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Frontiers of Chemical Science and Engineering

, Volume 14 Issue 6

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Selective hydrogenation of acetylene over Pd/CeO2
Kai Li, Tengteng Lyu, Junyi He, Ben W. L. Jang
Front. Chem. Sci. Eng.. 2020, 14 (6): 929-936.
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Five hundred ppm Pd/CeO2 catalyst was prepared and evaluated in selective hydrogenation of acetylene in large excess of ethylene since ceria has been recently found to be a reasonable stand-alone catalyst for this reaction. Pd/CeO2 catalyst could be activated in situ by the feed gas during reactions and the catalyst without reduction showed much better ethylene selectivity than the reduced one in the high temperature range due to the formation of oxygen vacancies by reduction. Excellent ethylene selectivity of ~100% was obtained in the whole reaction temperature range of 50°C–200°C for samples calcined at temperatures of 600°C and 800°C. This could be ascribed to the formation of PdxCe1xO2−y or Pd-O-Ce surface species based on the X-ray diffraction and X-ray photoelectron spectroscopy results, indicating the strong interaction between palladium and ceria.

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Room temperature oxidation of acetone by ozone over alumina-supported manganese and cobalt mixed oxides
Mehraneh Ghavami, Mostafa Aghbolaghy, Jafar Soltan, Ning Chen
Front. Chem. Sci. Eng.. 2020, 14 (6): 937-947.
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Volatile organic compounds (VOCs) are among the major sources of air pollution. Catalytic ozonation is an efficient process for removing VOCs at lower reaction temperature compared to catalytic oxidation. In this study, a series of alumina supported single and mixed manganese and cobalt oxides catalysts were used for ozonation of acetone at room temperature. The influence of augmenting the single Mn and Co catalysts were investigated on the performance and structure of the catalyst. The manganese and cobalt single and mixed oxides catalysts of the formula Mn10%-CoX and Co10%-MnX (where X= 0, 2.5%, 5%, or 10%) were prepared. It was found that addition of Mn and Co at lower loading levels (2.5% or 5%) to single metal oxide catalysts enhanced the catalytic activity. The mixed oxides catalysts of (Mn10%-Co2.5%) and (Mn10%-Co5%) led to acetone conversion of about 84%. It is concluded that lower oxidation state of the secondary metal improves ozone decomposition and oxidation of acetone.

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Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation
Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan
Front. Chem. Sci. Eng.. 2020, 14 (6): 948-955.
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Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions, including the oxygen evolution reaction (OER) and glucose oxidation reaction (GOR). Herein, we prepared cobalt hydroxide nanoparticles (CoHP) and cobalt hydroxide nanosheets (CoHS) on nickel foam. In the electrocatalytic OER, CoHS shows an overpotential of 306 mV at a current density of 10 mA·cm–2. This is enhanced as compared with that of CoHP (367 mV at 10 mA·cm–2). In addition, CoHS also exhibits an improved performance in the electrocatalytic GOR. The improved electrocatalytic performance of CoHS could be due to the higher ability of the two-dimensional nanosheets on CoHS in electron transfer. These results are useful for fabricating efficient catalysts for electrocatalytic oxidation reactions.

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Efficient degradation of orange II by ZnMn2O4 in a novel photo-chemical catalysis system
Qingzhuo Ni, Hao Cheng, Jianfeng Ma, Yong Kong, Sridhar Komarneni
Front. Chem. Sci. Eng.. 2020, 14 (6): 956-966.
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A ZnMn2O4 catalyst has been synthesized via a sucrose-aided combustion method and characterized by various analytical techniques. It is composed of numerous nanoparticles (15–110 nm) assembled into a porous structure with a specific surface area (SSA) of 19.1 m2·g–1. Its catalytic activity has been investigated for the degradation of orange II dye using three different systems, i.e., the photocatalysis system with visible light, the chemocatalysis system with bisulfite, and the photo-chemical catalysis system with both visible light and bisulfite. The last system exhibits the maximum degradation efficiency of 90%, much higher than the photocatalysis system (15%) and the chemocatalysis system (67%). The recycling experiments indicate that the ZnMn2O4 catalyst has high stability and reusability and is thus a green and eximious catalyst. Furthermore, the potential degradation mechanisms applicable to the three systems are discussed with relevant theoretical analysis and scavenging experiments for radicals. The active species such as Mn(III), O2, h+, eaq, SO4 and HO are proposed to be responsible for the excellent degradation results in the photo-chemical catalysis system with the ZnMn2O4 catalyst.

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The preparation, characterization, and catalytic performance of porous fibrous LaFeO3 perovskite made from a sunflower seed shell template
Zhifei Wu, Li Wang, Yixiao Hu, Hui Han, Xing Li, Ying Wang
Front. Chem. Sci. Eng.. 2020, 14 (6): 967-975.
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LaFeO3 perovskite with a porous fibrous structure was successfully synthesized using a sunflower seed shell as a template. To investigate the effects of this template, a sample was prepared without a template via the same procedure. Through various characterization techniques, such as X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, N2 adsorption-desorption analysis, X-ray photoelectron spectroscopy, oxygen temperature programed desorption, and hydrogen temperature programed reduction, the physiochemical properties of the samples were investigated. The results showed that the sample made with a template had a larger surface area and a larger amount of adsorbed oxygen, which further illustrated that the sunflower seed shell template had a significant impact on the physiochemical properties of the samples. Furthermore, we explored the catalytic activity for nitric oxide (NO) oxidation, and studied the factors affecting it, which highlighted its potential application in automobile exhausts.

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Kombucha SCOBY-based carbon and graphene oxide wrapped sulfur/polyacrylonitrile as a high-capacity cathode in lithium-sulfur batteries
Krishnaveni Kalaiappan, Subadevi Rengapillai, Sivakumar Marimuthu, Raja Murugan, Premkumar Thiru
Front. Chem. Sci. Eng.. 2020, 14 (6): 976-987.
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Hierarchically-porous carbon nano sheets were prepared as a conductive additive for sulfur/polyacrylonitrile (S/PAN) composite cathodes using a simple heat treatment. In this study, kombucha (that was derived from symbiotic culture of bacteria and yeast) carbon (KC) and graphene oxide (GO) were used as a carbon host matrix. These rational-designed S/PAN/KC/GO hybrid composites greatly suppress the diffusion of polysulfides by providing strong physical and chemical adsorption. The cathode delivered an initial discharge capacity of 1652 mAh·g−1 at a 0.1 C rate and a 100th cycle capacity of 1193 mAh·g−1. The nano sheets with embedded hierarchical pores create a conductive network that provide effective electron transfer and fast electrochemical kinetics. Further, the nitrogen component of PAN can raise the affinity/interaction of the carbon host with lithium polysulfides, supporting the cyclic performance. The results exploit the cumulative contribution of both the conductive carbon matrix and PAN in the enhanced performance of the positive electrode.

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Effects of gradient concentration on the microstructure and electrochemical performance of LiNi0.6Co0.2Mn0.2O2 cathode materials
Wenming Li, Weijian Tang, Maoqin Qiu, Qiuge Zhang, Muhammad Irfan, Zeheng Yang, Weixin Zhang
Front. Chem. Sci. Eng.. 2020, 14 (6): 988-996.
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Nickel(Ni)-rich layered materials have attracted considerable interests as promising cathode materials for lithium ion batteries (LIBs) owing to their higher capacities and lower cost. Nevertheless, Mn-rich cathode materials usually suffer from poor cyclability caused by the unavoidable side-reactions between Ni4+ ions on the surface and electrolytes. The design of gradient concentration (GC) particles with Ni-rich inside and Mn-rich outside is proved to be an efficient way to address the issue. Herein, a series of LiNi0.6Co0.2Mn0.2O2 (LNCM622) materials with different GCs (the atomic ratio of Ni/Mn decreasing from the core to the outer layer) have been successfully synthesized via rationally designed co-precipitation process. Experimental results demonstrate that the GC of LNCM622 materials plays an important role in their microstructure and electrochemical properties. The as-prepared GC3.5 cathode material with optimal GC can provide a shorter pathway for lithium-ion diffusion and stabilize the near-surface region, and finally achieve excellent electrochemical performances, delivering a discharge capacity over 176 mAh·g−1 at 0.2 C rate and exhibiting capacity retention up to 94% after 100 cycles at 1 C. The rationally-designed co-precipitation process for fabricating the Ni-rich layered cathode materials with gradient composition lays a solid foundation for the preparation of high-performance cathode materials for LIBs.

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Ultrathin microcrystalline hydrogenated Si/Ge alloyed tandem solar cells towards full solar spectrum conversion
Yu Cao, Xinyun Zhu, Xingyu Tong, Jing Zhou, Jian Ni, Jianjun Zhang, Jinbo Pang
Front. Chem. Sci. Eng.. 2020, 14 (6): 997-1005.
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Thin film solar cells have been proved the next generation photovoltaic devices due to their low cost, less material consumption and easy mass production. Among them, micro-crystalline Si and Ge based thin film solar cells have advantages of high efficiency and ultrathin absorber layers. Yet individual junction devices are limited in photoelectric conversion efficiency because of the restricted solar spectrum range for its specific absorber. In this work, we designed and simulated a multi-junction solar cell with its four sub-cells selectively absorbing the full solar spectrum including the ultraviolet, green, red as well as near infrared range, respectively. By tuning the Ge content, the record efficiency of 24.80% has been realized with the typical quadruple junction structure of a-Si:H/a-Si0.9Ge0.1:H/µc-Si:H/µc-Si0.5Ge0.5:H. To further reduce the material cost, thickness dependent device performances have been conducted. It can be found that the design of total thickness of 4 mm is the optimal device design in balancing the thickness and the PCE. While the design of ultrathin quadruple junction device with total thickness of 2 mm is the optimized device design regarding cost and long-term stability with a little bit more reduction in PCE. These results indicated that our solar cells combine the advantages of low cost and high stability. Our work may provide a general guidance rule of utilizing the full solar spectrum for developing high efficiency and ultrathin multi-junction solar cells.

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Immobilization of nano-zero-valent irons by carboxylated cellulose nanocrystals for wastewater remediation
Bangxian Peng, Rusen Zhou, Ying Chen, Song Tu, Yingwu Yin, Liyi Ye
Front. Chem. Sci. Eng.. 2020, 14 (6): 1006-1017.
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Nano-zero-valent irons (nZVI) have shown great potential to function as universal and low-cost magnetic adsorbents. Yet, the rapid agglomeration and easy surface corrosion of nZVI in solution greatly hinders their overall applicability. Here, carboxylated cellulose nanocrystals (CCNC), widely available from renewable biomass resources, were prepared and applied for the immobilization of nZVI. In doing so, carboxylated cellulose nanocrystals supporting nano-zero-valent irons (CCNC-nZVI) were obtained via an in-situ growth method. The CCNC-nZVI were characterized and then evaluated for their performances in wastewater treatment. The results obtained show that nZVI nanoparticles could attach to the carboxyl and hydroxyl groups of CCNC, and well disperse on the CCNC surface with a size of ~10 nm. With the CCNC acting as corrosion inhibitors improving the reaction activity of nZVI, CCNC-nZVI exhibited an improved dispersion stability and electron utilization efficacy. The Pb(II) adsorption capacity of CCNC-nZVI reached 509.3 mg·g1 (298.15 K, pH= 4.0), significantly higher than that of CCNC. The adsorption was a spontaneous exothermic process and could be perfectly fitted by the pseudo-second-order kinetics model. This study may provide a novel and green method for immobilizing magnetic nanomaterials by using biomass-based resources to develop effective bio-adsorbents for wastewater decontamination.

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Ion-imprinted silica gel and its dynamic membrane for nickel ion removal from wastewaters
Jiehui Zeng, Jianxian Zeng, Hu Zhou, Guoqing Liu, Zhengqiu Yuan, Jian Jian
Front. Chem. Sci. Eng.. 2020, 14 (6): 1018-1028.
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An ion-imprinted sorbent (IIP) was prepared by using Ni2+ as template, 3-[2-(2-aminoethylamino) ethylamino] propyl-trimethoxysilane as functional monomer, and silica gel as carrier. The adsorption performance of IIP towards Ni2+ was investigated. IIP showed a higher adsorption capacity than that of non-imprinted sorbent, and it also exhibited high selectivity for Ni2+ in the presence of Cu2+ and Zn2+ ions. Then, IIP was used to form a dynamic membrane onto the surface of ceramic membrane for treatment of electroplating wastewater containing Ni2+. Compared with ceramic membrane, IIP dynamic membrane had much higher steady membrane flux, and also rejected Ni2+ to obtain a lower concentration of Ni2+ in the permeate fluid. Perhaps it is suitable for future practice applications.

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Synthesis of graphene oxide nanoribbons/chitosan composite membranes for the removal of uranium from aqueous solutions
Xuewen Hu, Yun Wang, Jinbo Ou Yang, Yang Li, Peng Wu, Hengju Zhang, Dingzhong Yuan, Yan Liu, Zhenyu Wu, Zhirong Liu
Front. Chem. Sci. Eng.. 2020, 14 (6): 1029-1038.
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In this study, a graphene oxide nanoribbons/chitosan (GONRs/CTS) composite membrane was successfully prepared by encapsulating CTS into GONRs, which were unzipped from multi-walled carbon nanotubes. The GONRs/CTS composite membrane so prepared was characterized using scanning electron microscopy, X-Ray diffraction and Fourier transform infrared spectroscopy. The effects of the experimental conditions such as the pH (2‒7), adsorbent dosage (10‒50 mg), experimental time (5 min–32 h), uranium concentration (25‒300 mg∙L−1), experimental temperature (298 K‒328 K) on the adsorption properties of the composite membrane for the removal of U(VI) were investigated. The results showed that the U(VI) adsorption process of the GONRs/CTS composite membrane was pH-dependent, rapid, spontaneous and endothermic. The adsorption process followed the pseudo-secondary kinetics and Langmuir models. The maximum U(VI) adsorption capacity of the GONRs/CTS composite membrane was calculated to be 320 mg∙g−1. Hence, the GONRs/CTS composite membrane prepared in this study was found to be suitable for separating and recovering uranium from wastewater.

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A thermally flexible and multi-site tactile sensor for remote 3D dynamic sensing imaging
Guoting Xia, Yinuo Huang, Fujiang Li, Licheng Wang, Jinbo Pang, Liwei Li, Kai Wang
Front. Chem. Sci. Eng.. 2020, 14 (6): 1039-1051.
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A flexible, multi-site tactile and thermal sensor (MTTS) based on polyvinylidene fluoride (resolution 50 × 50) is reported. It can be used to implement spatial mapping caused by tactile and thermal events and record the two-dimensional motion trajectory of a tracked target object. The output voltage and current signal are recorded as a mapping by sensing the external pressure and thermal radiation stimulus, and the response distribution is dynamically observed on the three-dimensional interface. Through the mapping relationship between the established piezoelectric and pyroelectric signals, the piezoelectric component and the pyroelectric component are effectively extracted from the composite signals. The MTTS has a good sensitivity for tactile and thermal detection, and the electrodes have good synchronism. In addition, the signal interference is less than 9.5% and decreases as the pressure decreases after the distance between adjacent sites exceeds 200 µm. The integration of MTTS and signal processing units has potential applications in human-machine interaction systems, health status detection and smart assistive devices.

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Mechanism of methanol decomposition on the Pd/WC(0001) surface unveiled by first-principles calculations
Jinhua Zhang, Yuanbin She
Front. Chem. Sci. Eng.. 2020, 14 (6): 1052-1064.
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In this study, the decomposition of methanol into the CO and H species on the Pd/tungsten carbide (WC)(0001) surface is systematically investigated using periodic density functional theory (DFT) calculations. The possible reaction pathways and intermediates are determined. The results reveal that saturated molecules, i.e., methanol and formaldehyde, adsorb weakly on the Pd/ WC(0001) surface. Both CO and H prefer three-fold sites, with adsorption energies of −1.51 and −2.67 eV, respectively. On the other hand, CH3O stably binds at three-fold and bridge sites, with an adsorption energy of −2.58 eV. However, most of the other intermediates tend to adsorb to the surface with the carbon and oxygen atoms in their sp3 and hydroxyl-like configurations, respectively. Hence, the C atom of CH2OH preferentially attaches to the top sites, CHOH and CH2O adsorb at the bridge sites, while COH and CHO occupy the three-fold sites. The DFT calculations indicate that the rupture of the initial C–H bond promotes the decomposition of CH3OH and CH2OH, whereas in the case of CHOH, O–H bond scission is favored over the C–H bond rupture. Thus, the most probable methanol decomposition pathway on the Pd/WC(0001) surface is CH3OH → CH2OH → trans-CHOH → CHO → CO. The present study demonstrates that the synergistic effect of WC (as carrier) and Pd (as catalyst) alters the CH3OH decomposition pathway and reduces the noble metal utilization.

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Effect of electrolyte concentration on the tribological performance of MAO coatings on aluminum alloys
Chao Wang, Jun Chen, Jihua He, Jing Jiang, Qinyong Zhang
Front. Chem. Sci. Eng.. 2020, 14 (6): 1065-1071.
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Micro-arc oxidation (MAO) is an efficient approach to improve the hardness, wear resistance, and other properties of aluminum alloys. In order to investigate the effect of the electrolyte concentration on the properties of MAO coatings for LY12 alloy, the voltage variation during the MAO process was recorded. The surface morphologies and phase compositions of the coatings produced with different electrolytes were investigated using scanning electron microscopy and X-ray diffraction, respectively. The roughness and thickness of the coatings were measured using a pocket roughness meter and an eddy-current thickness meter, respectively. The tribological performances of the coatings were investigated against GCr15 bearing steel on a ball-on-disc wear tester in open air. The results showed that with an increase in the Na2SiO3 content, the working voltage of the MAO process decreased, the roughness and thickness of the coatings increased significantly, and the relative content of the α-Al2O3 phase decreased. With an increase in the KOH content, the working voltage decreased slightly, the roughness and thickness of the coatings increased slightly, and the α- and γ-Al2O3 phase contents remained unchanged. The friction coefficient and wear rate of the coatings increased with an increase in the Na2SiO3 and KOH concentrations. A decrease in the porosity and roughness and an increase in the α-Al2O3 content of the coatings reduced their wear mass loss.

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Facile preparation of polybenzoxazine-based carbon microspheres with nitrogen functionalities: effects of mixed solvents on pore structure and supercapacitive performance
Uthen Thubsuang, Suphawadee Chotirut, Apisit Thongnok, Archw Promraksa, Mudtorlep Nisoa, Nicharat Manmuanpom, Sujitra Wongkasemjit, Thanyalak Chaisuwan
Front. Chem. Sci. Eng.. 2020, 14 (6): 1072-1086.
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In this study, polybenzoxazine (PBZ)-based carbon microspheres were prepared via a facile method using a mixture of formaldehyde (F) and dimethylformamide (DMF) as the solvent. The PBZ microspheres were successfully obtained at the F/DMF weight ratios of 0.4 and 0.6. These microspheres exhibited high nitrogen contents after carbonization. The microstructures of all the samples showed an amorphous phase and a partial graphitic phase. The porous carbon with the F/DMF ratio of 0.4 showed significantly higher specific capacitance (275.1 Fg‒1) than the reference carbon (198.9 Fg‒1) at 0.05 Ag‒1. This can be attributed to the synergistic electrical double-layer capacitor and pseudo-capacitor behaviors of the porous carbon with the F/DMF ratio of 0.4. The presence of nitrogen/oxygen functionalities induced pseudo-capacitance in the microspheres, and hence increased their total specific capacitance. After activation with CO2, the specific surface area of the carbon microspheres with the F/DMF ratio of 0.4 increased from 349 to 859 m2g‒1 and the specific capacitance increased to 424.7 Fg‒1. This value is approximately two times higher than that of the reference carbon. The results indicated that the F/DMF ratio of 0.4 was suitable for preparing carbon microspheres with good supercapacitive performance. The nitrogen/oxygen functionalities and high specific surface area of the microspheres were responsible for their high capacitance.

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High-gravity-assisted emulsification for continuous preparation of waterborne polyurethane nanodispersion with high solids content
Weihong Zhang, Dan Wang, Jie-Xin Wang, Yuan Pu, Jian-Feng Chen
Front. Chem. Sci. Eng.. 2020, 14 (6): 1087-1099.
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In this work, we developed a continuous preparation strategy for the production of high-solids-content waterborne polyurethane (WPU) emulsions via high-gravity-assisted emulsification in a rotating packed bed (RPB) reactor. By adjusting the experimental parameters and formula, WPU emulsions with a high solids content of 55% and a low viscosity were prepared. Preliminary applications of the high-solids-content WPU as a thermally insulating material were demonstrated. RPB emulsification is an economical and environmentally friendly production strategy because of the low energy consumption, short emulsification time, and effective devolatilization. This study demonstrated an effective method for preparation of high-solids-content WPU, moving toward commercialization and industrialization.

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Catalytic process modeling and sensitivity analysis of alkylation of benzene with ethanol over MIL-101(Fe) and MIL-88(Fe)
Ehsan Rahmani, Mohammad Rahmani
Front. Chem. Sci. Eng.. 2020, 14 (6): 1100-1111.
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A solvothermal method was used to synthesize MIL-101(Fe) and MIL-88(Fe), which were used for alkylation of benzene. The synthesized catalysts were characterized by X-ray diffraction, Fourier transform infrared spectroscopy, field emission scanning electron microscope, dynamic light scattering, and BET techniques. Metal-organic frameworks (MOFs) were modeled to investigate the catalytic performance and existence of mass transfer limitations. Calculated effectiveness factors revealed absence of internal and external mass transfer. Sensitivity analysis revealed best operating conditions over MIL-101 at 120°C and 5 bar and over MIL-88 at 142°C and 9 bar.

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Supramolecular self-assembly of two-component systems comprising aromatic amides/Schiff base and tartaric acid
Xin Wang, Wei Cui, Bin Li, Xiaojie Zhang, Yongxin Zhang, Yaodong Huang
Front. Chem. Sci. Eng.. 2020, 14 (6): 1112-1121.
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The gelating properties and thermotropic behaviors of stoichiometric mixtures of aromatic amides 1, 2, and the aromatic Schiff base 3 with tartaric acid (TA) were investigated. Among the three gelators, 2-TA exhibited superior gelating ability. Mixture 2-TA exhibits a smectic B phase and an unidentified smectic mesophase during both heating and cooling runs. The results of Fourier transform infrared spectroscopy and X-ray diffraction revealed the existence of hydrogen bonding and p-p interactions in 2-TA systems, which are likely to be the dominant driving forces for the supramolecular self-assembly. Additionally, it was established that all of the studied gel self-assemblies and mesophases possess a lamellar structure. The anion response ability of the tetrahydrofuran gel of 2-TA was evaluated and it was found that it was responsive to the stimuli of F, Cl, Br, I, AcO.

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Novel engineered proteins for mechanomaterials
Giuseppe Portale
Front. Chem. Sci. Eng.. 2020, 14 (6): 1122-1123.
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Efficient elimination of environmental pollutants through sorption-reduction and photocatalytic degradation using nanomaterials
Njud S. Alharbi, Baowei Hu, Tasawar Hayat, Samar Omar Rabah, Ahmed Alsaedi, Li Zhuang, Xiangke Wang
Front. Chem. Sci. Eng.. 2020, 14 (6): 1124-1135.
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With the rapid development of industrial, large amounts of different inorganic and organic pollutants are released into the natural environments. The efficient elimination of environmental pollutants, i.e., photocatalytic degradation of persistent organic pollutants into nontoxic organic/inorganic chemicals, in-situ solidification or sorption-reduction of heavy metal ions, is crucial to protect the environment. Nanomaterials with large surface area, active sites and abundant functional groups could form strong surface complexes with different kinds of pollutants and thereby could efficiently eliminate the pollutants from the aqueous solutions. In this review, we mainly focused on the recent works about the synthesis of nanomaterials and their applications in the efficient elimination of different organic and inorganic pollutants from wastewater and discussed the interaction mechanism from batch experimental results, the advanced spectroscopy techniques and theoretical calculations. The adsorption and the photocatalytic reduction of organic pollutants and the sorption/reduction of heavy metal ions are generally considered as the main methods to decrease the concentration of pollutants in the natural environment. This review highlights a new way for the real applications of novel nanomaterials in environmental pollution management, especially for the undergraduate students to understand the recent works in the elimination of different kinds of inorganic and organic chemicals in the natural environmental pollution management.

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