MATERIALS RESEARCH BULLETIN
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2017
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IF 2.446
Aisheng Huang,Linlin Wan,Jürgen Caro
In a detailed study, the influence of microwave irradiation, synthesis time and temperature, addition of acetic acid (HAc) as a modulator on the morphology, crystallinity and stability of UiO-66-NH 2 is investigated to develop a reliable and reproducible strategy for the preparation of well-shaped UiO-66-NH 2 . The UiO-66-NH 2 were characterized by powder X-ray diffraction (PXRD), field emission scanning electron microscopy (FESEM), thermogravimetric analysis (TGA), and gas adsorption. It is found that well-shaped UiO-66-NH 2 with a high CO 2 adsorption capacity can be synthesized in a short time by microwave heating. The UiO-66-NH 2 crystals synthesized by microwave heating are of high quality and show a superior CO 2 adsorption capacity (5.8 mmol/g at 273k and 1 bar) due to the strong interactions between the −NH 2 group and CO 2 . The CO 2 /N 2 selectivity of the obtained UiO-66-NH 2 at 298 K and 1 bar is 66, which is much higher than that of the pristine UiO-66 of 17.8.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2017
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IF 5.951
Yaju Chen,Rongchang Luo,Qihang Xu,Jun Jiang,Xiantai Zhou,Hongbing Ji
Multifunctionalization of organic polymers for acting synergistically on substrate is of wide interest in the field of modern catalysis, but it is still a significant challenge. Herein, two novel bifunctional polymers were first designed and synthesized by combining ionic liquids (ILs) with zinc(II) porphyrin through simple and reversible Schiff base reactions. The fabricated polymers with flexible structures and nitrogen-rich environments presented high affinity toward CO2 molecules at ambient conditions. Owing to the cooperative nature of intercalated ILs and Lewis acidic metal sites, these materials could serve as efficient heterogeneous catalysts for the insertion of CO2 into epoxides to produce cyclic carbonates. As expected, these polymers exhibited good catalytic performance, robust constancy, excellent recyclability, and good substrate expansibility for this reaction in the absence of cocatalyst under mild or even ambient conditions. Notably, the selected catalyst SYSU-Zn@IL2 could directly convert diluted CO2 (15% CO2 in N2) into cyclic carbonate at 80 °C and 3.0 MPa, further offering the great application potential for recycling real-world carbon resource.
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高影响因子
Journal of CO2 Utilization
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2017
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IF 4.292
Tianze Xie,Jianyang Wang,Fanshu Ding,Anfeng Zhang,Wenhui Li,Xinwen Guo,Chunshan Song
The effect of support pore size of FeK/Al 2 O 3 catalysts on the catalytic performance in CO 2 hydrogenation reaction was investigated. A total of 8 iron-based catalysts supported on alumina with different pore size were prepared by incipient wetness impregnation where the amount of Fe and K were fixed at 15 and 10 wt%, respectively. N 2 adsorption/desorption, XRD, TPR and PZC were used to characterize the supports and catalysts. The results show that the support pore size impacts the size of Fe 2 O 3 particles formed in the catalyst; increasing pore size of Al 2 O 3 supports led to increased size of Fe 2 O 3 particles formed in the pores. Catalyst pore sizes of 7–10 nm and the corresponding Fe 2 O 3 particle sizes of 5–8 nm were the most active for CO 2 hydrogenation to hydrocarbons. Outside this range, larger pore size further decrease the iron dispersion and reduce the number of active sites; smaller pore size is not favorable on account of the too small Fe 2 O 3 particle sizes and lower reducibility of the small particle.
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International Journal of Greenhouse Gas Control
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2016
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IF 4.064
Shufeng Shen,Yangyang Bian,Yue Zhao
High energy consumption for aqueous amine-based CO 2 capture process is still a major drawback limiting its commercial deployment. Most of heat is used for water vaporization during solvent regeneration for CO 2 stripping. Development of phase-changing solvents is an attractive energy-efficient method to reduce energy requirement. In this work, we have proposed potassium prolinate (ProK)/ethanol solution as a novel non-aqueous absorbent. Its physical properties and the rate of CO 2 absorption were investigated and compared with the aqueous ProK systems. Phase behaviours during CO 2 absorption and partition of CO 2 absorbed between liquid and solid phases were characterized. The main species in solid precipitates were identified as bicarbonate and proline salts by 13 C NMR and XRD. Moreover, the regenerated absorbents can remain relatively stable after absorption-desorption cycles.
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ELECTROCHEMISTRY COMMUNICATIONS
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2016
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IF 4.569
Zheng Xia,Wenze Qiu,Han Bao,Bin Yang,Lecheng Lei,Zhikang Xu,Zhongjian Li
A novel solid polymer electrolyte was developed by co-deposition of catechol (CCh) and polyethyleneimine (PEI) on a polypropylene membrane for electrochemical reduction of CO 2 (ERC) in gas phase. ERC performance was both investigated in a gas-gas mode and a gas-liquid mode. The maximum CO production rate was 121 μmol/h and the faradaic efficiency was 51% in the gas-liquid mode, which were much higher than those obtained with AM-7001 under the same condition. The high loading rate of quaternary ammonium ions on the membrane and the large surface area provided by the porous nano-structure of the membrane contribute to the high ERC efficiency. Furthermore, the cost of the CCh/PEI-Q membrane was much lower than commercial Nafion membranes, endowing this novel composite SPE with great potential in industrial application.
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Reaction Chemistry & Engineering
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2024
·Vol. 10
·期 1
·203-213
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IF 3.4
Ning Ma,Liu Yang,Zhenchang Fang,Kaijia Jiang,Xinling Li,Zhen Huang
Deficiencies such as high viscosity, volatility, and rich phase precipitation limited the engineering application of non-aqueous absorbents. A series of high boiling point solvent screening experiments were conducted to develop an absorption saturated solution with a homogeneous phase at low viscosity (14.71 mPa s) in this study. Further addition of polyamines increased the absorption capacity by 42% (3.55 mol CO2 per kg). The 13C NMR results indicated that in the DETA/MEA/NMF blended amine system, MEA was involved in the deprotonation process of DETA zwitterions as proton acceptors. Quantum chemical calculations were utilized to compare the energies of each possible single-step reaction, providing insights into the reaction pathways of the blended amine system. The rate constant of the MEA/CO2 reaction was found to be 1.98 times that of the DETA/CO2 reaction, indicating lower reaction activity, consistent with NMR results. In addition, the results of the analysis of weak interactions revealed that the hydrogen bonds were key factors affecting the viscosity change and precipitation in non-aqueous absorbents, providing a new method for designing novel low-viscosity non-aqueous absorbents. The combination of theoretical analysis and experimental results underscores the potential of the blended amine non-aqueous absorbent as a feasible alternative for the industrial applications of CO2 capture.
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Applied Sciences-Basel
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2024
·Vol. 14
·期 20
·9232
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IF 2.5
Tao Jia,Jinpeng Yang,Jia Yu
Understanding the density of CO2+n-decane is crucial for designing and operating CO2capture, transport, and storage. The safety and effectiveness of CO2burial is directly affected by the density of CO2+n-decane mixtures. The liquid densities of CO2(1) +n-decane(2) mixtures with mole fractions of CO2x1= 0, 0.2032, 0.4434, 0.7589, and 0.8947 were measured using a vibrating tube densimeter. The combined expanded uncertainties of density with a level of confidence of 0.95 are estimated to be 0.6 kg·m−3. A total of 221 compressed liquid densities of CO2(1) +n-decane(2) mixtures along the five isotherms betweenT= (283 and 363) K with pressures up to 100 MPa were presented. The densities of mixtures were correlated by the modified Tait equation, resulting in absolute average deviations between the experimental and calculated values of 0.028%, 0.013%, 0.017%, 0.044%, and 0.042%. In addition, the isothermal compressibility, isobaric thermal expansivity, and excess molar volume were derived from the modified Tait equation.
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ACS Applied Energy Materials
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2024
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IF 5.4
Xiang Li,Zhitao Liu,Liyuan Zeng,Wanyi Ye,Guangxing Yang,Qiao Zhang,Shengjun Du,Zhiting Liu,Feng Peng
The CO2 electrochemical reduction (CO2ER) to produce valuable multicarbon products represents a promising approach for enhancing CO2 conversion. While previous research has investigated the impact of Cu electrode surface topography on C2 production, it is important to note that other parameters were also altered concurrently with changes in roughness. To isolate the specific effect of surface texture on CO2 electroreduction, this study prepared Cu layers with varying textures using the sputtering method with a varied sputtering time. To characterize the surface features of the sputtered Cu layers, the developed interfacial area ratio (Sdr), known as areal parameter, was introduced, with the aim of correlating it with C2 product selectivity. The results of this study indicate that the improved selectivity of C2 products can be attributed to higher Sdr values, primarily due to a rougher and finer surface texture that increases the local concentration of CO and OH–. This research underscores the significance of surface topography and offers perspectives for designing efficient Cu electrodes for the CO2ER.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Fan Sun,Xueli Xing,Chunyang Zhang,Jinrui Zhang,Hui Hong
Photocatalytic CO2 reduction with naturally abundant H2O as the proton source has attracted widespread concern for its environmental and sustainable advantages. Nevertheless, the high recombination rate of photogenerated electron–hole pairs leads to unsatisfactory solar-to-chemical energy conversion efficiency. In this work, we proposed and validated a strategy that photothermal–magnetic synergistically promotes the separation of photogenerated carriers, as well as their transport, leading to boosted photocatalytic performance. A paramagnetic Z-scheme ZnFe2O4/TiO2 heterojunction was fabricated, and its performance in CO2 reduction was examined under concentrated full-spectrum light illumination with an applied external magnetic field. The built-in electric field of the Z-scheme heterojunction improved the dynamic properties of electron–hole pairs. At the same time, the thermal effect induced by infrared light played a crucial role in promoting CO2 conversion. Importantly, the applied external magnetic field further suppressed the recombination of charge carriers via Lorentz force, magnetoresistance, and spin-polarization effects. As a result, the assistance of a magnetic field significantly increased the yields of CO, CH4, and H2 in comparison to the absence of a magnetic field, with maximum enhancements of 25.3, 29.6, and 62.9%, respectively. Moreover, the excessive heating due to the higher concentrated ratio may induce magnetic disorder within the material, potentially reducing the magnetic field’s ability to facilitate carrier transport. The photothermal–magnetic synergy mechanism was systematically explored. Our work has presented a new approach in which photothermal–magnetic effects synergistically contribute to solar fuel production.
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ChemPlusChem
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2024
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IF 3
Lixia Zhang,Lizhen Zeng,Jingting Wang,Haoran Wang,Decong Zheng,Xiaomei Wang,Daping Li,Guoqiang Zhan
Graphical A MoS 2 catalyzed bioelectrochemical system is successfully constructed, in which microbial protein can be produced from the simplest small molecule substances (CO 2 , N 2 , and H 2 O) and Xanthobacter -dominanted hydrogen oxidizing bacteria can be enriched. Additionally, MoS 2 can improve biofilm extracellular electron transfer (EET) and enhance proline production. Carbon dioxide can be relatively easily reduced to organic matter in a bioelectrochemical system (BES). However, due to insufficient reduction force from in-situ hydrogen evolution, it is difficult for nitrogen reduction. In this study, MoS 2 was firstly used as an electrocatalyst for the simultaneous reduction of CO 2 and N 2 to produce microbial protein (MP) in a BES. Cell dry weight (CDW) could reach 0.81±0.04 g/L after 14 d operation at −0.7 V (vs. RHE), which was 108±3 % higher than that from non-catalyst control group (0.39±0.01 g/L). The produced protein had a better amino acid profile in the BES than that in a direct hydrogen system (DHS), particularly for proline (Pro). Besides, MoS 2 promoted the growth of bacterial cell on an electrode and improved the biofilm extracellular electron transfer (EET) by microscopic observation and electrochemical characterization of MoS 2 biocathode. The composition of the microbial community and the relative abundance of functional enzymes revealed that MoS 2 as an electrocatalyst was beneficial for enriching Xanthobacter and enhancing CO 2 and N 2 reduction by electrical energy. These results demonstrated that an efficient strategy to improve MP production of BES is to use MoS 2 as an electrocatalyst to shift amino acid profile and microbial community.
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PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Yihan Yin,Qi Liu,Min Xiao,Hongxia Gao,Bo Jin,Zhiwu Liang
Membrane absorption has garnered significant attention due to its ability to combine the advantages of membrane separation and chemical absorption methods. During the scale-up of membrane absorption equipment, the fluid flow and mass transfer processes tend to have serious non-ideal effects, arising from the increase in aspect ratio and the number of membrane fibers. However, traditional one-dimensional (1D) and two-dimensional (2D) models are unable to describe the impact of geometry on mass transfer performance. In this study, a three-dimensional (3D) steady-state model is established to simulate the mass transfer process in a multi-fiber membrane contactor using COMSOL Multiphysics software. The 3D steady-state model is proven to be able to accurately predict the CO 2 absorption flux (J CO2 ) under various operating conditions by comparing the simulation results with experimental data. The results indicate a strong correlation between mass transfer performance and fluid velocity distribution. To further explore the flow behavior of gas and liquid at different locations, a 3D dynamic simulation model is developed and compared with experimental data. This model can describe the non-ideal flow behavior and the characteristics of gas and liquid phases in reactors with complex geometries. The results of the 3D dynamic model show that there are priority and slow regions for fluid flow, and CO 2 mass transfer performance can be enhanced by concentrating the membrane fiber arrangement in the priority region. The model developed in this study can be used to evaluate defects in fluid flow patterns, such as channeling, back mixing, and tailing. Furthermore, the 3D steady-state and dynamic models can guide the design of membrane contactors, optimize operating conditions, and provide a reference for analyzing fluid flow morphology and structural optimization in membrane contactors.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Jinbo Song,Ting Qu,Jinpeng Zhang,Yanxin Jia,Jieying Jing,Wen-Ying Li
CaCO 3 -MgO sorbents were prepared through mechanochemical methods to overcome the poor stability of MgO sorbents caused by sintering and agglomeration. The alkali metal salt-promoted MgCa5 (AMS-MgCa5) sorbent, with 5 wt% CaCO 3 doping, demonstrated the highest cycling stability, with an initial CO 2 capture capacity of 13.9 mmol/g, which stabilized at 9 mmol/g after 10 cycles, and the CO 2 capture ratio reached 77 %. The superior cycling stability of the sorbents was attributed to the existence of CaMg(CO 3 ) 2 , which enhanced the capture rate during the CO 2 chemisorption process. Additionally, the doped CaCO 3 served as an inert support, enhancing CO 2 diffusion and mass transfer, ensuring the uniform coverage of alkali metal salt on the MgO surface, and inhibiting the growth of MgO particles.
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