SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Da Wang,Shiwen Dong,Siqi Fu,Yi Shen,Tao Zeng,Weiti Yu,Xiaohui Lu,Lizhang Wang,Shuang Song,Jun Ma
It is a feasible strategy to prepare reliable biochar catalysts for heterogeneous catalytic ozonation (HCO) processes by using inexpensive, high quality, and easily available raw materials. Here, an environmentally friendly, simple, and green biochar catalyst rich in nitrogen (N) and sulfur (S) has been prepared by the pyrolysis of kelp. Compared with directly carbonized kelp biomass (KB), acid-activated KB (KBA) and base-activated KB (KBB) have higher specific surface areas and more extensive porous structures, although only KBB displays effective ozone activation. Imazapic (IMZC), a refractory organic herbicide, was chosen as the target pollutant, which has apparently not hitherto been investigated in the HCO process. Second-order rate constants ( k ) for the reactions of IMZC with three different reactive oxygen species (ROS), specifically k O3, IMZC , k OH, IMZC , and k 1O2, IMZC , have been determined as 0.974, 2.48 × 10 9 , and 6.23 × 10 5 M −1 s −1 , respectively. The amounts of graphitic N and thiophene S derived from the intrinsic N and S showed good correlations with the IMZC degradation rate, implicating them as the main active sites. OH and O 2 − and 1 O 2 were identified as main ROS in heterogeneous catalytic ozonation system for IMZC degradation. This study exemplified the utilization of endogenous N and S in biological carbon, and provided more options for the application of advanced oxidation processes and the development of marine resources.
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JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Guangjian Xing,Lei Zhang,Yan Zhao,Sai Li,Tian Li,Tiantian Lv,Chunna Yu,Chang Zhao
The visible-light-responsive photocatalysts with high efficiency have been attracting tremendous focus in environmental remediation. Herein, three-dimensional (3D) Sb 2 X 3 ( X = S , Se) nanowires/graphene aerogel (Sb 2 X 3 /GA) monoliths were prepared by a facile hydrothermal route. The as-prepared Sb 2 X 3 /GA monoliths show the shape of a cylinder with a hierarchical porous structure. FESEM and porosimetry analyses revealed that the monoliths have high porosity, large total pore area as well as large pore volume . Sb 2 X 3 /GA demonstrated excellent photodegradation performance for the representative anionic/cationic dyes (methyl orange, rhodamine B , and crystal violet) and antibiotic drug (tetracycline hydrochloride) under 120 min of visible light irradiation. The degradation efficiencies of Sb 2 X 3 /GA were found to be 92.6–99.8% for the above-mentioned dye/drug, which were much larger than that of the pristine Sb 2 X 3 nanowires . The enhanced photodegradation activity could be ascribed to the synergistic effect between the Sb 2 X 3 nanowires and graphene aerogel, which was confirmed by the results of the photoluminescence and electrochemical impedance spectra. These findings provide an innovative strategy for designing 3D visible-light-responsive photocatalysts for water purification .
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Journal of CO2 Utilization
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2022
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IF 8.321
Haolin Du,Yifei Ye,Ping Xu,Jianmin Sun
The development of novel and efficient catalysts for the cycloaddition of CO 2 -epoxide has attracted the interest of researchers. In this work, a series of dicationic vinyl-functionalized imidazolium ionic liquids (ILs) were prepared, then polymerized and further copolymerized with 1,4-divinylbenzene (DVB) by free radical reaction. The synthesized PIL-DVB-IV catalyst presented 93% yield and 99% selectivity to the product of propylene carbonate under the optimized reaction conditions of 110 °C, 2.0 MPa for 6 h. Besides, the PIL-DVB-IV catalyst exhibited excellent recyclability and generality to various epoxides. The potential energy surface of the catalytic reaction was given by the computation of Density Functional Theory (DFT), which further revealed the proton migration catalytic mechanism of PIL-DVB-IV catalyst. The kinetic process of the catalyst was illustrated through the study of catalytic reaction kinetics and the calculation of DFT.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Hui Lv,Zuoyi Xiao,Shangru Zhai,Xuting Wang,Jingai Hao,Qingda An
Developing advanced electrode materials for high-performance supercapacitor applications is of great significance. However, it challenging due to the low specific capacitance of carbon-based electrodes and the sluggish charge transfer kinetics of pseudocapacitive materials. In this work, a hybrid electrode material was designed and prepared to enhance the electrochemical performance. Pseudo-active copper sulfide (Cu x S) particles were uniformly loaded on the skeleton of S-doped sodium carboxymethyl cellulose (CMC)-derived 3D hierarchical porous carbon (S-CPC). Owning to the good electron conduction at the interface, abundant micro-/mesoporous pathways, large accessible surface, and excellent redox activity of Cu x S particles, the optimized Cu x S@S-CPC-400 sample showed a high specific capacitance of 1372 F g −1 (191 mAh g −1 ) at a current density of 0.5 A g −1 . Furthermore, the assembled asymmetric supercapacitor with activated carbon and Cu x S@S-CPC-400 as the negative and positive electrodes, respectively, displayed an energy density of 75.3 W h kg −1 at a power density of 380.8 W kg −1 and excellent long-life stability with a capacitance retention of 86.67% over 10000 cycles. This work provides a feasible route to develop hybrid electrodes for high-performance energy storage systems.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2023
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IF 6.1
Yulin Zhao,Haoyan Huang,Ning Lv,Chunyan Huang,Huili Chen,Han Xing,Chaorui Guo,Ning Li,Di Zhao,Xijing Chen,Yongjie Zhang
Genipin (GP), the reactive metabolite of geniposide (GE), is responsible for GE-induced hepatotoxicity. As a potential detoxification pathway, the inactivation of GP by glutathione S-transferases (GSTs) has not yet been characterized. In this study, the thiol-GSH conjugates of GP, M532-1 and M532-2 were first identified and the catalytic activities of GSTs were investigated both in vitro and in vivo. GSTA1-1 and GSTA4-4 showed high activity in the formation of both thiol-GSH conjugates, whereas GSTA4-4 specifically catalyzed M532-2 formation in vitro. The active GST isoforms protect against alkylation of N-acetylcysteine (NAC), a classic model nucleophile. GST inhibition attenuated M532-1 formation in rat bile, confirming the in vivo catalytic role of GSTs. In conclusion, this study demonstrated the inactivation of GP by GSTs and implied that interindividual variability of GSTs may be a risk factor for susceptibility to GE-induced hepatotoxicity.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Xu Xu,Chaonan Jiao,Hao Yang,Hao Chen,Jing Wang
Au NPs generated in situ by photochemical reduction method were used as catalysts for the oxidation of sodium cholate . The circular dichroism of the oxidation product of sodium cholate exhibits a positive Cotton effect at 335 nm and an intense negative Cotton effect at 281 nm. Electrospray ionization (ESI) mass spectra and nuclear magnetic resonance (NMR) spectra were performed to characterize the chemical composition of the oxidation product of sodium cholate, revealing that two of the hydroxyl groups were selectively oxidized to oxo groups and the oxidation product is 12-hydroxy-3,7-diketo-cholanic acid (3,7-DKCA). The chiral recognition abilities of the aggregates of 3,7-DKCA were investigated by using planar chiral molecules R- and S-binaphthyl compounds. Compared with sodium cholate, the aggregates of 3,7-DKCA displayed higher chiral selective host–guest binding to the model molecules and the chiral recognition mechanism was clarified.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 21
·10237-10245
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IF 3.925
Yunfan Xu,Mengdong Guo,Shilong Lu,Zengyue Wei,Shengyu Feng
To reduce the pressing environmental concerns and negative environmental impact of non-recyclable materials, recyclable polymers pose promising and useful solutions. In this work, recyclable poly(sulfone siloxane)s were synthesized by the introduction of siloxane units into the main chain of aliphatic polysulfones via ring-opening polymerization of three types of sulfone-containing cyclosiloxane monomers with different lengths of alkyl segments. The results of wide-angle X-ray diffraction analysis revealed that the prepared polymers were amorphous. Thermal properties of the recyclable poly(sulfone siloxane)s were further investigated by differential scanning calorimetry and thermogravimetric analysis. Moreover, poly(sulfone siloxane)s were selectively depolymerized into the initial cyclic monomers using KHSO4 in an aqueous tetrahydrofuran solution at room temperature, suggesting the recyclability of the polymers. This work may provide a simple and useful strategy to design novel poly(sulfone siloxane)s with good solubility and recyclability.
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ELECTROCHIMICA ACTA
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2022
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IF 7.336
Quanlu Wang,Yikun Wang,Tingting Zhang,Yanmin Wang,Qiang Zhang,Tingxi Li,Yongqin Han
Metal-organic frameworks (MOFs) are promising candidates for supercapacitors due to their intrinsic porous structure. However, their low conductivity limits their supercapacitive performances. Herein, carbon cloth/ZIF67/polypyrrole composites (CZPAs) are prepared by first in-situ growing ZIF67 on carbon cloth and then electrochemical polymerizing pyrrole on carbon cloth/ZIF67 utilizing alizarin red S (ARS) as redox dopant. The synergistic effects of ZIF67 and ARS including porous structure, doping effect and inducing limited/ordered growth of polyprrole are contributed to the improved electrochemical performances. The resulted composite doped by 35 mM ARS (CZPA-35) achieves the highest areal capacitance of 1198 mF cm −2 among the CZPAs. The asymmetric supercapacitor assembled by CZPA-35 and carbon cloth/active carbon as flexible electrodes demonstrates high areal capacitance (288 mF cm −2 ), high energy density (57.6 μWh cm −2 ) and power density (300.96 μW cm −2 ). Moreover, the flexible supercapacitor provides excellent cycle stability after 5000 cycles (87.1% capacitance retention) and flexibility (85% capacitance retention after bending angle of 180 °). This strategy can be extended to fabricate other kinds of flexible MOF/PPy composites for the potential application of flexible wearable and portable electronic products.
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Science China-Materials
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2022
·Vol. 65
·期 6
·1463-1475
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IF 8.64
Zheng Xiao,Wang Zhilong,Li Jinjin,Wei Liangming
The rechargeable aluminum-sulfur (Al-S) battery is a promising alternative-energy storage device with high energy density and made of cheap raw materials. However, Al-S batteries face several obstacles, especially the shuttle effect. Herein, a binder-free S@Ti 3 C 2 T x sandwich structure film with uniform sulfur dispersion was designed. The two-dimensional (2D) layered material Ti 3 C 2 T x not only has the function of binder and conductive agent but also is a promising host for sulfur anchoring. As a result, S@Ti 3 C 2 T x film showed an initial capacity of 489 mA h g −1 at 300 mA g −1 and retained the value at 415 mA h g −1 after 280 stable cycles, with an average Coulombic efficiency of ∼95%. The film displayed higher capacity and stability than the S + Ti 3 C 2 T x cathode prepared by the slurry-coating method (the initial capacity was 317 mA h g −1 and then decayed to 222 mA h g −1 after 160 cycles). The main capacity of S@Ti 3 C 2 T x film in the Al-S battery came from the reversible redox reaction of S 2− and S. This new 2D material combined with a controllable electrode structure design paves the way for the development of Al-S batteries.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Minghui Xiang,Zhen Lu,Siyang Li,Hui Li,Chen Wang,Jin Zhang,Lide Jin,Chunyang Li
In recent years, new heterogeneous catalysts derived from metal organic frameworks (MOFs) have been widely used in advanced oxidation processes (AOPs). In this work, zeolite imidazole framework-67 (ZIF-67) and sulfide nanozero-valent iron (S-Fe) were used as precursors to prepare S-Fe/Co bimetallic nanoparticles embedded in graphitized carbon (S-Fe/Co@GC) and used to activate peroxymonosulfate (PMS) to degrade tetrabromobisphenol A (TBBPA). Morphological and structural characterization indicated that S-Fe/Co@GC compared to pre-carbonization, the pore size of the material became larger, formed a graphite carbon skeleton with excellent electrical conductivity. In a 0.2 g/L S-Fe/Co@GC and 0.6 mM PMS system, 96.1% of TBBPA (20 mg/L) was degraded within 30 min, and the degradation yielded a total organic carbon (TOC) removal of 56.2% in 60 min. This excellent catalytic activity was attributed to the synergistic effect of graphitic carbon, sulfide nanozero-valent iron and metallic cobalt. Radical quenching experiments and electron paramagnetic resonance (EPR) technology indicated that reactive oxygen species (ROS) included HO • , SO 4 •− , O 2 •− and 1 O 2 , among which O 2 •− plays a leading role in the degradation of TBBPA. Based on the LC-MS analysis of the degradation intermediates, the degradation pathway of TBBPA in the S-Fe/Co@GC/PMS system was proposed. In addition, S-Fe/Co@GC showed a low ion leaching rate, and the regenerated S-Fe/Co@GC still had high catalytic performance. This work will extend the development of MOFs encapsulate functional nanoparticle materials for environmental remediation.
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IONICS
·
2022
·Vol. 28
·期 5
·2377-2388
·
IF 2.961
Wang Shuangyu,Li Jinde,Ke Yihu,Wei Yelin,Wang Dewei
Heteroatoms co-doped porous carbon attracts tremendous research interest for electrochemical energy storage applications. We demonstrate herein N/S co-doped 3D carbon frameworks with the large specific surface area through KOH activation in the presence of KSCN by utilizing red bean as the precursor. We found that KSCN can not only act as the N/S sources but also serve as the co-activator to generate nanopores. Benefitting from its large specific surface, hierarchical porosity, and N/S co-doping, the largest specific capacitance can be reached 293.4 F g −1 (at 0.5 A g −1 ) and satisfactory rate capability of 68% (at 50 A g −1 ) in 6 M KOH aqueous electrolyte. Encouragingly, a high-energy density achieves to 23.025 Wh kg −1 can be obtained and in Na 2 SO 4 /PVA gel electrolyte within the voltage window of 0–1.8 V. The quasi-solid-state supercapacitor could also be connected in series or parallel to further enhance the working voltage or current.
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EUROPEAN POLYMER JOURNAL
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2022
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IF 5.546
Zhaoyang Wang,Bo Jiang,Yunhe Zhang,Xuefeng Li,Yongpeng Wang,Yingshuang Shang,Haibo Zhang
The rapid development of high-speed communication networks (for example, 5G) has imposed more stringent requirements on the comprehensive performance of low dielectric constant (low- k ) polymeric materials, as an important member of which, fluoropolymer has gained much attention. In this study, a series of cross-linkable fluorinated poly(aryl ether)s with different phenylethynyl content have been synthesized through nucleophilic substitution reaction, then their polymeric films have been prepared and thermally cross-linked via phenylethynyl groups. Thermal, mechanical and dielectric properties of the films are systematically compared. Due to the presence of F atoms and cross-linked structure in polymer chains, these polymeric films exhibit remarkable dielectric properties with the lowest dielectric constant < 2.4 and dissipation factor < 0.003 at frequency from 100 Hz to 1 MHz. Moreover, the dielectric performance shows impressive temperature independence before 200 °C. Excellent mechanical properties of the films have been corroborated by the DMA data of Young’s modulus > 1.50 GPa and modulus retention rate > 70%. It is noteworthy that polymeric films possess very low dielectric constant and dielectric loss at high frequency of 10 GHz, of which the lowest values can reach 2.47 and 0.0018, respectively. The polymeric films constructed in this study have shown great application prospects in the field of high-speed communication.
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