POLYMER ENGINEERING AND SCIENCE
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2021
·Vol. 61
·期 9
·2257-2266
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IF 2.428
Yunpeng Zhang,Jiaofeng Ye,Dongan Qu,Haitao Wang,Changsheng Chai,Libang Feng
Micro-damage in materials could be repaired by endowing materials with self-healing performance. Herein, an epoxy resin with excellent self-healing performance grounded on thermo-reversible Diels–Alder dynamic chemical reaction was developed. Results showed that the bending strength and adhesive behavior of epoxy resin were influenced dramatically upon treatment with various temperatures. More importantly, damages created in epoxy resin could be repaired completely after suitable heat treatments. What is more, the healed epoxy resin exhibited much higher bending strength and adhesive performance than the pristine one did. The materials could be damaged and then repaired repeatedly. Meanwhile, the as-prepared self-healing epoxy resin exhibited excellent thermal reversibility and controllable adhesion. The thermo-adjusted self-healing performance endowed epoxy resin with recyclable and reusable performance. Therefore, the research made it possible of recycling waste epoxy resins.
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Reaction Chemistry & Engineering
·
2021
·Vol. 6
·期 10
·1811-1818
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IF 4.239
Hongxing Wang,Guoqiang Ding,Yubo Liu,Junbo Zhang,Yongwang Li,Yulei Zhu
A sustainable and cost-competitive catalytic process for high yield production of levulinic acid (LA) and γ-valerolactone (GVL) from biomass-derived furfuryl alcohol (FOL) fluid was proposed with GVL as a self-circulation solvent. The innovative process eliminated the separation of the final product GVL and intermediate product LA from the solvent, and the actual concentration of FOL was improved enormously. A higher yield (90.5%) of LA was realized in the fixed-bed reactors than that in the conventional autoclave since the short residence time of the FOL solution could alleviate the polymerization of FOL in the continuous process. UV-Raman spectroscopy demonstrated that fewer polymers deposited on the catalysts, so superior stability of the zeolite was observed in the fixed-bed reactors. Moreover, an 89.4% high yield of GVL can be achieved since the integration of the tandem reaction of hydration and hydrogenation could substantially avoid side reactions in the fixed-bed reactors.
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CHEMOSPHERE
·
2021
·
IF 7.086
Yu Li,Yong Feng,Bin Yang,Zequn Yang,Kaimin Shih
The activation of persulfate by ferrous iron (Fe(II)) is of great interest to the environmental remediation community, but the reduction of ferric iron (Fe(III)) to Fe(II) is slow and the accumulation of iron sludge resulted from the precipitation of Fe(III) is a great concern. Here, molybdenum disulfide (MoS 2 ) was studied as a co-catalyst to improve the activation of peroxymonosulfate (PMS) by Fe(III) for sulfadiazine (SDZ) degradation and different characterization technologies were used to reveal the reactive species. The results showed that a strong synergy existed between MoS 2 and Fe(III); approximately 94.3% of the SDZ was removed by MoS 2 -Fe(III)-PMS after reaction for 30 min, while only 8.5% and 56.4% of the SDZ was removed by Fe(III)-PMS and MoS 2 -PMS, respectively. Both hydroxyl radicals and sulfate radicals were generated and the latter was the primary species. In addition to the radicals, singlet oxygen was found to be generated and contributed to the degradation of SDZ. The chemical probe reaction with methyl phenyl sulfoxide showed that the generation of high-valent iron-oxo species was not obvious by MoS 2 -Fe(III)-PMS under both acidic and neutral conditions. MoS 2 had good stability. No noticeable deactivation was observed during the 1st to 5th run and no obvious oxidation of surface Mo(IV) occurred. Based on the characterization of catalyst and oxidizing species, a mechanism for the activation of PMS by MoS 2 -Fe(III) was proposed. The results from this study are expected to clarify the reactive species and deepen the understanding of MoS 2 -promoted persulfate activation by Fe(II)/Fe(III).
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Ting Yang,Shisuo Fan,Yang Li,Qi Zhou
A high-efficient iron-based heterogeneous catalyst is desired to active peroxymonosulfate (PMS). Due to a large catalytic contribution of atomically dispersed Fe-N x sites, single-atom iron–nitrogen-carbon catalysts exhibit superior performance in the catalytic activation of PMS. Herein, a sequence of Fe-N-C SACs with atomically dispersed Fe-N x sites, Fe SA -N-C and Fe SA -N/C, were prepared from Fe-doped ZIF-8 and FePc@ZIF-8, respectively. Single-atom Fe-N x sites were confirmed to be the main active sites for PMS activation. Fe SA -N/C-20 with a higher density of Fe-N x sites exhibited superior catalytic performance to N/C, Fe SA -N-C, Fe SA -N/C-15, and Fe SA -N/C-25 for BPA degradation. Integrated with chemical quenching experiments, electron spin resonance (ESR), in-situ Raman spectra, and electrochemical analysis, a nonradical pathway was demonstrated to dominate the degradation of BPA in the PMS + Fe SA -N/C-20 system. More importantly, the nature of this nonradical pathway was found to be an electron-transfer regime instead of a high-valent iron or singlet oxygenation process. The BPA was adsorbed onto the Fe-N x site by a “donor–acceptor complex” mechanism to form a nonradical PMS* intermediate during the process. Benefiting from this mechanism, the PMS + Fe SA -N/C-20 system showed wide pH adaptation and high resistance to inorganic anions.
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Molecular Catalysis
·
2021
·
IF 5.062
Weile Li,Mengzhu Li,Huai Liu,Wenlong Jia,Xin Yu,Shuai Wang,Xianhai Zeng,Yong Sun,Junnan Wei,Xing Tang,Lu Lin
The economic and highly efficient synthesis of γ-valerolactone (GVL) is being increasingly focused due to its wide applications in solvent, chemical, and fuel. Herein, a range of SAPO-34 supported zirconium phosphate (ZPS-X) catalysts were prepared for a facile one-pot conversion of furfural (FF) to GVL through a series of cascaded reactions involving transfer hydrogenation, etherification, alcoholysis and esterification. The introduction of zirconium phosphate renders the formation of relatively strong Lewis acid sites, and the amount of Lewis (L) and Brønsted (B) acid sites of ZPS-X catalysts could be modified by adjusting the molar ratio of Zr to P (Zr/P ratio). Specifically, ZPS-1.0 having an appropriate Zr/P ratio with relatively strong L acid sites exhibited superior activity and selectivity for the production of GVL from FF.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
·
IF 9.028
Yangke Long,Jian Dai,Shiyin Zhao,Yiping Su,Zhongying Wang,Zuotai Zhang
Pollutant degradation via periodate (IO4–)-based advanced oxidation processes (AOPs) provides an economical, energy-efficient way for sustainable pollution control. Although single-atomic metal activation (SMA) can be exploited to optimize the pollution degradation process and understand the associated mechanisms governing IO4–-based AOPs, studies on this topic are rare. Herein, we demonstrated the first instance of using SMA for IO4– analysis by employing atomically dispersed Co active sites supported by N-doped graphene (N-rGO-CoSA) activators. N-rGO-CoSA efficiently activated IO4– for organic pollutant degradation over a wide pH range without producing radical species. The IO4– species underwent stoichiometric decomposition to generate the iodate (IO3–) species. Whereas Co2+ and Co3O4 could not drive IO4– activation; the Co–N coordination sites exhibited high activation efficiency. The conductive graphene matrix reduced the contaminants/electron transport distance/resistance for these oxidation reactions and boosted the activation capacity by working in conjunction with metal centers. The N-rGO-CoSA/IO4– system exhibited a substrate-dependent reactivity that was not caused by iodyl (IO3·) radicals. Electrochemical experiments demonstrated that the N-rGO-CoSA/IO4– system decomposed organic pollutants via electron-transfer-mediated nonradical processes, where N-rGO-CoSA/periodate* metastable complexes were the predominant oxidants, thereby opening a new avenue for designing efficient IO4– activators for the selective oxidation of organic pollutants.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Chengbo Ma,Jun Wang,Fei Wang,Yuanzhi Zhu,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Wenchao Peng
Iron oxide (Fe x O y ) supported on porous nitrogen doped carbon is synthesized by a facile pyrolysis method. SiO 2 and NaNO 3 are used as the template and activation agent respectively for porous structure generation and large specific surface area (SSA) creation. The obtained materials show superior catalytic oxidation ability and can activate peroxymonosulfate (PMS) in a wide pH range (3–9) to degrade organic pollutants. The degradation process is a two-stage reaction, including a rapid initial decay and a following slow reaction stage. According to the free radical quenching experiments, electron paramagnetic resonance (EPR) spectroscopy analysis, and electrochemical tests, the superoxide radical (O 2 − ) and singlet oxygen ( 1 O 2 ) are proved to play crucial roles in organics degradation . The high SSA (773 m 2 g −1 ), abundant of structural defects, and synergistic effect between Fe x O y and the nitrogen doped carbon are the key factors for the enhanced activity. The catalysts in this study can be synthesized easily and contain no toxic metals, thus should have great potential in the wastewater remediation.
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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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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Meesam Ali,Muhammad Tariq,Yong Sun,Jingyao Huang,Xiaogang Gu,Sana Ullah,Muhammad Asif Nawaz,Zhengyuan Zhou,Ali Shan,Muhammad Danish,Shuguang Lyu
Carbonaceous materials (CMs) have been applied extensively for enhancing the catalytic performance of environmental catalysts, however, the self-catalytic mechanism of CMs for groundwater remediation is rarely investigated. Herein, we unveiled the catalytic ability of various CMs via Fe(III) reduction through polyvinyl alcohol-coated calcium peroxide nanoparticles (PVA@nCP) for trichloroethylene (TCE) removal. Among selected CMs (graphite (G), biochar (BC) and activated carbon (AC)), BC and AC showed enhancement of TCE removal of 89% and 98% via both adsorption and catalytic degradation. BET and SEM analyses showed a higher adsorption capacity of AC (27.8%) than others. The generation of solution-Fe(II) and surface-Fe(II) revealed the reduction of Fe(III) on CMs-surface. The role of O-containing groups was investigated by the FTIR technique and XPS quantified the 52% and 57% surface-Fe(II) in BC and AC systems, respectively. EPR and quenching tests confirmed that both solution and surface-bound species (HO•, O 2 − • and 1 O 2 ) contributed to TCE degradation. Acidic pH condition encouraged TCE removal and the presence of HCO 3 − negatively affected TCE removal than other inorganic ions. Both schemes (PVA@nCP/Fe(III)/BC and PVA@nCP/Fe(III)/AC) exhibited promising results in the actual groundwater, surfactant-amended solution, and removal of other chlorinated-pollutants, opening a new direction towards green environmental remediation for prolonged benefits.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Zhuofan Huang,Qintie Lin,Nan Cai,Qingsong Weng,Jingwei Xu,Shuchai Gan,Chao Chen,Quanfa Zhong,Hengyi Fu,Yuejie Xia,Pengran Guo
In this study, CuO/HNTs were applied to activate persulfate (PS) to firstly degrade and mineralize TCS. The morphology, crystal structure, specific surface and surface composition were characterized by SEM, TEM, BET, XRD and XPS. The experimental parameters were optimized with 0.2 g/L CuO/HNTs and 2 mM PS. TCS was totally removed in 180 min under optimized conditions. The mechanism study using the quenching reaction, EPR, XPS and electrochemistry demonstrated that even radical reactions (•OH and O 2 •- ) pathway existed; the nonradical mechanism ( 1 O 2 and surface electron transport) was dominant to the efficient TCS degradation. Using FT-ICR MS, the degradation intermediates were identified, and transformation pathways were proposed. The degradation intermediate studies indicated that TCS began to break from the aromatic ring containing monochlorine, and the Cl functional group was gradually substituted. CO 2 and H 2 O were generated with breaking of ether bonds. The toxicity of the solution was also evaluated by the survival rate of the luminescent bacteria, and the toxicity of the solution decreased overall. A stability study showed that CuO/HNTs retained good crystal structure and degradation efficiency even after 5 cycles.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Ying Cai,Shihao Shen,Jinhong Fan
This study applied a mineral material of FeS to activate sulfite for efficient degradation of TTC in the presence of Cu(II) based on the identified complexation mechanism through UV–Vis spectra, FTIR spectroscopy and DFT calculation . pH plays an important role in TTC degradation and the initial pH of 6 and 7 were the divide in the contributions of FeS/sulfite oxidation and complex-precipitation. TTC-Cu(II) exhibits a superior promoting effect on the TTC degradation in FeS/sulfite system due to the improvement of TTC electron transfer reactivity and Fe(II) dissolution from FeS. Moreover, the formation of Cu(I) improved the recycling of Fe(II) from Fe(III). Dissolved oxygen-dependent free radicals’ generation was confirmed, and TTC degradation was mainly attributed to SO 4 ·− and ·OH. The characterization of FeS surface through XPS, XRD , SEM-EDS, Fe(II) deactivation tests, together with the comparison of pseudo-first-order rate constants for TTC degradation by FeS and ferrous ion supported the important role of surface and dissolved Fe(II) in sulfite activation . Furthermore, reasonable degradation pathways of TTC have been proposed according to the detected products by LC-MS. This work highlights the important role of pH, DO and Cu(II) complexation in sulfite activation and TTC degradation, furnishing theoretical support for further relevant studies.
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