CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaona Dong,Xiaoxue Yang,Sheng Hua,Ziqian Wang,Tianming Cai,Canlan Jiang
The continuous accumulation of triphenyl phosphate (TPHP) in soil poses a potential threat to human health. Persulfate-based advanced oxidation processes (SR-AOPs) are promising soil remediation technologies. Naturally occurring soil constituents could interact with persulfate (PS) during soil remediation by SR-AOPs. However, the production and transformation of reactive oxygen species (ROS) by synthetic reactions between PS and different soil constituents, as well as their roles in the pollutants degradation, are still largely unknown. This study systematically investigated the generation of ROS and their roles in degradation of TPHP in soil constituents activated PS process and in soil constituents-heat (50 °C) co-activated PS process. Comprehensive studies including ROS identification, electron paramagnetic resonance analysis, and ROS-generated model systems were carried out. An appreciable degradation rate of TPHP (~21.9%) in soil-PS system and the significant discrepancy in degradation rate (69.0–97.0%) in heat-soil-PS systems with three different soils suggested that soil constituents exhibited complex effects on the activation of PS. The Fe/Mn-minerals in soil effectively activated PS and facilitated TPHP degradation. Specially, the iron redox cycle (Fe(II) ↔ Fe(III)) plays a key role in ROS generation. Small molecular soil organic matter (SOM) rapidly consumed the produced ROS which led to their mineralization, while the remaining macromolecular SOM became more hydrophilic by interaction with ROS. SO 4 •− , •OH, and 1 O 2 played major roles directly in TPHP degradation, while O 2 •− could not degrade TPHP directly but might promote TPHP degradation by reducing Fe(III)- to Fe(II)-minerals or converting to other ROS. This study provides new and deeper insights into the interaction between PS and soil constituents and their roles in organic pollutant degradation in contaminated soil using SR-AOPs.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 32
·17366-17379
·
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.
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Xiaoping Liao,Jinru Cao,Ying Hu,Caixiang Zhang,Lisong Hu
Although various activated peroxymonosulfate (PMS) processes have been applied widely for the destruction of recalcitrant organics due to its high generation potential of various electrophiles reactive oxygen species (e.g., sulfate and hydroxyl radicals and singlet oxygen), non-radical-based PMS reactions with pollutants are poorly understood. Especially, relatively little information exists on the reactivity of PMS towards organic ester compounds such an organophosphorus pesticides (OPPs). Herein, we systematically studied the unactivated PMS-induced transformation of methyl parathion, a stubborn and toxic OPP. Specifically, direct reaction rather than electrophile radical-based oxidation was responsible for the rapid degradation of methyl parathion. The contribution of the produced singlet oxygen ( 1 O 2 ) from the self-decomposition of PMS to methyl parathion degradation can be neglected. The degradation rate constant ( k obs ) was strongly dependent on PMS loading and solution pH. The implication of the PMS reaction with methyl parathion for environment treatment was further evaluated by investigating the effects of common water matrices such as sediment humic acids , Cl − , and natural water. The identified metabolic products revealed that exposure to PMS resulted in hydrolysis and oxidation to methyl parathion. Further study demonstrated that PMS was also capable of effectively oxidizing other typical OPPs without explicit activation. This study provides novel insights into the reaction of methyl parathion with PMS, which indicate feasibility for the decontamination of OPP-contaminated environments.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Lehui Ren,Mei Chen,Jinxing Ma,Yang Li,Zhiwei Wang
In this study, a novel reactive electrochemical membrane (REM) made of Pd-loaded porous Ti was prepared to achieve ultrafast and efficient oxidation of trace antibiotics sulfamethoxazole (SMX) under anodic polarization. At a current density of 0.5 mA/cm 2 , the percentage removal of SMX by the REM was 96.3% in flow-through mode, with the energy cost ( i.e. , the electrical energy per order of removal, 1.34 Wh/m 3 ) being much lower than the flow-by mode (125.76 Wh/m 3 ) under the same operating condition. Quenching experiments and electron spin resonance spectra demonstrated that singlet oxygen ( 1 O 2 ) was the main reactive oxygen species in the REM system, playing a vital role in SMX degradation. Results of this study indicated that 1 O 2 was mainly generated on the anode via Pd–O 2 interaction that directly activated oxygen, rather than the evolution of 1 O 2 precursors ( e.g ., O 2 − and H 2 O 2 ). The constantly high electrochemical removal of SMX (88.5–91.9%) from actual surface water demonstrated that the matrix effect on the process performance was minimal in realistic applications, highlighting this novel REM to be a viable way to remove trace organic contaminants from surface water.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Lincai Peng,Xueying Gao,Yao Liu,Junhua Zhang,Liang He
Alkyl levulinate as one kind of fuel additive and versatile biomass-based platform molecule has attracted significant interests in the field of sustainable chemistry, which can be harvested straight from furfural (FAL), an important industrial chemical derived from agricultural residues. The development of a high-efficiency and low-cost catalytic system is highly desirable toward this challenging valorization process. In this contribution, bifunctional zirconia-zeolite-supported heteropoly acid catalysts with adjustable Lewis and Brønsted acid sites were successfully designed via an in situ synthetic method and attempted to couple transfer hydrogenation and alcoholysis for one-pot conversion of FAL to alkyl levulinate. The catalyst characterization and catalytic behavior were systematically combined for insight into the structure–function relationship and reaction mechanism. Selectivity toward alkyl levulinate was found to be strongly dependent upon the distribution of acid sites. As-prepared HPMo(20)/Zr-MCM-41 with a Si/Zr molar ratio of 60 and H3[P(Mo3O10)4] (HPMo) impregnation concentration of 20 g/L was uniquely effective using isopropanol as a hydrogen donor and reaction medium, leading to a high isopropyl levulinate yield of 79.6%. This monolithic catalyst exhibited good stability and could be reused at least 5 times without any substantial change in the product yield after plain thermal regeneration.
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2021
·
IF 8.001
Ruoqing Wang,Feng Shen,Yiwei Tang,Haixin Guo,Richard Lee Smith,Xinhua Qi
Levulinic acid in high yields (90%) was produced from hemicellulose-derived furfuryl alcohol catalyzed by a uniform, dandelion-like, SO 3 H-modified silica nanoflower solid acid (SiNF–SO 3 H). The SiNF–SO 3 H catalyst was prepared by soft template method in microemulsion system, followed by grafting of –SH and oxidation of –SH to –SO 3 H at room temperature to avoid use of corrosive sulfonating agents such as concentrated H 2 SO 4 . Dandelion-like porous structures of the SiNF–SO 3 H catalyst provided accessible and abundant catalytic sites ensuring high activity for furfuryl alcohol conversion (100%). Mixed-solvent γ -valerolactone-water (GVL-H 2 O) inhibited undesirable furfuryl alcohol polymerization reactions ensuring highly selective conversion of furfuryl alcohol to levulinic acid. Combination of catalyst and solvent system allowed achievement of the highest levulinic acid yields that have been reported to date. Both the catalyst synthesis protocol and reaction solvent (GVL-H 2 O) are green and sustainable. The SiNF–SO 3 H/(GVL-H 2 O) catalytic system has application to many acid catalyzed schemes for lignocellulosic biomass conversion.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2020
·
IF 0
Yuxian Wang,Nuo Ren,Jiaxin Xi,Ya Liu,Tao Kong,Chunmao Chen,Yongbing Xie,Xiaoguang Duan,Shaobin Wang
High-performance and robust catalysts act as core drivers for advanced oxidation technologies for decontamination of water resources. In this study, we used a facile strategy to prepare magnetic and N-doped carbon nanotubes with cobalt encapsulation (Co–N@CNTs) to catalyze ozone for decomposition of aqueous organic pollutants. By regulating the thermal conditions during the synthesis, the derived Co–N@CNTs manifested maneuvered adsorption capabilities. The embedded Co nanoparticles (NPs) not only afforded carbon nanotubes with a magnetic property but also significantly boosted catalytic ozonation due to the synergistic coupling of the Co interface and N-doped graphitic layer. Formation of such a coordinating structure accelerated electron transfer at the interface and increased the conductivity of surface carbon to coordinate a redox reaction. Density functional theory (DFT) calculations and experimental evidence confirmed that cobalt coupled with graphene with pyridinic N dopants was the most favorable structure, which remarkably enhanced ozone adsorption and its dissociation to generate reactive oxygen species (ROS). Intriguingly, the catalytic ozonation underwent different nonradical regimes dependent on the molecular structures of target organics. In terms of ROS, surface-adsorbed atomic oxygen (*Oad) was responsible for degradation of oxalic acid, while phenolics were primarily degraded by O3 molecules and singlet oxygen (1O2). This study provides a cost-efficient and recyclable carbocatalyst for wastewater decontamination and new insights into the structure–functional relationships in carbon-based advanced oxidation processes.
✓ 已验证
产品关联
DOI
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jianan Yu,Zhiliang Zhu,Hua Zhang,Yanling Qiu,Daqiang Yin,Yi Cheng,Shaobin Wang
Metal-free nanocarbons with versatile structural dimensions and unique properties are promising materials for remediation of polluted environment. In this work, a 3-dimensional (3D) interconnected porous N-doped carbon (CN-3) was synthesized by stepwise pyrolysis of dicyandiamide and nanocellulose, and a solid-state-growth and rolling-up mechanism was proposed for the stepwise transformation from stacking layered structures (melem and g-C 3 N 4 ) into CN-3 with 3D interconnected network nano-architectures. It was found that the functional carbons obtained at varying annealing temperature presented different activities in peroxymonosulfate (PMS) activation for endocrine-disrupting chemical (estrone) oxidation, showing temperature-dependent mechanisms from radical-dominated reaction to nonradical oxidation. CN-3 presented 100% estrone removal in 10 min, much higher than the layered carbons. In addition, CN-3 exhibited satisfactory stability during the catalytic reactions. Characterizations indicated that persistent free radicals on the layered carbons tended to induce radical reaction while graphitic structure and N in derived 3D carbons are more responsible for nonradical reaction. This work provides new insights to the relationship between the carbon structural transformation and catalytic PMS activation to induce different oxidative pathways, which facilitate the generation of a highly active and stable carbon-based catalytic system for organic degradation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Quanhao Shen,Lingfei Wei,Rehana Bibi,Ke Wang,Dandan Hao,Jiancheng Zhou,Naixu Li
Graphitic carbon nitride is considered as one of the promising photocatalysts for pollution elimination from wastewater. Manipulating the microstructure of carbon nitride remains a challengeable task, which is essential for improving light absorption , separating photogenerated carrier and creating reactive sites. Herein, a carbon vacancy modified hierarchical carbon nitride microrod (CN1.5) has been prepared templated from a melamine-NH 2 OH·HCl complex. The hierarchical microrods are demonstrated to be comprised of interconnected nanosheets with rich carbon vacancies, which endows it with high specific surface area, enhanced light utilization efficiency, available reactive sites, improved charge carrier separation and numerous mass-transport channels. The resultant photocatalyst CN1.5 exhibits an excellent photodegradation efficiency of 87.9% towards tetracycline under visible light irradiation. The remarkable apparent rate constant of 4.91 × 10 −2 min −1 is 7.3 times higher than that of bulk CN. In addition, the degradation pathways are deduced base on the observation of degradation intermediates generating in the photocatalytic process. Mechanism investigation indicates that the major contribution for photodegradation is attributed to ·O 2 – , 1 O 2 and H 2 O 2 species. This work provides new insights into advancing carbon nitride's microstructure to improve photocatalytic degradation performance for highly efficient antibiotic removal and environment remediation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 4
·1772-1781
·
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.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）