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  • RESEARCH ARTICLE
    Iulian Patrașcu, Costin S. Bîldea, Anton A. Kiss
    Frontiers of Chemical Science and Engineering, 2022, 16(2): 316-331. https://doi.org/10.1007/s11705-021-2047-9

    Dimethyl carbonate is an eco-friendly essential chemical that can be sustainably produced from CO2, which is available from carbon capture activities or can even be captured from the air. The rapid increase in dimethyl carbonate demand is driven by the fast growth of polycarbonates, solvent, pharmaceutical, and lithium-ion battery industries. Dimethyl carbonate can be produced from CO2 through various chemical pathways, but the most convenient route reported is the indirect alcoholysis of urea. Previous research used techniques such as heat integration and reactive distillation to reduce the energy use and costs, but the use of an excess of methanol in the trans-esterification step led to an energy intensive extractive distillation required to break the dimethyl carbonate-methanol azeotrope. This work shows that the production of dimethyl carbonate by indirect alcoholysis of urea can be improved by using an excess of propylene carbonate (instead of an excess of methanol), a neat feat that we showed it requires only 2.64 kW·h·kg–1 dimethyl carbonate in a reaction-separation-recycle process, and a reactive distillation column that effectively replaces two conventional distillation columns and the reactor for dimethyl carbonate synthesis. Therefore, less equipment is required, the methanol-dimethyl carbonate azeotrope does not need to be recycled, and the overall savings are higher. Moreover, we propose the use of a reactive distillation column in a heat integrated process to obtain high purity dimethyl carbonate (>99.8 wt-%). The energy requirement is reduced by heat integration to just 1.25 kW·h·kg–1 dimethyl carbonate, which is about 52% lower than the reaction-separation-recycle process. To benefit from the energy savings, the dynamics and control of the process are provided for ±10% changes in the nominal rate of 32 ktpy dimethyl carbonate, and for uncertainties in reaction kinetics.

  • REVIEW ARTICLE
    Huan Wang, Guo Du, Jiaqing Jia, Shaohua Chen, Zhipeng Su, Rui Chen, Tiehong Chen
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1444-1461. https://doi.org/10.1007/s11705-021-2090-6

    Hierarchically porous zeolites are promising candidates in catalytic conversion of relatively bulky molecules, and their syntheses have attracted significant attention. From both industrial and scientific perspectives, different carbon materials have been widely employed as hard templates for the preparation of hierarchically porous zeolites during the past two decades. In this review, the progress in synthetic strategies using carbon materials as templates is comprehensively summarized. Depending on the affinity between the carbon templates and zeolite precursors, the substantial strategies for synthesizing hierarchical zeolites are introduced in direct templates and indirect templates. Direct templates methods, by which the carbon materials are directly mixed with precursors gel as hard templates, are first reviewed. Then, we discuss the indirect templates method (crystallization of carbon-silica composites), by which the carbon is produced by in situ pyrolysis of organic-inorganic precursors. In addition, the technique of encapsulating metal species into zeolites crystals with the assistance of carbon templates is also discussed. In the conclusion part, the factors affecting the synthesis of carbon-templated hierarchically porous zeolites are remarked. This review is expected to attract interest in the synthesis strategies of hierarchically porous zeolites, especially cost-effective and large-scale production methodologies, which are essential to the industrial application of hierarchical zeolites.

  • RESEARCH ARTICLE
    Ewan Chee, Wee Chin Wong, Xiaonan Wang
    Frontiers of Chemical Science and Engineering, 2022, 16(2): 237-250. https://doi.org/10.1007/s11705-021-2058-6

    Advanced model-based control strategies, e.g., model predictive control, can offer superior control of key process variables for multiple-input multiple-output systems. The quality of the system model is critical to controller performance and should adequately describe the process dynamics across its operating range while remaining amenable to fast optimization. This work articulates an integrated system identification procedure for deriving black-box nonlinear continuous-time multiple-input multiple-output system models for nonlinear model predictive control. To showcase this approach, five candidate models for polynomial and interaction features of both output and manipulated variables were trained on simulated data and integrated into a nonlinear model predictive controller for a highly nonlinear continuous stirred tank reactor system. This procedure successfully identified system models that enabled effective control in both servo and regulator problems across wider operating ranges. These controllers also had reasonable per-iteration times of ca. 0.1 s. This demonstration of how such system models could be identified for nonlinear model predictive control without prior knowledge of system dynamics opens further possibilities for direct data-driven methodologies for model-based control which, in the face of process uncertainties or modelling limitations, allow rapid and stable control over wider operating ranges.

  • RESEARCH ARTICLE
    Weiguang Lv, Xiaohong Zheng, Li Li, Hongbin Cao, Yi Zhang, Renjie Chen, Hancheng Ou, Fei Kang, Zhi Sun
    Frontiers of Chemical Science and Engineering, 2021, 15(5): 1243-1256. https://doi.org/10.1007/s11705-020-2029-3

    Spent lithium-ion battery recycling has attracted significant attention because of its importance in regard to the environment and resource importance. Traditional hydrometallurgical methods usually leach all valuable metals and subsequently extract target meals to prepare corresponding materials. However, Li recovery in these processes requires lengthy operational procedures, and the recovery efficiency is low. In this research, we demonstrate a method to selectively recover lithium before the leaching of other elements by introducing a hydrothermal treatment. Approximately 90% of Li is leached from high-Ni layered oxide cathode powders, while consuming a nearly stoichiometric amount of hydrogen ions. With this selective recovery of Li, the transition metals remain as solid residue hydroxides or oxides. Furthermore, the extraction of Li is found to be highly dependent on the content of transition metals in the cathode materials. A high leaching selectivity of Li (>98%) and nearly 95% leaching efficiency of Li can be reached with LiNi0.8Co0.1Mn0.1O2. In this case, both the energy and material consumption during the proposed Li recovery is significantly decreased compared to traditional methods; furthermore, the proposed method makes full use of H+ to leach Li+. This research is expected to provide new understanding for selectively recovering metal from secondary resources.

  • REVIEW ARTICLE
    Qifeng Lei, Chang Wang, Weili Dai, Guangjun Wu, Naijia Guan, Landong Li
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1462-1486. https://doi.org/10.1007/s11705-021-2099-x

    Multifunctional heteroatom zeolites have drawn broad attentions due to the possible synergistic effects in the catalytic reactions. Remarkable achievements have been made on the synthesis, characterization and catalytic applications of multifunctional heteroatom zeolite, while a review on this important topic is still missing. Herein, current research status of multifunctional heteroatom zeolites is briefly summarized, aiming to boost further researches. First, the synthesis strategies toward heteroatom zeolites are introduced, including the direct synthesis and postsynthesis routes; then, the spectroscopic techniques to identify the existing states of heteroatom sites and the corresponding physiochemical properties are shown and compared; finally, the catalytic applications of multifunctional heteroatom zeolites in various chemical reactions, especially in one-step tandem reactions, are discussed.

  • RESEARCH ARTICLE
    Wenjing Zhang, Xiaoxue Yuan, Xuehua Yan, Mingyu You, Hui Jiang, Jieyu Miao, Yanli Li, Wending Zhou, Yihan Zhu, Xiaonong Cheng
    Frontiers of Chemical Science and Engineering, 2022, 16(3): 420-432. https://doi.org/10.1007/s11705-021-2065-7

    Production cost, capacitance, and electrode materials safety are the key factors to be concerned about for supercapacitors. In this work, a type of carbon nanosheets was produced through the carbonization of tripotassium citrate monohydrate and nitric acidification. Subsequently, a well-designed manganese dioxide/carbon nanosheets composite was synthesized through hydrothermal treating. The carbon nanosheets served as the substrate for growing the manganese dioxide, regulating its distribution, and preventing it from inhomogeneous dimensions and severe agglomeration. Many manganese dioxide nanosheets grew vertically on the numerous functional groups generated on the surface of the carbon nanosheets during acidification. The synergistic combination of carbon nanosheets and manganese dioxide tailors the electrochemical performance of the composite, which benefits from the excellent conductivity and stability of carbon nanosheets. The carbon nanosheets derived from tripotassium citrate monohydrate are conducive to the remarkable performance of manganese dioxide/carbon nanosheets electrode. Finally, an asymmetric supercapacitor with active carbon as the cathode and manganese dioxide/carbon nanosheets as the anode was assembled, achieving an outstanding energy density of 54.68 Wh·kg–1 and remarkable power density of 6399.2 W·kg–1 superior to conventional lead-acid batteries. After 10000 charge-discharge cycles, the device retained 75.3% of the initial capacitance, showing good cycle stability. Two assembled asymmetric supercapacitors in series charged for 3 min could power a yellow light emitting diode with an operating voltage of 2 V for 2 min. This study may provide valuable insights for applying carbon materials and manganese dioxide in the energy storage field.

  • REVIEW ARTICLE
    Xiangsheng Liu, Hui Sun, Xueqing Wang, Huan Meng
    Frontiers of Chemical Science and Engineering, 2022, 16(3): 333-344. https://doi.org/10.1007/s11705-021-2059-5

    Compared to conventional hyperthermia that is limited by low selectivity and severe side effects, nano-enabled hyperthermia yields great potentials to tackle these limitations for cancer treatment. Another major advance is the observation of immunological responses associated with nano-enabled hyperthermia, which introduces a new avenue, allowing a potential paradigm shift from the acutely effective and cytotoxicity-centric response to the next-phase discovery, i.e., long-lasting and/or systemic anti-tumor immunity. This perspective first discusses the temperature-gradient and the spatially-structured immunological landscape in solid tumors receiving nano-enabled hyperthermia. This includes the discussion about underlying mechanism such as immunogenic cell death, which initiates a profound immunological chain reaction. In order to propagate the immune activation as a viable therapeutic principle, we further discussed the tumor type-specific complexity in the immunological tumor microenvironment, including the creative design of nano-enabled combination therapy to synergize with nano-enabled hyperthermia.

  • RESEARCH ARTICLE
    Yinteng Shi, Lin Ai, Haonan Shi, Xiaoyu Gu, Yujun Han, Jixiang Chen
    Frontiers of Chemical Science and Engineering, 2022, 16(4): 443-460. https://doi.org/10.1007/s11705-021-2079-1

    Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n-pentadecane and n-C6n-C16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO2 recovered the catalyst reactivity.

  • REVIEW ARTICLE
    Soheil Bahraminia, Mansoor Anbia, Esmat Koohsaryan
    Frontiers of Chemical Science and Engineering, 2021, 15(5): 1050-1074. https://doi.org/10.1007/s11705-020-2025-7

    Natural gas and biogas are two mixtures that consist of methane as their main component. These two gas mixtures are usually saturated with water vapor, which cause many problems, such as damaging the gas processing equipment by increasing the gas’s corrosion potential or clogging the pipelines due to gas hydrate formation. Thus, removing water vapor from these gas streams is mandatory. In this review paper, the main dehydration methods have been overviewed, and scrutiny of the adsorption dehydration has been carried out. Furthermore, the most important solid desiccants and their improvements have been reviewed.

  • RESEARCH ARTICLE
    Wanyue Liu, Xiaoqin Liu, Jinming Chang, Feng Jiang, Shishi Pang, Hejun Gao, Yunwen Liao, Sheng Yu
    Frontiers of Chemical Science and Engineering, 2021, 15(5): 1185-1196. https://doi.org/10.1007/s11705-020-2032-8

    The magnetic nitrogen-doped carbon (MNC) was prepared from polypyrrole by a simple high temperature calcination process in this paper. The structure and properties of MNC were analyzed by scanning electron microscope, Fourier transform infrared spectroscopy, X-ray diffraction, Brunner-Emmet-Teller, vibrating sample magnetometer, and X-ray photoelectron spectroscopy. The capacity of MNC to adsorb Cr(VI) and Pb(II) was evaluated. The effects of the initial pH, dosage, concentration and temperature on the adsorption capacity of MNC were measured. MNC had a large specific surface area and a special porous structure. Its nitrogen and carbon sources were rich, and the ratio of carbon to nitrogen was fixed. The maximum Cr(VI)-adsorption capacity and maximum Pb(II) adsorption capacity of MNC could reach 456.63 and 507.13 mg∙g1 at 318 K, respectively. The pseudo-second-order model was used to describe the adsorption kinetics of MNC, and the Freundlich model was employed to discuss its isotherms. The adsorption process was affected by the electrostatic force, the reducing reaction, pores and chelation. The results of this study suggest that MNC is a material with superior performance, and is very easily regenerated, reused, and separated in the adsorption process.

  • RESEARCH ARTICLE
    Pingle Liu, Yu Liu, Yang Lv, Wei Xiong, Fang Hao, Hean Luo
    Frontiers of Chemical Science and Engineering, 2022, 16(4): 461-474. https://doi.org/10.1007/s11705-021-2072-8

    The catalytic hydrogenation of nitroaromatics is an environmentally friendly technology for aniline production, and it is crucial to develop noble-metal-free catalysts that can achieve chemoselective hydrogenation of nitroaromatics under mild reaction conditions. In this work, zinc-modified Ni-Ti catalysts (NixZnyTi1) were fabricated and applied for the hydrogenation of nitroaromatics hydrogenation. It was found that the introduction of zinc effectively increases the surface Ni density, enhances the electronic effect, and improves the interaction between Ni and TiO2, resulting in smaller Ni particle size, more oxygen vacancies, higher dispersion and greater concentration of Ni on the catalyst surface. Furthermore, the electron-rich Niδ obtained by electron transfer from Zn and Ti to Ni effectively adsorbs and dissociates hydrogen. The results reveal that NixZnyTi1 (Ni0.5Zn0.5Ti1) shows excellent catalytic performance under mild conditions (70 °C and 6 bar). These findings provide a rational strategy for the development of highly active non-noble-metal hydrogenation catalysts.

  • RESEARCH ARTICLE
    Shan Wang, Xuelian Xu, Ping Xiao, Junjiang Zhu, Xinying Liu
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1524-1536. https://doi.org/10.1007/s11705-021-2106-2

    The effects of Zr doping on the existence of Cu and the catalytic performance of Ce0.7−xZrxCu0.3O2 for CO oxidation were investigated. The characterization results showed that all samples have a cubic structure, and a small amount of Zr doping facilitates Cu2+ ions entering the CeO2 lattice, but excessive Zr doping leads to the formation of surface CuO crystals again. Thus, the number of oxygen vacancies caused by the Cu2+ entering the lattice (e.g., Cu2+–□–Ce4+; □: oxygen vacancy), and the amount of reducible copper species caused by CuO crystals, varies with the Zr doping. Catalytic CO oxidation tests indicated that the oxygen vacancy and the reducible copper species were the adsorption and activation sites of O2 and CO, respectively, and the cooperative effects between them accounted for the high CO oxidation activity. Thus, the samples x = 0.1 and 0.3, which possessed the most oxygen vacancy or reducible copper species, showed the best activity for CO oxidation, with full CO conversion obtained at 110 °C. The catalyst is also stable and has good resistance to water during the reaction.

  • REVIEW ARTICLE
    Xiang-Hui Yu, Jin-Long Yi, Ru-Liang Zhang, Feng-Yun Wang, Lei Liu
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1380-1407. https://doi.org/10.1007/s11705-021-2097-z

    Hollow carbon spheres have garnered great interest owing to their high surface area, large surface-to-volume ratio and reduced transmission lengths. Herein, we overview hollow carbon sphere-based materials and their noble metal-free hybrids in catalysis. Firstly, we summarize the key fabrication techniques for various kinds of hollow carbon spheres, with a particular emphasis on controlling pore structure and surface morphology, and then heterogeneous doping as well as their metal-free/containing hybrids are presented; next, possible applications for non-noble metal/hollow carbon sphere hybrids in the area of energy-related catalysis, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, water splitting, rechargeable Zn-air batteries and pollutant degradation are discussed; finally, we introduce the various challenges and opportunities offered by hollow carbon spheres from the perspective of synthesis and catalysis.

  • REVIEW ARTICLE
    Weihang Sun, Dongfang Liu, Minghui Zhang
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1427-1443. https://doi.org/10.1007/s11705-021-2108-0

    The dye industry produces a large amount of hazardous wastewater every day worldwide, which brings potential threaten to the global environment. As an excellent method for removal of water chroma and chemical oxygen demand, electrocatalytic methods are currently widely used in the treatment of dye wastewater. The selection and preparation of electrode materials and electrocatalysts play an important role on the electrocatalytic treatment. The aim of this paper is to introduce the most excellent high-efficiency electrode materials and electrocatalysts in the field of dye wastewater treatment. Many electrode materials such as metal electrode materials, boron-doped diamond anode materials and three-dimensional electrode are introduced in detail. Besides, the mechanism of electrocatalytic oxidation is summarized. The composite treatment of active electrode and electrocatalyst are extensively examined. Finally, the progress of photo-assisted electrocatalytic methods of dye wastewater and the catalysts are described.

  • RESEARCH ARTICLE
    Ao Yang, Yang Su, Tao Shi, Jingzheng Ren, Weifeng Shen, Teng Zhou
    Frontiers of Chemical Science and Engineering, 2022, 16(2): 303-315. https://doi.org/10.1007/s11705-021-2044-z

    An energy-efficient triple-column extractive distillation process is developed for recovering tetrahydrofuran and ethyl acetate from industrial effluent. The process development follows a rigorous hierarchical design procedure that involves entrainer design, thermodynamic analysis, process design and optimization, and heat integration. The computer-aided molecular design method is firstly used to find promising entrainer candidates and the best one is determined via rigorous thermodynamic analysis. Subsequently, the direct and indirect triple-column extractive distillation processes are proposed in the conceptual design step. These two extractive distillation processes are then optimized by employing an improved genetic algorithm. Finally, heat integration is performed to further reduce the process energy consumption. The results indicate that the indirect extractive distillation process with heat integration shows the highest performance in terms of the process economics.

  • EDITORIAL
    Zhong-Yong Yuan
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1357-1359. https://doi.org/10.1007/s11705-021-2119-x
  • RESEARCH ARTICLE
    Yunpeng Shang, Xiaohong Sun, Zhe Chen, Kunzhou Xiong, Yunmei Zhou, Shu Cai, Chunming Zheng
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1500-1513. https://doi.org/10.1007/s11705-021-2086-2

    As a hybrid energy storage device of lithium-ion batteries and supercapacitors, lithium-ion capacitors have the potential to meet the demanding needs of energy storage equipment with both high power and energy density. In this work, to solve the obstacle to the application of lithium-ion capacitors, that is, the balancing problem of the electrodes kinetic and capacity, two electrodes are designed and adequately matched. For the anode, we introduced in situ carbon-doped and surface-enriched unsaturated sulfur into the graphene conductive network to prepare transition metal sulfides, which enhances the performance with a faster lithium-ion diffusion and dominant pseudocapacitive energy storage. Therefore, the lithium-ion capacitors anode material delivers a remarkable capacity of 810 mAh∙g–1 after 500 cycles at 1 A∙g–1. On the other hand, the biomass-derived porous carbon as the cathode also displays a superior capacity of 114.2 mAh∙g–1 at 0.1 A∙g–1. Benefitting from the appropriate balance of kinetic and capacity between two electrodes, the lithium-ion capacitors exhibits superior electrochemical performance. The assembled lithium-ion capacitors demonstrate a high energy density of 132.9 Wh∙kg–1 at the power density of 265 W∙kg–1, and 50.0 Wh∙kg–1 even at 26.5 kW∙kg–1. After 10000 cycles at 1 A∙g–1, lithium-ion capacitors still demonstrate the high energy density retention of 81.5%.

  • REVIEW ARTICLE
    Giuseppe Sanzone, Jinlong Yin, Hailin Sun
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1360-1379. https://doi.org/10.1007/s11705-021-2101-7

    Many research works have demonstrated that the combination of atomically precise cluster deposition and theoretical calculations is able to address fundamental aspects of size-effects, cluster-support interactions, and reaction mechanisms of cluster materials. Although the wet chemistry method has been widely used to synthesize nanoparticles, the gas-phase synthesis and size-selected strategy was the only method to prepare supported metal clusters with precise numbers of atoms for a long time. However, the low throughput of the physical synthesis method has severely constrained its wider adoption for catalysis applications. In this review, we introduce the latest progress on three types of cluster source which have the most promising potential for scale-up, including sputtering gas aggregation source, pulsed microplasma cluster source, and matrix assembly cluster source. While the sputtering gas aggregation source is leading ahead with a production rate of ~20 mg·h–1, the pulsed microplasma source has the smallest physical dimensions which makes it possible to compact multiple such devices into a small volume for multiplied production rate. The matrix assembly source has the shortest development history, but already show an impressive deposition rate of ~10 mg·h–1. At the end of the review, the possible routes for further throughput scale-up are envisaged.

  • RESEARCH ARTICLE
    Haoqin Fang, Jianzhao Zhou, Zhenyu Wang, Ziqi Qiu, Yihua Sun, Yue Lin, Ke Chen, Xiantai Zhou, Ming Pan
    Frontiers of Chemical Science and Engineering, 2022, 16(2): 274-287. https://doi.org/10.1007/s11705-021-2043-0

    Modeling and optimization is crucial to smart chemical process operations. However, a large number of nonlinearities must be considered in a typical chemical process according to complex unit operations, chemical reactions and separations. This leads to a great challenge of implementing mechanistic models into industrial-scale problems due to the resulting computational complexity. Thus, this paper presents an efficient hybrid framework of integrating machine learning and particle swarm optimization to overcome the aforementioned difficulties. An industrial propane dehydrogenation process was carried out to demonstrate the validity and efficiency of our method. Firstly, a data set was generated based on process mechanistic simulation validated by industrial data, which provides sufficient and reasonable samples for model training and testing. Secondly, four well-known machine learning methods, namely, K-nearest neighbors, decision tree, support vector machine, and artificial neural network, were compared and used to obtain the prediction models of the processes operation. All of these methods achieved highly accurate model by adjusting model parameters on the basis of high-coverage data and properly features. Finally, optimal process operations were obtained by using the particle swarm optimization approach.

  • RESEARCH ARTICLE
    Linlin You, Yandong Guo, Yanjing He, Feng Huo, Shaojuan Zeng, Chunshan Li, Xiangping Zhang, Xiaochun Zhang
    Frontiers of Chemical Science and Engineering, 2022, 16(2): 141-151. https://doi.org/10.1007/s11705-020-2009-7

    Ionic liquid (IL)/polyimide (PI) composite membranes demonstrate promise for use in CO2 separation applications. However, few studies have focused on the microscopic mechanism of CO2 in these composite systems, which is important information for designing new membranes. In this work, a series of systems of CO2 in 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide composited with 4,4-(hexafluoroisopropylidene) diphthalic anhydride (6FDA)-based PI, 6FDA-2,3,5,6-tetramethyl-1,4-phenylene-diamine, at different IL concentrations were investigated by all-atom molecular dynamics simulation. The formation of IL regions in PI was found, and the IL regions gradually became continuous channels with increasing IL concentrations. The analysis of the radial distribution functions and hydrogen bond numbers demonstrated that PI had a stronger interaction with cations than anions. However, the hydrogen bonds among PI chains were destroyed by the addition of IL, which was favorable for transporting CO2. Furthermore, the self-diffusion coefficient and free energy barrier suggested that the diffusion coefficient of CO2 decreased with increasing IL concentrations up to 35 wt-% due to the decrease of the fractional free volume of the composite membrane. However, the CO2 self-diffusion coefficients increased when the IL contents were higher than 35 wt-%, which was attributed to the formation of continuous IL domain that benefitted the transportation of CO2.

  • RESEARCH ARTICLE
    Qilei Liu, Yinke Jiang, Lei Zhang, Jian Du
    Frontiers of Chemical Science and Engineering, 2022, 16(2): 152-167. https://doi.org/10.1007/s11705-021-2060-z

    Chemical industry is always seeking opportunities to efficiently and economically convert raw materials to commodity chemicals and higher value-added chemical-based products. The life cycles of chemical products involve the procedures of conceptual product designs, experimental investigations, sustainable manufactures through appropriate chemical processes and waste disposals. During these periods, one of the most important keys is the molecular property prediction models associating molecular structures with product properties. In this paper, a framework combining quantum mechanics and quantitative structure-property relationship is established for fast molecular property predictions, such as activity coefficient, and so forth. The workflow of framework consists of three steps. In the first step, a database is created for collections of basic molecular information; in the second step, quantum mechanics-based calculations are performed to predict quantum mechanics-based/derived molecular properties (pseudo experimental data), which are stored in a database and further provided for the developments of quantitative structure-property relationship methods for fast predictions of properties in the third step. The whole framework has been carried out within a molecular property prediction toolbox. Two case studies highlighting different aspects of the toolbox involving the predictions of heats of reaction and solid-liquid phase equilibriums are presented.

  • RESEARCH ARTICLE
    Guiqin Bai, Jianzhong Xia, Bing Cao, Rui Zhang, Junquan Meng, Pei Li
    Frontiers of Chemical Science and Engineering, 2022, 16(5): 709-719. https://doi.org/10.1007/s11705-021-2078-2

    Pervaporation desalination has a unique advantage to recycle concentrated salt solutions. The merit can be applied to treat alkaline wastewater if the membrane has superior alkali-resistance. In this paper, we used polyethylene microfiltration membrane as the substrate and deposited a glutaraldehyde crosslinked sodium carboxymethylcellulose layer by spray-coating. Pervaporation flux of the composite membrane reached 35 ± 2 kg·m–2·h–1 with a sodium chloride rejection of 99.9% ± 0.1% when separating a 3.5 wt-% sodium chloride solution at 70 °C. The desalination performance was stable after soaking the membrane in a 20 wt-% NaOH solution at room temperature for 9 d and in a 10 wt-% NaOH solution at 60 °C for 80 h. Moreover, the membrane was stable in 4 wt-% sulfuric acid and a 500 mg·L−1 sodium hypochlorite solution. In a process of concentrating a NaOH solution from 5 to 10 wt-% at 60 °C, an average water flux of 23 kg·m–2·h–1 with a NaOH rejection over 99.98% was obtained.

  • RESEARCH ARTICLE
    Wei Wang, Linlin Song, Huoli Zhang, Guanghui Zhang, Jianliang Cao
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1537-1549. https://doi.org/10.1007/s11705-021-2094-2

    Human health is deteriorating due to the effluent containing heavy metal ions and organic dyes. Hence, photoreduction of Cr(VI) to Cr(III) and degradation of rhodamine B (RhB) using a novel photocatalyst is particularly important. In this work, h-BN/NiS2/NiS composites were prepared via a simple solvothermal method and a double Z-scheme heterojunction was constructed for efficiently removing RhB and Cr(VI). The 7 wt-% h-BN/NiS2/NiS composites were characterized via a larger specific surface area (15.12 m2·g–1), stronger light absorption capacity, excellent chemical stability, and high yield of electrons and holes. The experimental result indicated that the photoreduction efficiency of the 7 wt-% h-BN/NiS2/NiS photocatalyst achieved 98.5% for Cr(VI) after 120 min, which was about 3 times higher than that of NiS2/NiS (34%). However, the removal rate of RhB by the 7 wt-% h-BN/NiS2/NiS photocatalyst reached 80%. This is due to the double Z-scheme heterojunction formed between NiS2/NiS and h-BN, which improved the charge separation efficiency and transmission efficiency. Besides, the influence of diverse photogenerated electron and hole scavengers upon the photoreduction of Cr(VI) was studied, the results indicated that graphene-like h-BN promoted transportation of photoinduced charges on the surface of the h-BN/NiS2/NiS photocatalyst via the interfacial effects.

  • REVIEW ARTICLE
    Faheem Mushtaq, Xiang Zhang, Ka Y. Fung, Ka M. Ng
    Frontiers of Chemical Science and Engineering, 2021, 15(5): 1033-1049. https://doi.org/10.1007/s11705-020-2002-1

    In chemical product design, the aim is to formulate a product with desired performance. Ingredients and internal product structure are two key drivers of product performance with direct impact on the mechanical, electrical, and thermal properties. Thus, there is a keen interest in elucidating the dependence of product performance on ingredients, structure, and the manufacturing process to form the structure. Design of product structure, particularly microstructure, is an intrinsically complex problem that involves different phases of different physicochemical properties, mass fraction, morphology, size distribution, and interconnectivity. Recently, computational methods have emerged that assist systematic microstructure quantification and prediction. The objective of this paper is to review these computational methods and to show how these methods as well as other developments in product design can work seamlessly in a proposed performance, ingredients, structure, and manufacturing process framework for the design of structured chemical products. It begins with the desired target properties and key ingredients. This is followed by computation for microstructure and then selection of processing steps to realize this microstructure. The framework is illustrated with the design of nanodielectric and die attach adhesive products.

  • RESEARCH ARTICLE
    Yong Luo, Yuhui Xie, Renjie Chen, Ruizhi Zheng, Hua Wu, Xinxin Sheng, Delong Xie, Yi Mei
    Frontiers of Chemical Science and Engineering, 2021, 15(5): 1332-1345. https://doi.org/10.1007/s11705-021-2035-0

    Design and exploitation of flame retardant polymers with high electrical conductivity are desired for polymer applications in electronics. Herein, a novel phosphorus-nitrogen intumescent flame retardant was synthesized from pentaerythritol octahydrogen tetraphosphate, phenylphosphonyl dichloride, and aniline. Low-density polyethylene was combined with the flame retardant and multi-walled carbon nanotubes to form a nanocomposite material via a ball-milling and hot-pressing method. The electrical conductivity, mechanical properties, thermal performance, and flame retardancy of the composites were investigated using a four-point probe instrument, universal tensile machine, thermogravimetric analysis, and cone calorimeter tests, respectively. It was found that the addition of multi-walled carbon nanotubes can significantly improve the electrical conductivity and mechanical properties of the low-density polyethylene composites. Furthermore, the combination of multi-walled carbon nanotubes and phosphorus–nitrogen flame retardant remarkably enhances the flame retardancy of matrixes with an observed decrease of the peak heat release rate and total heat release of 49.8% and 51.9%, respectively. This study provides a new and effective methodology to substantially enhance the electrical conductivity and flame retardancy of polymers with an attractive prospect for polymer applications in electrical equipment.

  • RESEARCH ARTICLE
    Nikolaus I. Vollmer, Resul Al, Krist V. Gernaey, Gürkan Sin
    Frontiers of Chemical Science and Engineering, 2022, 16(2): 251-273. https://doi.org/10.1007/s11705-021-2071-9

    The conceptual process design of novel bioprocesses in biorefinery setups is an important task, which remains yet challenging due to several limitations. We propose a novel framework incorporating superstructure optimization and simulation-based optimization synergistically. In this context, several approaches for superstructure optimization based on different surrogate models can be deployed. By means of a case study, the framework is introduced and validated, and the different superstructure optimization approaches are benchmarked. The results indicate that even though surrogate-based optimization approaches alleviate the underlying computational issues, there remains a potential issue regarding their validation. The development of appropriate surrogate models, comprising the selection of surrogate type, sampling type, and size for training and cross-validation sets, are essential factors. Regarding this aspect, satisfactory validation metrics do not ensure a successful outcome from its embedded use in an optimization problem. Furthermore, the framework’s synergistic effects by sequentially performing superstructure optimization to determine candidate process topologies and simulation-based optimization to consolidate the process design under uncertainty offer an alternative and promising approach. These findings invite for a critical assessment of surrogate-based optimization approaches and point out the necessity of benchmarking to ensure consistency and quality of optimized solutions.

  • COMMUNICATION
    Yusheng Xie, Jie Zhang, Liu Yang, Qingxin Chen, Quan Hao, Liang Zhang, Hongyan Sun
    Frontiers of Chemical Science and Engineering, 2022, 16(1): 121-127. https://doi.org/10.1007/s11705-021-2051-0

    Lysine lipoylation plays vital roles in cell metabolism and redox processes. For example, removal of lipoylation will decrease pyruvate dehydrogenase activity and affect the citric acid cycle. Despite the important functions of lysine lipoylation, the mechanisms for the addition and removal of this modification remain largely unexplored. Very few useful chemical tools are available to study the interactions of lysine lipoylation with its regulatory delipoylation proteins. For example, immunoaffinity purification-mass spectrometry is one of such tools, which highly relies on antibody efficiency and purification techniques. Single-step activity based fluorogenic probes developed by our groups and others is also an efficient method to study the deacylation activity. Affinity-based labeling probe using photo-cross-linker is a powerful platform to study the transient and dynamic interactions of peptide ligands with the interacting proteins. Herein, we have designed and synthesized a dual-function probe KTLlip for studying enzymatic delipoylation (eraser) activity and interaction of lysine lipoylation with the eraser at the same time. We show that KTLlip can be used as a useful tool to detect delipoylation as demonstrated by its ability to fluorescently label the eraser activity of recombinant Sirt2. We envision that the probe will help delineate the roles of delipoylation enzyme in biology.

  • RESEARCH ARTICLE
    Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu
    Frontiers of Chemical Science and Engineering, 2021, 15(5): 1111-1124. https://doi.org/10.1007/s11705-020-2031-9

    The hydroisomerization of n-hexadecane over Pt-Pd bimetallic catalysts is an effective way to produce clean fuel oil. This work reports a useful preparation method of bimetallic bifunctional catalysts by a co-impregnation or sequential impregnation process. Furthermore, monometallic catalysts with loading either Pt or Pd are also prepared for comparison. The effects of the metal species and impregnation order on the characteristics and catalytic performance of the catalysts are investigated. The catalytic test results indicate that the maximum iso-hexadecane yield over different catalysts increases as follows: Pt/silicoaluminophosphate SAPO-41<Pd/SAPO-41<Pt*-Pd/SAPO-41 (prepared by sequential impregnation)<Pt-Pd/SAPO-41 (prepared by co-impregnation). Owing to the synergic effects between Pt and Pd, the Pt-Pd/SAPO-41 catalyst prepared by the co-impregnation method demonstrates the effective promotion of (de)hydrogenation activity. Therefore, this catalyst exhibits the highest iso-hexadecane yield of 89.4% when the n-hexadecane conversion is 96.3%. Additionally, the Pt-Pd/SAPO-41 catalyst also presents the highest catalytic activity and best stability even after 150 h long-term tests.

  • RESEARCH ARTICLE
    Xiangyu Liu, Yanling Pan, Peng Zhang, Yilin Wang, Guohao Xu, Zhaojie Su, Xuedong Zhu, Fan Yang
    Frontiers of Chemical Science and Engineering, 2022, 16(3): 384-396. https://doi.org/10.1007/s11705-021-2045-y

    Alkylation of benzene to value-added, high octane number and low toxic toluene and xylenes provides a way to lower benzene content in gasoline pool, and is hence a method to promote fuel quality. On the other hand, CO2 accumulation in the atmosphere causes global warming and requires effective route for its valorization. Utilization of CO2 as a carbon source for benzene alkylation could achieve both goals. Herein, alkylation of benzene with CO2 and H2 was realized by a series of low-cost bifunctional catalysts containing zinc/titanium oxides (Zn/Ti oxides) and HZSM-5 molecular sieves in a fixed-bed reactor. By regulating and controlling oxygen vacancies of Zn/Ti oxides and the acidities of HZSM-5, benzene conversion and CO2 conversion reached 28.7% and 29.9% respectively, along with a total selectivity of toluene and xylene higher than 90%. In this process, more than 25% CO2 was effectively utilized and incorporated into the target products. Moreover, the mechanism of the reaction was analyzed and the course was simultaneously traced. CO2 was transformed into methanol firstly, and then methanol reacted with benzene generating toluene and xylene. The innovation provides a new method for upgrading of fuels and upcycling the emissions of CO2, which is of great environmental and economic benefits.

  • REVIEW ARTICLE
    Stefano Capizzano, Mirko Frappa, Francesca Macedonio, Enrico Drioli
    Frontiers of Chemical Science and Engineering, 2022, 16(5): 592-613. https://doi.org/10.1007/s11705-021-2105-3

    One of the problems that most afflicts humanity is the lack of clean water. Water stress, which is the pressure on the quantity and quality of water resources, exists in many places throughout the World. Desalination represents a valid solution to the scarcity of fresh water and several technologies are already well applied and successful (such as reverse osmosis), producing about 100 million m3·d−1 of fresh water. Further advances in the field of desalination can be provided by innovative processes such as membrane distillation. The latter is of particular interest for the treatment of waste currents from conventional desalination processes (for example the retentate of reverse osmosis) as it allows to desalt highly concentrated currents as it is not limited by concentration polarization phenomena. New perspectives have enhanced research activities and allowed a deeper understanding of mass and heat transport phenomena, membrane wetting, polarization phenomena and have encouraged the use of materials particularly suitable for membrane distillation applications. This work summarizes recent developments in the field of membrane distillation, studies for module length optimization, commercial membrane modules developed, recent patents and advancement of membrane material.