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  • RESEARCH ARTICLE
    Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song
    Frontiers of Chemical Science and Engineering, 2018, 12(1): 83-93. https://doi.org/10.1007/s11705-017-1691-6

    A series of Al2O3 and CeO2 modified MgO sorbents was prepared and studied for CO2 sorption at moderate temperatures. The CO2 sorption capacity of MgO was enhanced with the addition of either Al2O3 or CeO2. Over Al2O3-MgO sorbents, the best capacity of 24.6 mg-CO2/g-sorbent was attained at 100 °C, which was 61% higher than that of MgO (15.3 mg-CO2/g-sorbent). The highest capacity of 35.3 mg-CO2/g-sorbent was obtained over the CeO2-MgO sorbents at the optimal temperature of 200 °C. Combining with the characterization results, we conclude that the promotion effect on CO2 sorption with the addition of Al2O3 and CeO2 can be attributed to the increased surface area with reduced MgO crystallite size. Moreover, the addition of CeO2 increased the basicity of MgO phase, resulting in more increase in the CO2 capacity than Al2O3 promoter. Both the Al2O3-MgO and CeO2-MgO sorbents exhibited better cyclic stability than MgO over the course of fifteen CO2 sorption-desorption cycles. Compared to Al2O3, CeO2 is more effective for promoting the CO2 capacity of MgO. To enhance the CO2 capacity of MgO sorbent, increasing the basicity is more effective than the increase in the surface area.

  • REVIEW ARTICLE
    Simin Feng, Xiaoli Zhang, Dunyun Shi, Zheng Wang
    Frontiers of Chemical Science and Engineering, 2021, 15(2): 221-237. https://doi.org/10.1007/s11705-020-1927-8

    Zeolitic imidazolate framework-8 (ZIF-8), composed of Zn ions and imidazolate ligands, is a class of metal-organic frameworks, which possesses a similar structure as conventional aluminosilicate zeolites. This material exhibits inherent porous property, high loading capacity, and pH-sensitive degradation, as well as exceptional thermal and chemical stability. Extensive research effort has been devoted to relevant research aspects ranging from synthesis methods, property characterization to potential applications of ZIF-8. This review focuses on the recent development of ZIF-8 synthesis methods and its promising applications in drug delivery. The potential risks of using ZIF-8 for drug delivery are also summarized.

  • RESEARCH ARTICLE
    Xiyuan Bu, Ming Tian, Hongqing Wang, Lin Wang, Liyong Yuan, Weiqun Shi
    Frontiers of Chemical Science and Engineering, 2022, 16(11): 1632-1642. https://doi.org/10.1007/s11705-022-2187-6

    Although metal–organic frameworks offer a new platform for developing versatile sorption materials, yet coordinating the functionality, structure and component of these materials remains a great challenge. It depends on a comprehensive knowledge of a “real sorption mechanism”. Herein, a ternary mechanism for U(VI) uptake in metal–organic frameworks was reported. Analogous MIL-100s (Al, Fe, Cr) were prepared and studied for their ability to sequestrate U(VI) from aqueous solutions. As a result, MIL-100(Al) performed the best among the tested materials, and MIL-100(Cr) performed the worst. The nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(VI) uptake in the three metal–organic frameworks involves different mechanisms. Specifically, hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s (Al, Fe) by exchanging with hydrogen ions of terminal hydroxyl groups (Al-OH2, Fe-OH2), and/or, hydrated uranyl ions are bound directly to Al(III) center in MIL-100(Al) through a strong inner-sphere coordination. For MIL-100(Cr), however, the U(VI) uptake is attributed to electrostatic attraction. Besides, the sorption mechanism is also pH and ionic strength dependent. The present study suggests that changing metal center of metal–organic frameworks and sorption conditions alters sorption mechanism, which helps to construct effective metal–organic frameworks-based sorbents for water purification.

  • RESEARCH ARTICLE
    Huaxin Qu, Jie Deng, Bei Wang, Lezi Ouyang, Yong Tang, Kai Yu, Lan-Lan Lou, Shuangxi Liu
    Frontiers of Chemical Science and Engineering, 2021, 15(6): 1514-1523. https://doi.org/10.1007/s11705-021-2092-4

    A base-free catalytic system for the aerobic oxidation of 5-hydroxymethyl-2-furfural was exploited by using Pt nanoparticles immobilized onto a thermoresponsive poly(acrylamide-co-acrylonitrile)-b-poly(N-vinylimidazole) block copolymer, with an upper critical solution temperature of about 45 °C. The Pt nanocatalysts were well-dispersed and highly active for the base-free oxidation of 5-hydroxymethyl-2-furfural by molecular oxygen in water, affording high yields of 2,5-furandicarboxylic acid (up to>99.9%). The imidazole groups in the block copolymer were conducive to the improvement of catalytic performance. Moreover, the catalysts could be easily separated and recovered based on their thermosensitivity by cooling the reaction system below the upper critical solution temperature. Good stability and reusability were observed over these copolymer-immobilized catalysts with no obvious decrease in catalytic activity in the five consecutive cycles.

  • RESEARCH ARTICLE
    Jing Wang, Guoyuan Pan, Yu Li, Yang Zhang, Hongwei Shi, Xuanbo Liu, Hao Yu, Muhua Zhao, Yiqun Liu, Changjiang Wu
    Frontiers of Chemical Science and Engineering, 2022, 16(8): 1268-1280. https://doi.org/10.1007/s11705-022-2143-5

    The micro-nano composite structure can endow separation membranes with special surface properties, but it often has the problems of inefficient preparation process and poor structural stability. In this work, a novel atomization-assisted nonsolvent induced phase separation method, which is also highly efficient and very simple, has been developed. By using this method, a bicontinuous porous microfiltration membrane with robust micro-nano composite structure was obtained via commercially available polymers of polyacrylonitrile and polyvinylpyrrolidone. The formation mechanism of the micro-nano composite structure was proposed. The microphase separation of polyacrylonitrile and polyvinylpyrrolidone components during the atomization pretreatment process and the hydrogen bonding between polyacrylonitrile and polyvinylpyrrolidone molecules should have resulted in the nano-protrusions on the membrane skeleton. The membrane exhibits superhydrophilicity in air and superoleophobicity underwater. The membrane can separate both surfactant-free and surfactant-stabilized oil-in-water emulsions with high separation efficiency and permeation flux. With excellent antifouling property and robust microstructure, the membrane can easily be recycled for long-term separation. Furthermore, the scale-up verification from laboratory preparation to continuous production has been achieved. The simple, efficient, cost-effective preparation method and excellent membrane properties indicate the great potential of the developed membranes in practical applications.

  • RESEARCH ARTICLE
    Tianyi Bao, Yuanyuan Shao, Haiping Zhang, Jesse Zhu
    Frontiers of Chemical Science and Engineering, 2022, 16(6): 985-995. https://doi.org/10.1007/s11705-021-2126-y

    The high contents of nitrogen-containing organic compounds in biocrude obtained from hydrothermal liquefaction of microalgae are one of the most concerned issues on the applications and environment. In the project, Chlorella sp. and Spirulina sp. were selected as raw materials to investigate the influence of different reaction conditions (i.e., reaction temperature, residence time, solid loading rate) on the distribution of nitrogen in the oil phase and aqueous phase. Three main forms of nitrogen-containing organic compounds including nitrogen-heterocyclic compounds, amide, and amine were detected in biocrudes. The contents of nitrogen-heterocyclic compounds decreased with temperature while amide kept increasing. The effect of residence time on the components of nitrogen-containing organic compounds was similar with that of temperature. However, the influence of solid loading rate was insignificant. Moreover, it was also found that the differences of amino acids in the protein components in the two microalgae might affect the nitrogen distribution in products. For example, nitrogen in basic amino acids of Spirulina sp. preferred to go into the aqueous phase comparing with the nitrogen in neutral amino acids of Chlorella sp. In summary, a brief reaction map was proposed to describe the nitrogen pathway during microalgae hydrothermal liquefaction.

  • REVIEW ARTICLE
    Sainab Omar, Yang Yang, Jiawei Wang
    Frontiers of Chemical Science and Engineering, 2021, 15(1): 4-17. https://doi.org/10.1007/s11705-020-1933-x

    This review article summarizes the key published research on the topic of bio-oil upgrading using catalytic and non-catalytic supercritical fluid (SCF) conditions. The precious metal catalysts Pd, Ru and Pt on various supports are frequently chosen for catalytic bio-oil upgrading in SCFs. This is reportedly due to their favourable catalytic activity during the process including hydrotreating, hydrocracking, and esterification, which leads to improvements in liquid yield, heating value, and pH of the upgraded bio-oil. Due to the costs associated with precious metal catalysts, some researchers have opted for non-precious metal catalysts such as acidic HZSM-5 which can promote esterification in supercritical ethanol. On the other hand, SCFs have been effectively used to upgrade crude bio-oil without a catalyst. Supercritical methanol, ethanol, and water are most commonly used and demonstrate catalyst like activities such as facilitating esterification reactions and reducing solid yield by alcoholysis and hydrolysis, respectively.

  • RESEARCH ARTICLE
    Yu-Chao Wang, Tian-Tian Li, Li Huang, Xiao-Qin Liu, Lin-Bing Sun
    Frontiers of Chemical Science and Engineering, 2022, 16(11): 1623-1631. https://doi.org/10.1007/s11705-022-2202-y

    The number of active components and their dispersion degree are two key factors affecting the performance of adsorbents. Here, we report a simple but efficient strategy for dispersing active components by using a confined space, which is formed by mesoporous silica walls and templates in the as-prepared SBA-15 (AS). Such a confined space does not exist in the conventional support, calcined SBA-15, which does not contain a template. The Cu and Zn precursors were introduced to the confined space in the AS and were converted to CuO and ZnO during calcination, during which the template was also removed. The results show that up to 5 mmol·g–1 of CuO and ZnO can be well dispersed; however, severe aggregation of both oxides takes place in the sample derived from the calcined SBA-15 with the same loading. Confined space in the AS and the strong interactions caused by the abundant hydroxyl groups are responsible for the dispersion of CuO and ZnO. The bimetallic materials were employed for the adsorptive separation of propene and propane. The samples prepared from the as-prepared SBA-15 showed superior performance to their counterparts from the calcined SBA-15 in terms of both adsorption capacity of propene and selectivity for propene/propane.

  • RESEARCH ARTICLE
    Na Wang, Fujian Li, Bangyu Fan, Suojiang Zhang, Lu Bai, Xiangping Zhang
    Frontiers of Chemical Science and Engineering, 2022, 16(11): 1584-1594. https://doi.org/10.1007/s11705-022-2189-4

    The separation of rare earth elements is particularly difficult due to their similar physicochemical properties. Based on the tiny differences of ionic radius, solvent extraction has been developed as the “mass method” in industry with hundreds of stages, extremely intensive chemical consumption and large capital investments. The differences of the ionic magnetic moment among rare earths are greater than that of ionic radius. Herein, a novel method based on the large ionic magnetic moment differences of rare earth elements was proposed to promote the separation efficiency. Rare earths were firstly dissolved in the ionic liquid, then the ordering degree of them was improved with the Z-bond effect, and finally the magnetic moment differences between paramagnetic and diamagnetic rare earths in quasi-liquid system were enhanced. Taking the separation of Er/Y, Ho/Y and Er/Ho as examples, the results showed that Er(III) and Ho(III) containing ionic liquids had obvious magnetic response, while ionic liquids containing Y(III) had no response. The separation factors of Er/Y and Ho/Y were achieved at 9.0 and 28.82, respectively. Magnetic separation via quasi-liquid system strategy provides a possibility of the novel, green, and efficient method for rare earth separation.

  • RESEARCH ARTICLE
    Yixuan Chang, Fanwei Kong, Zihao Zhu, Ziai Wang, Chunxia Chen, Xiaobai Li, Hongwei Ma
    Frontiers of Chemical Science and Engineering, 2023, 17(7): 966-975. https://doi.org/10.1007/s11705-022-2244-1

    The efficient utilization of natural lignin, which is the main by-product of the cellulose industry, is crucial for enhancing its economic value, alleviating the environmental burden, and improving ecological security. By taking advantage of the large sp2 hybrid domain of lignin and introducing amino functional groups, new lignin-derived carbon dots (SPN-CDs) with red fluorescence were successfully synthesized. Compared with green and blue fluorescent materials, red SPN-CDs have desirable anti-interference properties of short-wave background and exhibit superior luminescence stability. The SPN-CDs obtained exhibited sensitive and distinctive visible color with fluorescence-dual responses toward hypochlorite. Considering this feature, a portable, low-cost, and sensitive fluorescence sensing paper with a low limit of detection of 0.249 μmol∙L–1 was fabricated using the SPN-CDs for hypochlorite detection. Furthermore, a new type of visible-light and fluorescence dual-channel information encryption platform was constructed. Low-concentration hypochlorite can be employed as an accessible and efficient information encryption/decryption stimulus, as well as an information “eraser”, facilitating a safe and diversified transmission and convenient decryption of information. This work opens new avenues for high-value-added applications of lignin-based fluorescent materials.

  • RESEARCH ARTICLE
    Yiyi Fan, Jinyong Li, Saidi Wang, Xiuxia Meng, Yun Jin, Naitao Yang, Bo Meng, Jiaquan Li, Shaomin Liu
    Frontiers of Chemical Science and Engineering, 2021, 15(4): 882-891. https://doi.org/10.1007/s11705-020-1990-1

    Hydrogen fuel has been embraced as a potential long-term solution to the growing demand for clean energy. A membrane-assisted separation is promising in producing high-purity H2. Molecular sieving membranes (MSMs) are endowed with high gas selectivity and permeability because their well-defined micropores can facilitate molecular exclusion, diffusion, and adsorption. In this work, MXene nanosheets intercalated with Ni2+ were assembled to form an MSM supported on Al2O3 hollow fiber via a vacuum-assisted filtration and drying process. The prepared membranes showed excellent H2/CO2 mixture separation performance at room temperature. Separation factor reached 615 with a hydrogen permeance of 8.35 × 108 mol·m2·s1·Pa1. Compared with the original Ti3C2Tx/Al2O3 hollow fiber membranes, the permeation of hydrogen through the Ni2+-Ti3C2Tx/Al2O3 membrane was considerably increased, stemming from the strong interaction between the negatively charged MXene nanosheets and Ni2+. The interlayer spacing of MSMs was tuned by Ni2+. During 200-hour testing, the resultant membrane maintained an excellent gas separation without any substantial performance decline. Our results indicate that the Ni2+ tailored Ti3C2Tx/Al2O3 hollow fiber membranes can inspire promising industrial applications.

  • RESEARCH ARTICLE
    Zihan Xu, Huajie Xu, Lu Liu, Rongpei Jiang, Haisheng Ren, Xiangyuan Li
    Frontiers of Chemical Science and Engineering, 2022, 16(12): 1743-1750. https://doi.org/10.1007/s11705-022-2184-9

    The standard enthalpy of formation is an important predictor of the reaction heat of a chemical reaction. In this work, a high-precision method was developed to calculate accurate standard enthalpies of formation for polycyclic aromatic hydrocarbons based on the general connectivity based hierarchy (CBH) with the discrete correction of atomization energy. Through a comparison with available experimental findings and other high-precision computational results, it was found that the present method can give a good description of enthalpy of formation for polycyclic aromatic hydrocarbons. Since CBH schemes can broaden the scope of application, this method can be used to investigate the energetic properties of larger polycyclic aromatic hydrocarbons to achieve a high-precision calculation at the CCSD(T)/CBS level. In addition, the energetic properties of CBH fragments can be accurately calculated and integrated into a database for future use, which will increase computational efficiency. We hope this work can give new insights into the energetic properties of larger systems.

  • RESEARCH ARTICLE
    Yang Zhang, Guowu Zhan, Yibo Song, Yiping Liu, Jiale Huang, Shu-Feng Zhou, Kok Bing Tan, Qingbiao Li
    Frontiers of Chemical Science and Engineering, 2022, 16(12): 1793-1806. https://doi.org/10.1007/s11705-022-2191-x

    Recycling industrial solid waste not only saves resources but also eliminates environmental concerns of toxic threats. Herein, we proposed a new strategy for the utilization of petrochemical-derived carbon black waste, a waste vanadium-bearing resource (V > 30000 ppm (10 −6)). Chemical leaching was employed to extract metallic vanadium from the waste and the leachate containing V was used as an alternative raw material for the fabrication of vanadate nanomaterials. Through the screening of various metal cations, it was found that the contaminated Na+ during the leaching process showed strong competitive coordination with the vanadium ions. However, by adding foreign Ce3+ and Y3+ cations, two rare-earth vanadates, viz., flower-like CeVO4 and spherical YVO4 nanomaterials, were successfully synthesized. Characterization techniques such as scanning electron microscopy, transmission electron microscopy, X-ray diffraction, energy-dispersive X-ray spectroscopy, Fourier-transform infrared, and N2 physisorption were applied to analyze the physicochemical properties of the waste-derived nanomaterials. Importantly, we found that rare-earth vanadate catalysts exhibited good activities toward the semi-hydrogenation of α,β-unsaturated aldehydes. The conversion of cinnamaldehyde and cinnamic alcohol selectivity were even higher than those of the common CeVO4 prepared using pure chemicals (67.2% vs. 27.7% and 88.4% vs. 53.5%). Our work provides a valuable new reference for preparing vanadate catalysts by the use of abundant vanadium-bearing waste resources.

  • RESEARCH ARTICLE
    Dongyang Liu, Yibo Zhi, Yuen Bai, Liang Zhao, Jinsen Gao, Chunming Xu
    Frontiers of Chemical Science and Engineering, 2022, 16(12): 1700-1712. https://doi.org/10.1007/s11705-022-2207-6

    The chain length and hydrocarbon type significantly affect the production of light olefins during the catalytic pyrolysis of naphtha. Herein, for a better catalyst design and operation parameters optimization, the reaction pathways and equilibrium yields for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins were analyzed thermodynamically. The results revealed that the thermodynamically favorable reaction pathways for n/iso-paraffins and cyclo-paraffins were the protolytic and hydrogen transfer cracking pathways, respectively. However, the formation of light paraffin severely limits the maximum selectivity toward light olefins. The dehydrogenation cracking pathway of n/iso-paraffins and the protolytic cracking pathway of cyclo-paraffins demonstrated significantly improved selectivity for light olefins. The results are thus useful as a direction for future catalyst improvements, facilitating superior reaction pathways to enhance light olefins. In addition, the equilibrium yield of light olefins increased with increasing the chain length, and the introduction of cyclo-paraffin inhibits the formation of light olefins. High temperatures and low pressures favor the formation of ethylene, and moderate temperatures and low pressures favor the formation of propylene. n-Hexane and cyclohexane mixtures gave maximum ethylene and propylene yield of approximately 49.90% and 55.77%, respectively. This work provides theoretical guidance for the development of superior catalysts and the selection of proper operation parameters for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins from a thermodynamic point of view.

  • 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
    Xinhe Wang, Liuqing Yang, Xiaolin Ji, Yunfei Gao, Fanxing Li, Junshe Zhang, Jinjia Wei
    Frontiers of Chemical Science and Engineering, 2022, 16(12): 1726-1734. https://doi.org/10.1007/s11705-022-2188-5

    Chemical looping reforming of methane is a novel and effective approach to convert methane to syngas, in which oxygen transfer is achieved by a redox material. Although lots of efforts have been made to develop high-performance redox materials, a few studies have focused on the redox kinetics. In this work, the kinetics of SrFeO3−δ–CaO∙MnO nanocomposite reduction by methane was investigated both on a thermo-gravimetric analyzer and in a packed-bed microreactor. During the methane reduction, combustion occurs before the partial oxidation and there exists a transition between them. The weight loss due to combustion increases, but the transition region becomes less inconspicuous as the reduction temperature increased. The weight loss associated with the partial oxidation is much larger than that with combustion. The rate of weight loss related to the partial oxidation is well fitted by the Avrami–Erofeyev equation with n = 3 (A3 model) with an activation energy of 59.8 kJ∙mol‒1. The rate law for the partial oxidation includes a solid conversion term whose expression is given by the A3 model and a methane pressure-dependent term represented by a power law. The partial oxidation is half order with respect to methane pressure. The proposed rate law could well predict the reduction kinetics; thus, it may be used to design and/or analyze a chemical looping reforming reactor.

  • REVIEW ARTICLE
    Lixin Xing, Jiaming Wang, Xuehua Ruan, Gaohong He
    Frontiers of Chemical Science and Engineering, 2022, 16(11): 1536-1559. https://doi.org/10.1007/s11705-022-2221-8

    Poly(ether−ether ketone) (PEEK) is a linear aromatic macromolecule, which can form semi-crystalline aggregative status, allowing PEEK materials to have strong environment tolerance and excellent physicochemical properties. PEEK materials have become a promising alternative to fabricate particular membranes used in extreme conditions. In the past few decades, many researches and evolutions have emerged in membrane fabrication with PEEK materials and its applications for treating organic solvents and their mixtures; however, there are little systematic and comprehensive literature to summarize fabrication approaches, compile applications, and elaborate PEEK property-structure relationship. In this review, the main approaches to fabricate PEEK-based membranes are illustrated concretely, including conventional thermal-induced and non-solvent-induced phase separation, and novel chemical-induced crystallization; the representative applications in ultrafiltration, nanofiltration and membrane contactor containing organic solvents are demonstrated systematically. Meanwhile, the mechanism to tune PEEK solubility in solvents, which can be achieved by altering monomers in synthesis processes or changing membrane preparation routes, is deeply analyzed. Moreover, the existing problems and the future prospects are also discussed. This review provides positive guidance for designing and fabricating membranes using PEEK and its derivative materials for task-specific applications in harsh conditions.

  • 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
    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%.

  • RESEARCH ARTICLE
    Yanli Fang, Hui Wang, Xuyun Wang, Jianwei Ren, Rongfang Wang
    Frontiers of Chemical Science and Engineering, 2023, 17(4): 373-386. https://doi.org/10.1007/s11705-022-2223-6

    The bind-free carbon cloth-supported electrodes hold the promises for high-performance electrochemical capacitors with high specific capacitance and good cyclic stability. Considering the close connection between their performance and the amount of carbon material loaded on the electrodes, in this work, NiCo2O4 nanowires were firstly grown on the substrate of active carbon cloth to provide the necessary surface area in the longitudinal direction. Then, the quinone-rich nitrogen-doped carbon shell structure was formed around NiCo2O4 nanowires, and the obtained composite was used as electrode for electric double layer capacitor. The results showed that the composite electrode displayed an area-specific capacitance of 1794 mF∙cm–2 at the current density of 1 mA∙cm–2. The assembled symmetric electric double layer capacitor achieved a high energy density of 6.55 mW∙h∙cm–3 at a power density of 180 mW∙cm–3. The assembled symmetric capacitor exhibited a capacitance retention of 88.96% after 10000 charge/discharge cycles at the current density of 20 mA∙cm–2. These results indicated the potentials in the preparation of the carbon electrode materials with high energy density and good cycling stability.

  • RESEARCH ARTICLE
    Leijing Liu, Hao Zhang, Bo Xiao, Yang Liu, Bin Xu, Chen Wang, Shanpeng Wen, Erjun Zhou, Gang Chen, Chan Im, Wenjing Tian
    Frontiers of Chemical Science and Engineering, 2021, 15(1): 127-137. https://doi.org/10.1007/s11705-020-1936-7

    Effects of a benzotriazole (BTA)-based small molecule, BTA2, as the third component on the charge carrier generation and recombination behavior of poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]] (PTB7):[6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) organic solar cells (OSCs) were investigated by optical simulation of a transfer matrix model (TMM), photo-induced charge extraction by linearly increasing voltage (photo-CELIV) technique, atomic force microscope (AFM), and the Onsager–Braun model analysis. BTA2 is an A2-A1-D-A1-A2-type non-fullerene small molecule with thiazolidine-2,4-dione, BTA, and indacenodithiophene as the terminal acceptor (A2), bridge acceptor (A1), and central donor (D), respectively. The short-circuit current density of the OSCs with BTA2 can be enhanced significantly owing to a complementary absorption spectrum. The optical simulation of TMM shows that the ternary OSCs exhibit higher internal absorption than the traditional binary OSCs without BTA2, resulting in more photogenerated excitons in the ternary OSCs. The photo-CELIV investigation indicates that the ternary OSCs suffer higher charge trap-limited bimolecular recombination than the binary OSCs. AFM images show that BTA2 aggravates the phase separation between the donor and the acceptor, which is disadvantageous to charge carrier transport. The Onsager-Braun model analysis confirms that despite the charge collection efficiency of the ternary OSCs being lower than that of the binary OSCs, the optimized photon absorption and exciton generation processes of the ternary OSCs achieve an increase in photogenerated current and thus improve power conversion efficiency.

  • RESEARCH ARTICLE
    Ruiqi Li, Kang Li, Wei Wang, Fan Zhang, Shichao Tian, Zhongqi Ren, Zhiyong Zhou
    Frontiers of Chemical Science and Engineering, 2023, 17(6): 749-758. https://doi.org/10.1007/s11705-022-2261-0

    Since lithium iron phosphate cathode material does not contain high-value metals other than lithium, it is therefore necessary to strike a balance between recovery efficiency and economic benefits in the recycling of waste lithium iron phosphate cathode materials. Here, we describe a selective recovery process that can achieve economically efficient recovery and an acceptable lithium leaching yield. Adjusting the acid concentration and amount of oxidant enables selective recovery of lithium ions. Iron is retained in the leaching residue as iron phosphate, which is easy to recycle. The effects of factors such as acid concentration, acid dosage, amount of oxidant, and reaction temperature on the leaching of lithium and iron are comprehensively explored, and the mechanism of selective leaching is clarified. This process greatly reduces the cost of processing equipment and chemicals. This increases the potential industrial use of this process and enables the green and efficient recycling of waste lithium iron phosphate cathode materials in the future.

  • RESEARCH ARTICLE
    Yong Zheng, Mingjin Li, Yongye Wang, Niu Huang, Wei Liu, Shan Chen, Xuepeng Ni, Kunming Li, Siwei Xiong, Yi Shen, Siliang Liu, Baolong Zhou, Niaz Ali Khan, Liqun Ye, Chao Zhang, Tianxi Liu
    Frontiers of Chemical Science and Engineering, 2023, 17(5): 525-535. https://doi.org/10.1007/s11705-022-2232-5

    Fe–Nx nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–Nx nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–Nx nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

  • 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
    Wenjie Sun, Jiale Mao, Shuang Wang, Lei Zhang, Yonghong Cheng
    Frontiers of Chemical Science and Engineering, 2021, 15(1): 18-34. https://doi.org/10.1007/s11705-020-1939-4

    Polymer-based dielectric capacitors are widely-used energy storage devices. However, although the functions of dielectrics in applications like high-voltage direct current transmission projects, distributed energy systems, high-power pulse systems and new energy electric vehicles are similar, their requirements can be quite different. Low electric loss is a critical prerequisite for capacitors for electric grids, while high-temperature stability is an essential pre-requirement for those in electric vehicles. This paper reviews recent advances in this area, and categorizes dielectrics in terms of their foremost properties related to their target applications. Requirements for polymer-based dielectrics in various power electronic equipment are emphasized, including high energy storage density, low dissipation, high working temperature and fast-response time. This paper considers innovations including chemical structure modification, composite fabrication and structure re-design, and the enhancements to material performances achieved. The advantages and limitations of these methods are also discussed.

  • RESEARCH ARTICLE
    Chenxi Xu, Shunli Li, Zhaohui Hou, Liming Yang, Wenbin Fu, Fujia Wang, Yafei Kuang, Haihui Zhou, Liang Chen
    Frontiers of Chemical Science and Engineering, 2023, 17(6): 679-690. https://doi.org/10.1007/s11705-022-2266-8

    The massive conversion of resourceful biomass to carbon nanomaterials not only opens a new avenue to effective and economical disposal of biomass, but provides a possibility to produce highly valued functionalized carbon-based electrodes for energy storage and conversion systems. In this work, biomass is applied to a facile and scalable one-step pyrolysis method to prepare three-dimensional (3D) carbon nanotubes/mesoporous carbon architecture, which uses transition metal inorganic salts and melamine as initial precursors. The role of each employed component is investigated, and the electrochemical performance of the attained product is explored. Each component and precise regulation of their dosage is proven to be the key to successful conversion of biomass to the desired carbon nanomaterials. Owing to the unique 3D architecture and integration of individual merits of carbon nanotubes and mesoporous carbon, the as-synthesized carbon nanotubes/mesoporous carbon hybrid exhibits versatile application toward lithium-ion batteries and Zn-air batteries. Apparently, a significant guidance on effective conversion of biomass to functionalized carbon nanomaterials can be shown by this work.

  • RESEARCH ARTICLE
    Shangcong Zhang, Qian Liu, Xinyue Tang, Zhiming Zhou, Tieyan Fan, Yingmin You, Qingcheng Zhang, Shusheng Zhang, Jun Luo, Xijun Liu
    Frontiers of Chemical Science and Engineering, 2023, 17(6): 726-734. https://doi.org/10.1007/s11705-022-2274-8

    Designing advanced and cost-effective electrocatalytic system for nitric oxide (NO) reduction reaction (NORR) is vital for sustainable NH3 production and NO removal, yet it is a challenging task. Herein, it is shown that phosphorus (P)-doped titania (TiO2) nanotubes can be adopted as highly efficient catalyst for NORR. The catalyst demonstrates impressive performance in ionic liquid (IL)-based electrolyte with a remarkable high Faradaic efficiency of 89% and NH3 yield rate of 425 μg·h−1·mgcat.−1, being close to the best-reported results. Noteworthy, the obtained performance metrics are significantly larger than those for N2 reduction reaction. It also shows good durability with negligible activity decay even after 10 cycles. Theoretical simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites, thereby enhancing the NO adsorption and facilitating the desorption of *NH3. Moreover, the utilization of IL further suppresses the competitive hydrogen evolution reaction. This study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH3 at a high efficiency and rate.

  • 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
    Ammaru Ismaila, Xueli Chen, Xin Gao, Xiaolei Fan
    Frontiers of Chemical Science and Engineering, 2021, 15(1): 60-71. https://doi.org/10.1007/s11705-020-1975-0

    Thermodynamic chemical equilibrium analysis of steam reforming of glycerol (SRG) for selective hydrogen production was performed based on the Gibbs free energy minimisation method. The ideal SRG reaction (C3H8O3+3H2O→3CO2+7H2) and a comprehensive set of side reactions during SRG are considered for the formation of a wide range of products. Specifically, this work focused on the analysis of formation of H2, CO2, CO and CH4 in the gas phase and determination of the carbon free region in SRG under the conditions at atmospheric pressure, 600 K–1100 K and 1.013 × 105–1.013 × 106 Pa with the steam-to-glycerol feed ratios (SGFR) of 1:5–10. The reaction conditions which favoured SRG for H2 production with minimum coke formation were identifies as: atmospheric pressure, temperatures of 900 K–1050 K and SGFR of 10:1. The influence of using the inert carrier gas (i.e., N2) in SRG was studied as well at atmospheric pressure. Although the presence of N2 in the stream decreased the partial pressure of reactants, it was beneficial to improve the equilibrium yield of H2. Under both conditions of SRG (with/without inert gas), the CH4 production is minimised, and carbon formation was thermodynamically unfavoured at steam rich conditions of SGFR>5:1.

  • RESEARCH ARTICLE
    Qian Wu, Jincheng Zhang, Shengpeng Wang, Bajin Chen, Yijun Feng, Yongbing Pei, Yue Yan, Longcheng Tang, Huayu Qiu, Lianbin Wu
    Frontiers of Chemical Science and Engineering, 2021, 15(4): 969-983. https://doi.org/10.1007/s11705-020-1988-8

    A facile strategy was developed to fabricate flexible polyurethane (PU) foam composites with exceptional flame retardancy. The approach involves the incorporation of graphene oxide (GO) into a silicone resin (SiR) solution, which is then deposited onto a PU foam surface via the dip-coating technique and cured. Fourier-transform infrared spectroscopy, scanning electron microscopy, and Raman spectroscopy measurements demonstrated that the SiR and GO were successfully coated onto the PU skeleton and the intrinsic porous structure of the PU foam remained intact. The effects of SiR and GO on the mechanical and thermal stability and flame retardancy of PU composites were evaluated through compression tests, thermogravimetric analysis, vertical combustion tests, and the limiting oxygen index. The measurement results revealed that the composites (PU@SiR-GO) showed superior flame retardancy and thermal and mechanical stability compared to pristine PU or PU coated with SiR alone. The mechanical and thermal stability and the flame-retardant properties of the PU composites were enhanced significantly with increasing GO content. Based on the composition, microstructure, and surface morphology of PU@SiR-GO composites before and after combustion tests, a possible flame-retardance mechanism is proposed. This work provides a simple and effective strategy for fabricating flame-retardant composites with improved mechanical performance.