewater remediation.
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