FUEL
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2022
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IF 8.035
Baicheng Feng,Zichen Zhang,Jiaqiang Wang,Donglin Yang,Qun Li,Yaping Liu,Hengjun Gai,Tingting Huang,Hongbing Song
The catalytic hydrogenation of carbon dioxide (CO 2 ) into formic acid is among the most important reactions to alleviate global warming and realize the carbon cycle. How to achieve rapid activation of CO 2 remains a challenge. In this work, we designed two novel hydrophobic poly(ionic liquid)s (PILs) with a good affinity for CO 2 . Since the abundant N atoms in the PILs can anchor palladium (Pd) nanoparticles, the designed catalyst can rapidly activate CO 2 and H 2 simultaneously, thus efficiently catalyzing the hydrogenation of CO 2 to formic acid under mild conditions. Due to the synergy from the bis(trifluoromethanesulfonyl)amide anion ([Tf 2 N − ]) with strong hydrophobicity and CO 2 affinity and trimethylamine (NEt 3 ) as a low dissociation energy alkaline additive, the resultant Pd/PIL-bip-Tf 2 N exhibited the best catalytic performance on the hydrogenation of CO 2 to formic acid. The TOF value reached 1,190 h −1 in the aqueous solution of NEt 3 at 100 °C, 1 h, and a total pressure of 4 MPa. The activation energy and dissociation energy during the catalytic process were calculated by DFT, indicating that the synergistic effect of NEt 3 is better than that of other alkaline additives. In addition, the catalytic activity of the catalyst remained stable after several cycling experiments. Based on the obtained results, we proposed a possible reaction pathway. Therefore, PILs have great potential as catalyst carrier material for CO 2 hydrogenation.
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高影响因子
Materials Today Communications
·
2022
·
IF 3.662
Shaocan Dong,Weiqiu Huang,Xufei Li,Xinya Wang,Baoyou Yan,Zhen Zhang,Jing Zhong
In response to global climate change, most countries have set carbon reduction targets. Mixed matrix membranes (MMMs), which combine the characteristics of inorganic nanofillers and organic matrices, have received wide attentions because of their good permeability and selective performance for the separation of CO 2 from industrial waste gases. However, the poor dispersion, compatibility and interfacial defects often lead to poor gas separation performance. In this paper, according to the dissolution-diffusion and Lewis acid-base theories, inorganic filler of amino-functionalized Bentonite (APTES-Bentonite) with -NH 2 was firstly synthesized to improve the affinity of CO 2 . Then, the dual-functionalized MMMs of APTES-Bentonite/PVDF (A-B/P MMMs) was prepared and adopted for the separation of CO 2 /CH 4 and CO 2 /N 2 , showing the increase of 87.76% and 75.31% compared to the pristine PVDF membrane, respectively. These excellent performances were attributed to the synergistic effect of APTES-Bentonite with -NH 2 groups and PVDF with -F groups, which provide a dual-functional transport pathway for CO 2 molecules due to the interactions of host-guest. Overall, the customized A-B/P MMMs offer superior CO 2 separation performance, which provides some valuable references for large-scale CO 2 capture studies.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Wenjia Luo,Zhenhua Niu,Peng Mu,Jian Li
Membrane separation systems have received extensive attention in the field of gas separation due to its low cost, high-efficiency and eco-friendly advantages. However, it is till challenging to break through the trade-off effect for a highly efficient membrane separation process. Herein, a high-performance CO 2 -philic MXene/PEG mixed matrix membrane is prepared by a simple vacuum filtration process. Excellent CO 2 permeance and selectivity in separation of the CO 2 /N 2 and CO 2 /CH 4 is shown for the as-prepared MXene/PEG (600) mixed matrix membrane because of CO 2 -philic property of the PEG and the nanochannels of the MXene . In permeation experiment, exceptional CO 2 permeance of 1626.99 GPU and ideal selectivity of 32.18 for CO 2 /N 2 and 27.84 for CO 2 /CH 4 , is exhibited, respectively, for 25 wt% MXene/PEG (600) mixed matrix membrane. This study provides a new strategy for design and fabrication of the CO 2 -philic MXene-based membrane with highly efficient separation of the CO 2 from natural gas and flue gas.
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高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
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2020
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IF 2.888
Hui Li,Hui Guo,Shufeng Shen
Water-lean amino acid salt (AAS) solutions have attracted special attentions for energy-efficient CO 2 absorbents. In this work, 2-methoxyethanol was proposed as a novel anti-solvent due to its excellent properties such as low volatility, low specific heat capacity and low viscosity. Density and viscosity were measured at atmospheric pressure for water-lean blends of potassium sarcosinate (SarK) or potassium L -prolinate (ProK)/water/2-methoxyethanol over the temperature range from (293 to 353) K and the AAS molality up to 4.914 mol·kg −1 . Partially CO 2 loaded solutions were also investigated. Equilibrium solubility of CO 2 in AAS/water/2-methoxyethanol solutions was measured in a stirred equilibrium cell at temperatures of (313, 333 and 373) K and CO 2 partial pressures up to 190 kPa. These property data were correlated using empirical correlations as a function of AAS molality, CO 2 molality and/or temperature. The predicted values of density and viscosity matched well with the measured data, with AADs within 0.31% for density and 3.76% for viscosity. The solubility data of CO 2 were fairly fitted with a proposed Soft model.
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高影响因子
FUEL PROCESSING TECHNOLOGY
·
2019
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IF 4.507
Hailong Li,Mingyu Qu,Yingchao Hu
Li 4 SiO 4 has been demonstrated as a promising adsorbent for CO 2 capture. However, Li 4 SiO 4 adsorbents from the conventional solid-state method usually exhibit dense microstructures and, thus, poor CO 2 capture performance. Treating Li 4 SiO 4 with organic acids has been proved effective to improve the microstructures. The commonly used acids such as acetic acid, citric acid and gluconic acid are too expensive, restricting the application of this modification technique. In addition, in the typical Li 4 SiO 4 -based CO 2 capture looping system, CO 2 usually exists in the desorption reactor. However, the effect of the existence of CO 2 at the desorption stage on adsorption performance has been rarely studied. Focusing on these two issues, this work employed pyroligneous acid (PA), a low-cost by-product of the fast pyrolysis of biomass, to modify the microstructures of Li 4 SiO 4 . It was found that modification by pyroligneous acid (PA) successfully improved the microstructures and enhanced the surface area of Li 4 SiO 4 adsorbent. As a result, the obviously improved CO 2 adsorption performance was achieved. In addition, the test results under CO 2 -containing desorption atmospheres indicated that the existence of CO 2 at the desorption stage decreased the adsorption performance due to the severe sintering caused by the existence of CO 2 at the desorption stage.
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Journal of Materials Chemistry A
·
2016
·Vol. 5
·期 4
·1509-1515
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IF 8.262
Shaolei Wang,Kunpeng Song,Chengxin Zhang,Yu Shu,Tao Li,Bien Tan
A novel metalporphyrin-based microporous organic polymer (HUST-1-Co), which possesses a high surface area of 1360 m2 g−1 and a high CO2 uptake of 21.39 wt% (1 bar and 273 K) for CO2 capture and storage (CCS) and the efficient chemical conversion of CO2 under ambient conditions, is reported. This polymer incorporated both ultra-micropores and catalytic sites, and was synthesized by a novel solvent knitting hypercrosslinked polymers method, using 5,10,15,20-tetraphenylporphyrin (TPP) as the building block. The N2 sorption isotherms of the polymers show that HUST-1-Co possesses abundant ultra-micropores (centered at 0.68 nm), and a continuous mesoporous and macroporous structure, which not only enhances the interaction between the pore walls and CO2, but is also favourable for the catalysis process. The synergy of the ultra-micropores, abundant nitrogen atoms and Co2+ ions makes HUST-1-Co one of the highest CO2 uptake MOP materials reported so far and further endows it with efficient catalytic performance. HUST-1-Co is one of the most efficient catalysts for the coupling of CO2 with substituted epoxides with various functional groups at room temperature and atmospheric pressure, with an excellent recycling performance (more than 15 times). Moreover, the role of the mesoporous and macroporous structure of HUST-1-Co gives it a unique catalytic performance for different molecular sizes of epoxide substrates with excellent yields (>93%).
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FLUID PHASE EQUILIBRIA
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2017
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IF 2.473
Qiaoyan Shang,Shuqian Xia,GuanWei Cui,Bo Tang,Peisheng Ma
Interfacial tension (IFT) is crucial for characterizing the phase and interphase behavior in the enhanced oil recovery (EOR) process. CO 2 and N 2 are commonly used as injection gases in the EOR process. In this work, an experimental apparatus using the pendent drop method was adopted to measure IFTs for the EOR process with different injection gases, temperatures (40.0–120.0 °C) and pressures (0.22–17.32 MPa). The relative Gibbs adsorption isotherm ( Γ ij ) of a species i on species j were calculated by the experimental IFTs. Theoretically, new correlations were proposed to predict paraffin IFTs for pure CO 2 and mixture gas (CO 2 + N 2 ) injection. A total of 561 and 268 experimental IFTs were used to derive the correlations for pure CO 2 and mixture gas injection, respectively. The square of correlation coefficient ( R 2 ), root mean square error ( RMSE ) and average absolute relative deviations ( AARD ) for pure CO 2 were 0.9884, 0.58 and 5.45%, respectively. For the mixture gas injection, the R 2 , RMSE and AARD of the correlation were 0.9851, 0.57 and 4.47%, respectively.
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ENERGY & FUELS
·
2025
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IF 5.3
Qing Sun,Qingqiao Zhao,Lifang Zhang,Fengjun Ming,Weidong Zhang
Water lean solvents have received growing attention for CO2 capture due to their low solvent evaporation and potential for energy saving. The previous study mainly focused on the organic diluent selection and paid less efforts on the amine effect. In this study, 11 types of amines with representative structures were selected to explore the effect of amine on CO2 loading and CO2 distribution with poly(ethylene glycol) dimethyl ether (NHD) as organic diluent. Based on the cyclic loading and reaction heat comparison, N-ethylethanolamine (EAE) was selected and the EAE/NHD water lean solvent was constructed. The liquid–liquid phase separation was found in the EAE/NHD/H2O system with more than 95% CO2 concentrated in the lower phase, which yielded high cyclic loading and benefited regeneration energy consumption. The water content effect was further investigated in terms of CO2 cyclic loading and phase separation behaviors, suggesting that EAE/NHD/H2O with a mass ratio of 3:6:1 exhibited the excellent performance of 3.03 mol·kg–1 cyclic loading and 2.27 GJ·t–1 CO2 regeneration energy consumption. 13C NMR and quantum chemistry calculations were conducted to explain the reaction route and phase change mechanism. The large difference between the ion–dipole interaction of ion–H2O and the molecule–molecular interaction of ion-NHD was regarded as the main reason for phase separation. The long-term tests indicated the cycling stability and low corrosivity of EAE/NHD/H2O, as exhibited by the stable CO2 cyclic loading during 8 runs of absorption–desorption and lower corrosivity rate of carbon steel than 30 wt % MEA aqueous solution.
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Advanced Energy Materials
·
2024
·
IF 24.4
Xiecheng Yang,Dantong Zhang,Lanqing Zhao,Chao Peng,Kun Ren,Changfan Xu,Pan Liu,Yingjie Zhou,Yong Lei,Bin Yang,Dongfeng Xue,Feng Liang
Rechargeable Na-CO 2 batteries are considered to be an effective way to address the energy crisis and greenhouse effect due to their dual functions of CO 2 fixation/utilization and energy storage. However, the insolubility and irreversibility of solid discharge products lead to poor discharge capacity and poor cycle performance. Herein, a novel strategy is proposed to enhance the electrochemical performance of hybrid Na-CO 2 batteries, using water-in-salt electrolyte (WiSE) to establish an optimal reaction environment, regulate the CO 2 reduction pathway, and ultimately convert the discharge product of the battery from Na 2 CO 3 to formic acid (HCOOH). This strategy effectively resolves the issue of poor reversibility, allowing the battery to exhibit excellent cycle performance (over 1200 cycles at 30 °C), especially under low-temperature conditions (2534 cycles at −20 °C). Furthermore, density functional theory (DFT) calculations and experiments indicate that by adjusting the relative concentration of H/O atoms at the electrolyte/catalyst interface, the CO 2 reduction pathway in the battery can be regulated, thus effectively enhancing CO 2 capture capability and consequently achieving an ultra-high discharge specific capacity of 148.1 mAh cm −2 . This work effectively promotes the practical application of hybrid Na-CO 2 batteries and shall provide a guidance for converting CO 2 into products with high-value-added chemicals.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Min Deng,Jing Wei,Zikang Qin,Zheng Yan,Junfeng Zheng,Lin Yang,Lu Yao,Wenju Jiang,Zhongde Dai
Styrene-butadiene-styrene triblock copolymer (SBS) has attracted increasing research attention due to its low cost, excellent mechanical properties, and superior gas permeability performance. In this work, a series of novel SBS doped membranes were prepared by introducing polyphosphoric acid (PPA), lithium 2,2,2- trifluoroacetate (TFALi), and 1,3-dichloro-1,1,3,3-tetraisopropyldisiloxane (Siloxane-Cl) into SBS as dopants. The results indicated that the addition of dopants into SBS membranes simultaneously enhanced the CO 2 permeability and CO 2 /N 2 selectivity of SBS membranes. Specially, doping Siloxane-Cl expanded the d-spacing, introduced flexible siloxane (Si-O) groups to enlarge molecular spaces, and formed more crosslinked network structure. Therefore, the SBS/Siloxane-20 membrane showed an approximately 4-fold increase CO 2 permeability compared to the pristine SBS membranes (from 203.3 to 842.9 barrer), accompanied by an increase in CO 2 /N 2 selectivity from 15.8 to 22.0. The obtained membranes also exhibited attractive anti-plasticization and anti-physical aging properties, no obvious decline in CO 2 permeability and/or CO 2 /N 2 selectivity can be observed after 1-week continuous permeation test, making them promising candidates for CO 2 /N 2 separation.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2025
·
IF 3.7
Yiqian Yang,Gang Wang,Xiaoyan Sun,Shuguang Xiang,Chunshan Li
Gas-liquid hydrodynamic characteristics under chemical reaction-enhanced mass transfer are crucial parameters for analyzing mass transfer behavior in microreactor, which can facilitate the optimization of the reaction conditions to achieve efficient mass transfer and improve catalytic performance. Herin, the movement and shrinkage of CO 2 bubbles in the microreactor were visualized and monitored using a high-speed camera. Four typical patterns such as bubble flow, bubble-Taylor flow, Taylor flow and Taylor-annular flow were observed, and the impact of temperature on flow pattern transition lines was investigated. Furthermore, the correlation models for predicting dimensionless initial CO 2 bubble length ( L B / d ) and liquid-side volumetric mass transfer coefficient were developed to illustrate the effects of reaction conditions on the hydrodynamics and mass transfer behavior of CO 2 bubble accompanying the chemical reaction. This work deepens the understanding of the hydrodynamics and mass transfer characteristics in a real CO 2 cycloaddition reaction system and provides a theoretical basis for the design and optimization of gas-liquid microreactor.
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JOURNAL OF MATERIALS SCIENCE
·
2025
·Vol. 60
·期 48
·25741-25761
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IF 3.9
Gao Ningning,Pan Yucheng,Huang Wei,Xin Qingping,Zhang Min,Wu Jiaxin,Wu Dengdi,Wang Mengke,Ding Xiaoli,Lin Ligang,Zhang Yuzhong
Due to its benefits of low energy consumption, minimal environmental pollution, and simple operation, membrane technology is considered a carbon capture technology with extensive application possibilities. In this study, the ultraviolet cross-linking method is used to inhibit crystallization of polymers with a molecular weight of less than 1500 and enable polyethylene oxide (PEO) to form a rubbery polymer matrix. This approach avoids membrane separation defects and low CO 2 solubility caused by high crystallinity. The hydroxyl-rich surface of layered double hydroxide (LDH) is used to provide the CO 2 -philic site in the form of “docking station-like” by introducing amino groups with a strong affinity for CO 2 , and forming a dual facilitated transport channel through the nanosheet interlayer channel and the presence of bound water to strengthen the reaction mechanism of the membrane. Based on the coupling of solubility-diffusion and facilitated transport mechanisms, the optimal separation performance is achieved when the NH 2 -PDA-LDH doping is 0.4 wt%, with a CO 2 permeability of 572.4 Barrer and a selectivity of up to 60.5. The interlayer fast transport channels result in a maximum permeability of 3982 Barrer in the wet state. Graphical
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