SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Yu Wang,Lianhu Fang,Zhen Wang,Qi Yang
Graphitic carbon nitride (g-C 3 N 4 ) doped with metals and nonmetals has been widely applied to activating peroxymonosulfate (PMS) for removing organic pollutants. Herein, g-C 3 N 4 co-doped with manganese, cobalt, and oxygen (MCOCN) was prepared via a facile sol–gel calcination protocol for PMS activation to eliminate trichloroethylene (TCE). The influence of different oxygen precursors, namely citric acid, oxalic acid, and barbituric acid, on the catalytic capability of the MCOCN was investigated. Superior performance was found when the MCOCN was synthesized by the citric acid as the oxygen precursor; 100% TCE removal was achieved within 10 min by adding a 0.5 g/L catalyst and 1 mM of the PMS without a pH adjustment. The difference in the activity of the resultant catalysts could be ascribed to the carbon-to-nitrogen ratio and the content of metal on the surface of prepared catalysts. The impacts of parameters such as the concentration of the PMS, the initial pH, and the dose of the catalyst on the kinetics of trichloroethylene degradation were also investigated. A competitive kinetic model was employed to confirm that contribution of the sulfate radicals in TCE degradation was underestimated when the concentration of the quencher was set at 100 times the concentration of the oxidant. The quenching experiments demonstrated that OH ∙ and SO 4 ∙ - were the main reactive species, while 1 O 2 and O 2 ∙ - played a minor role in the degradation of the TCE by the MCOCN–PMS system. Furthermore, the reusability and ion leaching of the prepared catalysts were evaluated. Our results provide fundamental insights into applying the MCOCN to PMS activation for eliminating trichloroethylene in groundwater.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Renji Zheng,Jing Li,Runliang Zhu,Ranhao Wang,Xuezhen Feng,Zhijie Chen,Wenfei Wei,Dazhong Yang,Hong Chen
Wastewater with complex compositions of both heavy metals and organic pollutants is of critical environmental and socioeconomic threat worldwide, which urgently requires feasible remediation technologies to target this challenge. In this study, natural chalcopyrite (CuFeS 2 , NCP), the most abundant copper-based mineral in the Earth's crust , has been discovered to be a heterogeneous catalyst that can activate peroxydisulfate (PDS) for the simultaneous degradation of organic pollutant Rhodamine B (RhB) and reduction of hexavalent chromium (Cr(VI)). Batch experimental results indicate that both RhB and Cr(VI) could be simultaneously removed under a near-neutral condition in NCP/PDS combined system. The radicals SO 4 •− and • OH generated from PDS activation are the main oxidative species detected by electron paramagnetic resonance (EPR) spectroscopy. SO 4 •− acted as a predominant role in RhB degradation, while Cr(VI) reduction is mainly attributed to the oxidization of S 2− and S 2 2− species on NCP surface, as well as the photoreduction performance of NCP, which could be enhanced by the intermediates generated from RhB degradation. Density functional theory (DFT) calculation results disclose that Fe is the critical catalytic site for PDS activation. This work demonstrates a user-friendly strategy for remediation of complex wastewater containing both heavy metal and organic pollutants by combining photoreduction and advanced oxidation processes (AOPs) with natural minerals. It paves a way for wastewater treatment by utilizing low-cost natural abundant minerals as catalysts.
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Environmental Science-Nano
·
2021
·Vol. 8
·期 11
·3138-3152
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IF 8.131
Weirui Chen,Hengxi He,Ruini Zou,Yidan Chen,Xukai Li,Jing Wang,Yiming Tang,Laisheng Li
In this study, CeOx with different exposed facets was prepared to investigate their potential effect on activating the peroxone reaction (H2O2/O3) and breaking through the restriction of solution pH on peroxone. By controlling the concentration of hydroxide, cube CeOx with a (100) facet, rod CeOx with a (110) facet and octahedron CeOx with a (111) facet were prepared by the hydrothermal precipitation method, and they all promoted heterogeneous peroxone for oxalic acid (OA) under acidic conditions. The catalytic activity of CeOx was highly related to their surface oxygen vacancies (OVs) and the interfacial electron transfer process. Both experiments and theoretical calculations showed that CeOx with different exposed facets activated peroxone in different ways and (111) CeOx possessed better activity than (100) or (110) CeOx. The low efficiencies of (100) and (110) CeOx were due to their inefficient use of H2O2 to reduce surface Ce4+ and their large energy gap to generate surface peroxide (OVs-OOH). (111) CeOx was stable with surface-adsorbed H2O2, and the rich electrons at OVs could be donated to H2O2 and generate OVs-OOH, which then triggered O3 decomposition into hydroxyl radical (˙OH) and superoxide radical (˙O2−). These electron migration processes depended on the electron-donating ability of the OVs rather than solution pH, therefore, still greater amounts of reactive species were generated under acidic conditions. The flexibility of the (111) CeOx/H2O2/O3 process was further investigated for removing 20 kinds of pharmaceuticals. The synergy effect of (111) CeOx/O3 and H2O2 varied with the structure of the pharmaceuticals.
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Soft Matter
·
2021
·Vol. 17
·期 30
·7158-7167
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IF 3.679
Hanqi Xu,Jinbo Wu,Yaying Hong,Weijia Wen
The impact of two nonionic surfactants, namely Span 20 and Span 85, on the electrorheological response and colloidal stability of urea-coated barium titanyl oxalate (BTRU)/silicone oil suspensions is investigated. We quantitatively analyze the surfactant effect on modified ER performance through the measurements of yield stress and current density, as well as the tuned suspension stability through calculation of the Turbiscan stability index (TSI) and naked-eye observations of sedimentation phenomena. The surfactant effect on particle–oil interactions and agglomeration effects is examined by measuring the permeability of silicone oil when mixed with the Span surfactant and the cluster size of particles in dispersing medium, respectively. Our results indicate that with the presence of a Span surfactant, the yield stress of the suspension exhibits a local maximum at certain Span concentrations. We hypothesize that below the optimal Span concentration, the ER properties are enhanced by the increase of the electrostatic interaction between particles. Above the limiting concentration, the ER activity is weakened by the formation of a double-layer surfactant structure that generates a steric hindrance effect. We discover that the addition of the Span surfactant favors the improvement of the particle agglomeration phenomenon, thereby promoting colloidal stability of the suspension. Consequently, in the consideration of both ER properties and suspension stability, an optimal ER fluid with the addition of 0.4 wt% Span 85 is acquired with remarkable integrated ER properties.
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ACS Omega
·
2021
·
IF 3.512
Hongzhi Lu,Shoufang Xu
Manganese dioxide (MnO2) nanosheet-based fluorescence sensors often use oxidase-like activity or wide absorption spectrum for detection of antioxidants. In those strategies, MnO2 nanosheets were reduced to Mn2+ by antioxidants. However, few strategies emphasize the role of Mn2+ obtained from MnO2 reduction in the design of the fluorescence sensor. Herein, we expanded the application of a MnO2 nanosheet-based fluorescence sensor by involving Mn2+ in the detection process using ascorbic acid (AA) as a model target. In this strategy, carbon dots (CDs), MnO2 nanosheets, and tetraphenylporphyrin tetrasulfonic acid (TPPS) comprise a ternary system for ratiometric fluorescence detection of AA. Initially, CDs were quenched by MnO2 nanosheets based on the inner filter effect, while TPPS maintained its fluorescence intensity. After the addition of AA, MnO2 nanosheets were reduced to Mn2+ so that the fluorescence intensity of CDs was recovered and TTPS was quenched by coordination with Mn2+. Overall, AA triggered an emission intensity increase at 440 nm for CDs and a decrease at 640 nm for TPPS. The ratio intensity of CDs to TPPS (F440/F640) showed a good linear relationship from 0.5 to 40 μM, with a low detection limit of 0.13 μM for AA detection. By means of the alkaline phosphatase (ALP)-triggered generation of AA, this strategy can be applied for the detection of ALP in the range of 0.1–100 mU/mL, with a detection limit of 0.04 mU/mL. Furthermore, this sensor was applied to detect AA and ALP in real, complex samples with ideal recovery. This novel platform extended the application of MnO2 nanosheet-based fluorescence sensors.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Guojuan Hai,Jianfeng Huang,Liyun Cao,Koji Kajiyoshi,Long Wang,Liangliang Feng,Jun Chen
The electrochemical conversion is closely correlated with the electrocatalytic activities of the electrocatalyst. Herein, the urchin-like Ni-doped W 18 O 49 /NF with enriched active sites was prepared by solvothermal method followed by a low-temperature pyrolysis treatment was reported. Results demonstrate that the incorporation of Ni-doping triggers the lattice distortion of W 18 O 49 for the increasement of oxygen defects. Further, high-valent W 6+ are partially reduced to low-valent W 4+ , wherein the electrons originate from the oxidation process of Ni 2+ to Ni 3+ . The Ni 3+ ions show an enhanced orbital overlap with the OER reaction intermediates. The generated W 4+ ions contribute to release oxygen vacancies, eventually reorganizing Ni-doped W 18 O 49 /NF to unique electrochemical active species with a special amorphous-crystalline interface (AM/NiWO x /NiOOH/NF). Simultaneously, the reconstruction results in an optimized valence band and conduction band. Eventually, the resultant AM/NiWO x /NiOOH/NF with abundant active sites and improved oxidation/reduction capability exhibits more superior catalytic performance compared with the Ni-doped W 18 O 49 /NF counterpart. This study gives more insights in the electrochemical evolution of the tungsten-based oxide and provides effective strategies for optimizing the catalytic activity of materials with inherent hydrogen evolution reaction limitations.
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ANALYTICA CHIMICA ACTA
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2021
·
IF 6.558
Hyok-Chol Ri,Jishou Piao,Long Cai,Xuejun Jin,Xiangfan Piao,Xiangzi Jin,Chol-San Jon,Lu Liu,Jinhua Zhao,Hai-Bo Shang,Donghao Li
A reciprocating magnetic-field-assisted on-line solid-phase extraction (RMF-SPE) method coupled with liquid chromatography-tandem mass spectrometry (LC-MS/MS) has been developed for continuous enrichment of trace chemicals in water samples. Under the assist of the reciprocating magnetic field, carboxyl-modified magnetic nanoparticles (CMNPs) were applied to prepare microcolumn with even dispersion by periodical motion, instead of traditional compaction as extraction sorbents . When water sample passed through the extraction region, dynamic sorbents generates an advantage of countless contacts between sorbents and targets without blocking for high efficient extraction. In this study, the on-line RMF-SPE method was established and evaluated by determination of tetracyclines (TCs) from water samples as analysis models, including oxytetracycline , tetracycline, demeclocycline , metacycline, chlortetracycline , and doxycycline . Experimental conditions have been investigated such as flow rate , reciprocating speed, elution time, and so on. The method showed high relative recovery (95.4–111.1%) and good repeatability with RSD from 2.9 to 11.8% for the 200 mL water sample. The linearity range, limits of detection (LODs), and limits of quantification (LOQs) were 0.5–200 μg L −1 (chlortetracycline) and 0.1–200 μg L −1 (other TCs), 12.0–74.1 ng L −1 , and 40.1–247 ng L −1 , respectively. More importantly, the high enrichment factors in a range of 204 (chlortetracycline) to 276 (demeclocycline) indicate that a small amount of dynamic sorbents (only 10 mg) give full play to extraction attributing to the reciprocating movement, especially for trace analysis and continuous extraction, which is significant for water samples from sea, river and domestic waste.
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Materials Today Energy
·
2021
·
IF 7.311
Qiushi Sun,Xiao Chen,Jian Xie,Changhai Shen,Yuan Jin,Cheng Huang,Xiongwen Xu,Jian Tu,Bo Wang,Tiejun Zhu,Xinbing Zhao,Jipeng Cheng
A solid-state lithium metal battery has been considered as a promising next-generation energy storage system for its high safety. Great challenges remain for the scale-up fabrication of solid-state Li batteries with the current manufacturing facility used for liquid Li-ion batteries. In this work, a scale-up route is employed to fabricate quasi-solid-state Li batteries by cathode-supported coating of a solid electrolyte combined with in-situ polymerization for interfacial modification. A Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) layer with a polyvinylidene fluoride (PVDF) binder is coated on the LiCoO 2 cathode as the solid electrolyte. A iquid electrolyte containing a poly(ethylene glycol) methyl ether acrylate (PEGMEA) monomer is injected during the battery fabrication process followed by in-situ polymerization. The in-situ formed gel electrolyte acts as a soft interface to enhance the contact between the electrode and the solid electrolyte. A coin-type quasi-solid-state Li||LiCoO 2 battery delivers a high capacity of 122 mAh g −1 and retains 81% of its initial capacity after 100 cycles at 0.5 C and 60 °C. A pouch-type Li||LiCoO 2 battery is also fabricated using a commercial LiCoO 2 electrode and shows a satisfactory safety performance and stable cycling at 0.5 C.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 29
·16290-16306
·
IF 4.22
Liu Cansen,Zhuang Mingta,Huang Qishan,Mai Yongjin,Zhang Liuyan,Jie Xiaohua
Mold fouling during vulcanization is a widespread issue faced by tire industry that urgently needed to be addressed as it can degrade comprehensive performance of molded products and increase production time for cleaning mold, resulting in tremendous economic loss and resource consumption. Here, a novel and promising fouling mitigation strategy inspired by nature is presented, and its antifouling behavior in vulcanization conditions is investigated. The inspired slippery liquid-infused surfaces were successfully designed on aluminum alloy by anodic oxidation, followed by myristic acid modification and impregnation with perfluorinated oil. The prepared surfaces showed a water contact angle of 112.3° and sliding angle of 0.5°, accompanying with self-cleaning ability, stability for repelling hot water and under high-pressure condition as well as excellent corrosion resistance in 0.05 M H 2 SO 4 corrosive medium. Moreover, remarkable antifouling performance was obtained for slippery liquid-infused surfaces as no trace of fouling was observed after vulcanization test and thus a potential strategy for practical industrial applications. Graphical abstract
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Materials Chemistry Frontiers
·
2021
·Vol. 5
·期 18
·6941-6950
·
IF 6.482
Dongli Chen,Wenwei Zhan,Xue Fu,Ming Zhu,Jinle Lan,Gang Sui,Xiaoping Yang
Lithium–sulfur (Li–S) batteries with high theoretical capacity and low cost are challenged by the polysulfide shuttle effect and sluggish reaction kinetics. Herein, a functional composite interlayer consisting of metallic 1T-MoS2 with high catalytic activity and carbon fiber cloth is firstly designed and fabricated for high-performance Li–S batteries. The 1T-MoS2@carbon fiber cloth (1T-MoS2@CFC) composite interlayer with high electrical conductivity not only serves as the upper current collector to improve the utilization of the sulfur cathode, but also acts as a polysulfide barrier and trapper to suppress the shuttle effect of polysulfides by strong chemical interaction.
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CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Linying Yang,Shuwei Sun,Kai Du,Huiling Zhao,Dong Yan,Hui Ying Yang,Caiyan Yu,Ying Bai
Layered O3 type oxides exhibit promising prospects as high-performance cathodes for sodium-ion batteries (SIBs) due to their low cost and high theoretical capacities. Nevertheless, the intrinsic surface composition and bulk structure degradation upon cycling presents a huge obstacle to stable sodium-ion storage/transportation. Besides, the effective surface decoration on layered O3 oxides is still challenging through conventional wet chemical route owing to their extraordinarily high surface sensitivities. Herein, a typical O3 type layered oxide of NaNi 0.5 Mn 0.5 O 2 (NNMO) was selected and successfully encapsulated by precisely controlled Al 2 O 3 layers via atomic layer deposition (ALD) technology. With the optimally controlled Al 2 O 3 thickness of 3 nm, the surface regulated NNMO delivers a highly reversible capacity of 73.6 mA h g -1 , with a significantly improved capacity retention of 68.0% after 300 cycles at 0.5 C, and a superior rate capability of 65.8 mA h g -1 at 10 C. Further air sensitivity tests demonstrate that the protective layer could effectively mitigate the generation of sodium-based impurities on NNMO, and reduce the surface sensitivities. Both chemical and electrochemical aging tests confirm the contribution of Al 2 O 3 coating layer in alleviating ion dissolution as well as stabilizing the structure and morphology of NNMO. Based on regulating the surface of O3 type layered oxides utilizing ALD technique, this work supplies an effective and facile strategy to overcome the challenges from fast structure degradation and electrochemical property decay, which not only highlights the significance and effectiveness of surface engineering in secondary batteries, but also sheds light on accurate interface construction and regulation for active electrode materials, particularly for those sensitive to ambient atmosphere.
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DYES AND PIGMENTS
·
2021
·
IF 4.889
Shijun Lin,Shuwen Liu,Guofei Dai,Xiaojin Zhang,Fan Xia,Yu Dai
Gold nanoparticles (AuNPs), as one of the major tools of fluorescence-quenching sensors, have been widely used in biochemical analysis through fluorescence resonance energy transfer (FRET) effect. With the development of chemistry and biochemistry, reaction-based fluorescent sensors have attracted increasing attention because of their unique selectivity, high sensitivity and rapid detection. Here we report a click-induced fluorescence-quenching sensor based on AuNPs for detection of copper ion (Cu 2+ ) and ascorbic acid (AA). A fluorescent dye Rhodamine B-(CH 2 CH 2 O) 4 -azide (RB-PEG 4 -N 3 ) is conjugated to the surface of AuNPs via Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) in the presence of Cu 2+ and AA, leading to the fluorescence quenching of Rhodamine B. The sensor responds quickly (within less than 3 min). The fluorescent intensity linearly correlates with the concentration of Cu 2+ in the range of 0–108 μM. The limit of detection (LOD) for Cu 2+ is 5.8 μM. The concentration range for detection of AA is 0–3 mM. The LOD for AA is 0.13 mM. In addition, the application of the sensor is verified by performing detection in real samples such as fresh orange, juice, VC tablet, and lake water. This work expands the application of AuNPs-based fluorescence-quenching sensors for multi-component detection.
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危险品化学品经营许可证（带存储）