MACROMOLECULES
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2024
·
IF 5.1
Fuwei Wang,Guoke Zhao,Yiqun Liu,Gongqing Tang,Peiyong Qin,Pei Li
Thermally rearranged (TR) polymers have good gas separation property, but the high TR temperature often caused pore collapsing and embrittlement of hollow fiber. We designed two copolyimides by reacting a TR-able 3,3′-diaminophenolphthalein (DAP), and two non-TR able diamines, 2,4,6-trimethyl-m-phenylenediamine (DAM) and diethyl-toluene diamine (DETDA) with hexafluoroisopropylidene diphthalic anhydride (6FDA) using azeotropic distillation. The bulky DAM and DETDA diamines and the hydrogen bonding provided by the OH groups of DAP enabled high glass transition temperatures of Co-PI-DAM and Co-PI-DETDA copolyimides so that the thermal cross-linking and TR reaction realized at sub-Tg. Moreover, compared with the 6FDA–DAP polyimide, copolymerization greatly improved the tensile strength from 35 to 75 MPa (Co-PI-DAM). The cross-linked TR polymers exhibited high separation performance to CO2/CH4 and were not plasticized by CO2 at 30 atm. The two copolyimides show great potential for fabricating TR hollow fiber membranes.
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ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Yong Song,Zhiyuan Jin,Jiawei Zhang,Bo Jin,Rufang Peng
In this work, we report a novel spiral gas–solid two-phase flow (S-GSF) technique for the continuous mechanochemical synthesis of N-acylhydrazone derivatives. The synthesis of (E)-N′-(4-nitrobenzylidene)benzoylhydrazide (compound 1) was used as a model reaction to demonstrate the feasibility of this approach. The prepared products were characterized by Fourier transform infrared spectroscopy, nuclear magnetic resonance, powder X-ray diffraction, differential scanning calorimetry, thermogravimetric analysis, ultraviolet–visible (UV–vis) spectroscopy, and scanning electron microscopy (SEM). Results showed that the product prepared by this method was analytically pure and had a high yield. No solvent was used in the reaction, and the byproduct water was in the form of water of crystallization. Moreover, SEM images showed that the method can directly obtain ultrafine powder products that are attractive to the pharmaceutical industry. Subsequently, kinetic analysis was performed by detecting the UV–vis spectra of the products under different optimized reaction conditions. The green chemistry metrics of the method showed that it is more environmentally friendly than the conventional solution method. In addition, the method was used in preparing a variety of N-acylhydrazone derivatives by using aldehydes with different substituents.
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ANALYTICAL LETTERS
·
2024
·
IF 1.6
Yigong Geng,Shun Zhang,Jing Lin,Xuchu Zhu,Wenqing Gao,Junhui Li,Chenlu Wang,Yong Wu,Renlu Han,Keqi Tang,Jiancheng Yu
Ethanol abuse is increasingly becoming a global issue, adversely affecting both society and families. In blood alcohol concentration (BAC) detection, traditional techniques have long experimental cycles and harsh experimental conditions and often fail to produce timely results. Consequently, achieving swift and precise on-site detection of ethanol poisoning in humans poses a formidable challenge in analytical science. We designed a novel assay for swift on-site analysis of ethanol and BTEX (benzene, toluene, ethylbenzene, and xylene) poisoning in humans using a custom portable headspace injector (portable HS) and portable gas chromatography-mass spectrometry (portable GC-MS). This setup, known for its lightweight design and speed, allows on-site sampling and delivers rapid results. We established a calibration curve (R2 > 0.99) for ethanol in blood using portable gas chromatography-mass spectrometry (portable GC-MS). This on-site blood alcohol concentration (BAC) assay proves simpler than traditional methods, enabling rapid analysis of each sample within a short timeframe and requiring only a small blood volume (0.1 ml). In addition to our investigation on ethanol, we developed a portable method for detecting BTEX in blood. This method provides a favorable coefficient of determination (R2 > 0.99) for various substances, thereby broadening the utility of portable mass spectrometry in areas such as traffic inspection and forensic identification.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xingbo Wang,Yibo Pan,Weidong Fan,Hao Guo,Hai Zhang
CaO-based sorbents are among the most promising materials for capturing CO 2 from high-temperature flue gas in coal-fired power plants. Fly ash, a solid waste product generated by coal-fired power plants, can be utilized as a calcium source for the in-situ preparation of CaO-based sorbents to capture CO 2 from high-temperature flue gas. Nevertheless, the inherent characteristics of fly ash, such as its low adsorption capacity and poor activity, present challenges in its utilization. Doping is an effective method for enhancing the adsorption capacity and activity of sorbents. In this study, fly ash-CaO sorbents were doped and hydrated with six common chlorides and hydroxides in order to investigate the potential effects of the dopants on the sorbents. The carbonation performance of these sorbents was evaluated in a calcination/carbonation reaction system, and the modified sorbents were characterized using multiple methods to elucidate the underlying mechanisms. The results indicate that the carbonation conversion of the six modified sorbents is in the order of Fe(OH) 3 / Fe(Cl) 3 > KCl > NaCl > KOH>NaOH. The element enhancement of the modified sorbents at the same doping ratio is in the order of Fe 3+ > K + > Na + , and Cl − exhibit better synergistic effects with K + and Na + compared to OH − . Some dopants improve the carbonation reaction kinetics of the sorbents, promoting the overall reaction shift towards the rapid reaction stage. This study provides a promising pathway for the reuse of solid waste fly ash and the development of CaO-based sorbents suitable for rapid reaction scenarios.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Dongxu Zhang,Xin Wang,Cheng Liu,Lechun Song,Huiyuan Li,Qiyu Huang,Jianfeng Zhang
Hydrate formation is one of the major flow assurance issues for the subsea multiphase pipelines. The effects of the interaction between heavy fractions of crude oil components on hydrate behaviors are still not well understood. In this study, the effects of resins on hydrate formation behaviors in asphaltene-containing emulsions were investigated using a high-pressure reactor apparatus. The results indicated that both resins and asphaltenes inhibited hydrate nucleation and increased the induction time. Furthermore, considerable synergistic effects of asphaltenes and resins on the hydrate formation behaviors were discovered in the water-in-oil emulsions, depending on the aggregation state of asphaltenes. The addition of resins was observed to disperse the asphaltene aggregates significantly and enhance the inhibitory effect of asphaltenes on hydrate nucleation. Additionally, the calculated results of gas consumption showed that the presence of resins can decrease the growth rate of hydrates in the asphaltene-containing emulsions. A potential mechanism was presented to illustrate how resins affect hydrate formation in an emulsion with varying asphaltene aggregation states. These findings offer a better knowledge of the synergistic effects between the heavy components of resins and asphaltenes and have potential application in the hydrate management of crude oil pipelines.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Guoxuan Tang,Yu Chen,Jiaojiao Chen,Lin Liu,Haocun Wen,Wenda Liu,Jingyun Liu,Zeyi Xiao,Senqing Fan
Several CoS 2 /Ni flow-through porous electrodes are fabricated to promote gas bubble release for enhanced oxygen evolution reaction. Structural characterization shows that CoS 2 catalyst is immobilized on the porous Ni substrate. The bubble average diameter can be decreased from 29.21 ± 17.9 μm to 13.38 ± 5.05 μm, and the desorption time is decreased from 1.615 s to 0.067 s, with the electrolyte velocity increasing from 0 cm/s to 2.89 cm/s at the current density of 100 mA/cm 2 . A mathematical model is proposed to describe gas bubble growth, which is found that higher current density is not bring much bigger gas bubble. The overpotential of the CoS 2 /Ni electrode for OER is 498 mV at 100 mA/cm 2 . The overpotential of CoS 2 /Ni electrode can be decreased from 754 mV to 661 mV with the electrolyte velocity increase from 0 cm/s to 9.42 cm/s at 200 mA/cm 2 with the energy required for hydrogen production reduced by 5.01 kWh/kmol.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Fangxu Fan,Yongchao Sun,Lu Bai,Tianyou Li,Zeyuan Gao,Gaohong He,Canghai Ma
Thermally rearranged (TR) material has emerged as a focal point in gas separation membranes. However, further enhancing the gas separation performance of TR materials remains a key hurdle. In this study, fluorinated-cardo-based diamine (FFDA) was strategically incorporated into the polybenzoxazole structure to improve the gas selectivity. The size-sieving ability of the polymers was significantly enhanced through the interchain hydrogen bonding and π-π stacking induced by the cardo groups. Furthermore, the aromatic fluorine atoms in FFDA exhibited superior CO 2 adsorption capacity. As the thermal rearrangement progressed and the polybenzoxazole structure developed, pores with a diameter of approximately 3 Å were formed, leading to increased diffusion rate of CO 2 and H 2 . The TR400 °C membranes surpassed the 2018 CO 2 /CH 4 mixed-gas upper bound. Particularly, the 6FDA-FFDA/6FAP(1:1)-TR400 membrane achieved a CO 2 permeability of 185.3 Barrer and a CO 2 /CH 4 selectivity of 79.9—representing increases of 227.3 % and 37.5 %, respectively, compared to the precursor membranes. Moreover, the robust structure of the membrane demonstrated enhanced plasticization resistance, with no discernible plasticization observed under CO 2 /CH 4 mixed-gas conditions up to 20 bar. Our design approach paves the way for developing mechanically robust and highly selective TR membranes, with significant potentials for application in CO 2 separation under aggressive conditions.
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Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Wen-Wang Yu,Xiang-Guang Meng,Wen Li,Li-Yu Chen,Zi-Yu Gan,Yu-Lian Zhang,Jie Zhou
Chemical conversion of CO 2 to cyclic carbonates is one of the most attractive strategies for CO 2 capture and storage utilization. Herein, a binary organocatalyst of 3-aminobenzylalcohol/ n -Bu 4 NI was used to gently catalyze the insertion of CO 2 into the terminal/internal epoxides to generate cyclic carbonates under metal-free and solvent-free conditions. Twelve representative terminal epoxides reacted with CO 2 to achieve excellent cyclic carbonate yields of up to 98.3 % at 30 °C and 1 atm CO 2 and six low activity internal di-substituted epoxides were converted to corresponding cyclic carbonates with yields of up to 96.2 %. Experiments on actual flue gas and water resistance revealed the potential industrial value of this binary organocatalyst. The yield of cyclic carbonate reached 99 % by using actual flue gas under very mild conditions of 60 °C and 1 atm. The results of 4-fold epoxide amplification experiment showed that the residual CO 2 in the flue gas was only 793 ppm after reaction at 1 atm and 60 °C, indicating the good CO 2 capture and conversion ability. Reaction kinetics and catalytic mechanism of the cycloaddition were investigated in detail. The synergistic effect among functional groups of catalysts on substrates is the essential factor for the high activity of the catalyst.
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RENEWABLE ENERGY
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2024
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IF 9
Xiaofeng Gu,Xiaomin Yan,Mingyang Zhou,Gaochang Zou,Zidai Fan,Jiang Liu
For the first time, biochar derived from a renewable resource, cotton stalk, is used as the feedstock of direct carbon solid oxides fuel cells (DC-SOFCs) for electricity and gas cogeneration. It turns out that the cotton stalk biochar has plenty of naturally grown K and Ca, which are active catalysts for the reverse Boudouard reaction in DC-SOFCs. This natural advantage of the cotton stalk biochar enables an extremely high power density of an anode-supported DC-SOFC at 850 °C, 0.9 W cm −2 , which is the highest among those of the reported DC-SOFCs. Meanwhile, high concentration of CO gas, which is an important feedstock for chemical industry, is obtained from the DC-SOFCs. The energy conversion efficiency of the electricity-gas cogeneration of DC-SOFCs reaches over 70%. A novel method, using compressed char, is proposed and carried out for continuous supply of cotton stalk char to a DC-SOFC. The present work has demonstrated the feasibility and advantages of cogenerating electricity and gas through DC-SOFCs with biochar derived from cotton stalk as the feedstock.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Dong Li,Renyi Li,Yizhou Zhao,Kaixuan Wang,Ke Fan,Wei Guo,Qi Chen,Yujing Li
Perovskite CsPbBr 3 quantum dot shows great potential in artificial photosynthesis, attributed to its outstanding optoelectronic properties. Nevertheless, its photocatalytic activity is hindered by insufficient catalytic active sites and severe charge recombination. In this work, a CsPbBr 3 @Ag-C 3 N 4 ternary heterojunction photocatalyst is designed and synthesized for high-efficiency CO 2 reduction. The CsPbBr 3 quantum dots and Ag nanoparticles are chemically anchored on the surface of g-C 3 N 4 sheets, forming an electron transfer tunnel from CsPbBr 3 quantum dots to Ag nanoparticles via g-C 3 N 4 sheets. The resulting CsPbBr 3 @Ag-C 3 N 4 ternary photocatalyst, with spatial separation of photogenerated carriers, achieves a remarkable conversion rate of 19.49 μmol·g −1 ·h −1 with almost 100 % CO selectivity, a 3.13-fold enhancement in photocatalytic activity as compared to CsPbBr 3 quantum dots. Density functional theory calculations reveal the rapid CO 2 adsorption/activation and the decreased free energy (0.66 eV) of *COOH formation at the interface of Ag nanoparticles and g-C 3 N 4 in contrast to the g-C 3 N 4 , leading to the excellent photocatalytic activity, while the thermodynamically favored CO desorption contributes to the high CO selectivity. This work presents an innovative strategy of constructing perovskite-based photocatalyst by modulating catalyst structure and offers profound insights for efficient CO 2 conversion.
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PubMed
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 21
·15039-15047
·
IF 3.9
Zhixiang Deng,Zhixuan Wu,Xinkuan Liu,Zhengai Chen,Yan Sun,Ning Dai,Meiying Ge
The influence of ambient humidity on the gas-sensing characteristics of metal oxide semiconductors has been one of the greatest obstacles for gas-sensing applications. In this paper, the pure WO3 and CeO2-modified WO3 nanocubes were prepared by a simple hydrothermal method, and their gas-sensing characteristics in dry and humid atmospheres were investigated. The results show that CeO2/WO3 demonstrated excellent gas-sensing properties toward H2S with high sensitivity and high selectivity at 115 °C. Noteworthy, the humidity independence of the CeO2/WO3 increased compared to the WO3. The response retentions over the whole humidity range of the CeO2/WO3-6 and CeO2/WO3-15 sensors were 70.3, and 76%, respectively, which were much higher than the WO3 sensor (17.9%). The gas-sensing mechanism of CeO2-modified WO3 is discussed based on the gas sensitivity properties. The obtained results provide a promising route to enhance the anti-humidity properties of metal oxide semiconductor gas sensors.
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Chemosensors
·
2024
·Vol. 13
·期 1
·3
·
IF 3.7
Jiaying Sun,Zhuoru Huang,Xiaojing Zhang,Hangming Xiong,Weijie Yu,Shimeng Mou,Wenwu Zhu,Hao Wan
Methane is a common intestinal gas that has been linked to a variety of gastrointestinal disorders. In this study, we prepared a LIG-based electrochemical sensor modified with PEDOT:PSS/Au-Pt nanocomposites for high-sensitivity methane detection. LIG’s high porosity, flexibility, and excellent electrical conductivity are beneficial for electrochemical detection. The PEDOT:PSS film is electrodeposited on the electrode surface to amplify the signal further. The synergistic effect of bimetallic nanocomposites can improve the electrochemical catalytic activity and increase the specific surface area and the advantages of active sites. The experimental results show that the LIG sensor has a wide linear detection range (2–500 ppm), a low detection limit (about 0.36 ppm), high sensitivity, and good repeatability. The sensor is easy to manufacture, is low-cost, operates at room temperature, has high sensitivity, has a low detection limit, and is expected to be used for methane breath detection in the future.
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