ACS Sustainable Chemistry & Engineering
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2019
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IF 6.97
Xiaomin Zhang,Wenjie Xiong,Zhuoheng Tu,Lingling Peng,Youting Wu,Xingbang Hu
Selective separation of CO2 from flue gas conforms to the criterion of sustainable society. Herein, a series of imidazolium-based phenolate ionic liquids (ILs) that have dual-site interaction centers to isolate CO2 from N2 by supported ionic liquid membranes (SILMs) is designed and prepared. Density, viscosity, and CO2 solubility in these ILs were measured. The effects of the electron-withdrawing or electron-donating ability of the substituents on the anion, the operation temperature and partial pressure on the permeability of CO2, and the ideal selectivity of CO2/N2 were investigated systematically. High permeability (up to 2540 barrers) and selectivity of CO2/N2 (up to 127) are achieved in 1-butyl-3-methylimidazolium phenolate ([bmim][PhO]) containing 15 wt % H2O under humidified condition. A novel facilitated transport mechanism, transfer of CO2 from carbene to phenolated anion, is proposed based on NMR, FT-IR, and theoretical calculation results. The new pathway is believed to offer an alternative opportunity for designing novel CO2 separation materials.
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Journal of the Taiwan Institute of Chemical Engineers
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2019
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IF 3.834
Jingru Guan,Huiqin Wang,Jinze Li,Changchang Ma,Pengwei Huo
A series of novel porous indium (III) oxide (In 2 O 3 ) and nanocubic cerium oxide (CeO 2 ) loading HCl treated attapulgite (HATP) ternary photocatalysts were successfully synthesized. Simultaneously, all photocatalysts were performed the CO 2 reduction under UV-light. To explore the crystal structures, morphologies and electrochemical characteristics of as-synthesized samples, the XRD, SEM and TEM, and transient photocurrent techniques were performed in this work. Besides, as an optimized In 2 O 3 /CeO 2 /HATP sample presents the highest activity for CO (32.03 µmol/g) and CH 4 (16.94 µmol/g) yields, which is 6.11-fold and 6.78-fold times higher than those of pure CeO 2 under UV-light (8 W) irradiation.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2019
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IF 2.298
Siqi Wang,Lishu Shao,Yafei Sang,Jianhan Huang
Herein, we prepared a series of hollow hyper-cross-linked polymer (HCP) microspheres with a hollow core–shell structure via the hard-template method, and the as-prepared HCPs were employed for rhodamine B (RB) adsorption and CO2 capture. The results indicate that the porosity of the HCPs can be easily tuned and the hollow microspheres are favorable for the fast mass transfer of RB in the pore channels; accordingly, the adsorption equilibrium can be attained quickly. In addition, the hollow microspheres are helpful for increasing the equilibrium capacity. The RB adsorption shows that HCPs-5% holds the best capacity (1400 mg/g) and acceptable equilibrium time (60 min). On the other hand, the CO2 adsorption exhibits that HCPs-5% holds the highest CO2 uptake (99.0 mg/g) and the ultramicropores play important roles in the adsorption. The HCPs hold moderate isosteric heat of CO2 adsorption (24.4–35.0 kJ/mol) and exhibit excellent recycling performance.
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APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Jiaojiao Tan,Jiaming Wang,Ziyang Zhang,Zhi Ma,Luhui Wang,Yuan Liu
To improve the catalytic activity of CO 2 methanation at low temperature, a series of Ni/ZrO 2 catalysts with different Ni loadings were prepared by citrate complexing method. Based on the optimal Ni loading of 6 wt%, a certain amount of MgO was doped to improve the thermal stability of Ni/ZrO 2 catalyst. When Ni/Mg molar ratio was 4, there was the best performance, getting as high as 90% CO 2 conversion and nearly 100% CH 4 selectivity at 250 °C, 0.1 MPa and a WHSV of 15,000 ml g −1 h −1 , and the equilibrium CO 2 conversion was obtained at 300 °C. XRD , BET, TPR, CO 2 -TPD, H 2 -TPD, XPS , TG and TEM were conducted to investigate the reason of high activity of Ni/ZrO 2 catalyst at low temperature and the effect of doping MgO. Results suggested that highly dispersed Ni nanoparticles are responsible for the excellent catalytic activity. MgO can effectively improve stability of Ni-based catalysts by the confinement effect. Meanwhile, it is also found that there are little improvements on catalytic activity after doping MgO, and the TOF of catalysts with different MgO doping is basically the same, indicating CO 2 can be efficiently adsorbed and activated on the monoclinic ZrO 2 , and MgO do not contribute to the intrinsic activity.
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FUEL
·
2019
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IF 5.128
Yannan Li,Jun Cheng,Leiqing Hu,Niu Liu,Junhu Zhou,Kefa Cen
To study the relationship between crystal structures of amine-carbamates and regeneration energy consumptions, two new solid–liquid phase-changing solutions of ethylenediamine/N,N-dimethylacetamide (EDA/DMA) and ethylenediamine/N,N-dimethylformamide (EDA/DMF) were prepared to capture CO 2 efficiently and regulate the crystal structures of CO 2 absorption products (EDA-carbamates). The CO 2 absorption capacity and peak absorption rate of EDA/DMA and EDA/DMF solutions were both 30% and 67%, respectively, higher than those of EDA/water solution. EDA-carbamates in EDA/DMA and EDA/DMF solutions had the same molecular structures but different molecular arrangements (they belonged to orthorhombic and monoclinic crystals, respectively). The regeneration heat of EDA-carbamates in EDA/DMF solution (181.28 kJ/mol) was higher than orthorhombic EDA-carbamates in EDA/DMA solution (133.76 kJ/mol), which was attributed to the endothermic process (recrystallization process) during the transition from monoclinic EDA-carbamates to orthorhombic EDA-carbamates.
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Greenhouse Gases-Science and Technology
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2019
·Vol. 10
·期 2
·461-471
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IF 1.693
Xue-Fei Wang,Long Xiong,Li Li,Jun-Jun Zhong
Porous carbon fibers (PCFs) were prepared from porous polyacrylonitrile fibers by cross-linking, oxidation, and carbonization. X-ray diffraction patterns revealed that graphite structures as well as disordered carbon coexisted in the PCFs. Nitrogen content was more than 15.3 wt% with the variation of oxidation temperature, and a maximum value was obtained at 275°C. Nitrogen was quickly released with carbonization temperature. Compared with the fiber prepared at elevated carbonization temperatures, those owning high nitrogen contents deserved better carbon dioxide (CO 2 ) adsorption performance in the simulated flue gas environment (10% CO 2 /90% N 2 ). The CO 2 adsorption had a better relationship with nitrogen content rather than specific surface area and pore volumes. Especially, nitrogen was very useful to enhance the CO 2 adsorption of the fibers with low microporosity. The heat of CO 2 adsorption was in the range of 39.8–54.6 kJ mol −1 , which indicated good selectivity of CO 2 adsorption. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd.
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ACS Catalysis
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2019
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IF 12.221
Jian Li,Yaping Lin,Xiulian Pan,Dengyun Miao,Ding Ding,Yi Cui,Jinhu Dong,Xinhe Bao
Strong metal–support interaction (SMSI) has been widely recognized for platinum-group metals on reducible oxide supports. Herein we report that the catalytic activity of Ni catalyst in CO2 methanation is significantly suppressed over conventional anatase (a-TiO2) support due to the SMSI-induced formation of a titania overlayer around the Ni nanoparticles. Furthermore, CO is the only product . In contrast, the NH3-treatment and H2-treatment of the a-TiO2 support enhance remarkably the activity of Ni, i.e., CO2 conversion increases by 1 order of magnitude and CO2 is hydrogenated almost exclusively to CH4. X-ray photoelectron spectroscopy (XPS), H2 and CO chemisorption, and low temperature electron paramagnetic resonance (EPR) reveal that the enhanced CO2 methanation activity may be related with the Ti3+ species in the bulk that are generated by reduction treatment, which likely have altered the SMSI between Ni and a-TiO2 support. This simple reduction treatment approach may be applicable to modulate the SMSI of other reducible oxide-supported metal catalysts.
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Polymers
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2019
·Vol. 11
·期 6
·985
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IF 3.164
Yidong Liu,Lingfeng Jian,Tianhua Xiao,Rongtao Liu,Shun Yi,Shiyang Zhang,Lingzhi Wang,Ruibin Wang,Yonggang Min
CO2has been regarded as one of the most promising blowing agents for polystyrene (PS) foam due to its non-flammability, low price, nontoxicity, and eco-friendliness. However, the low solubility and fast diffusivity of CO2in PS hinder its potential applications. In this study, an attapulgite (ATP)/polypyrrole (PPy) nanocomposite was developed using the in situ polymerization method to generate the hierarchical cell texture for the PS foam based on the supercritical CO2foaming. The results demonstrated that the nanocomposite could act as an efficient CO2capturer enabling the random release of it during the foaming process. In contrast to the pure PS foam, the ATP/PPy nanocomposite reinforced PS foam is endowed with high cell density (up to 1.9 × 106) and similar thermal conductivity as the neat PS foam, as well as high compression modulus. Therefore, the in situ polymerized ATP/PPy nanocomposite makes supercritical CO2foaming desired candidate to replace the widely used fluorocarbons and chlorofluorocarbons as PS blowing agents.Keywords:supercritical CO2;polystyrene foam;blowing agent;in situ polymerization;attapulgite/polypyrrole nanocomposite
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PubMed
高影响因子
ELECTROCHIMICA ACTA
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2019
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IF 5.383
Yunfei Chen,Mingyong Wang,Songle Lu,Jiguo Tu,Shuqiang Jiao
s Electrochemical conversion of CO 2 to carbon in molten salts is a promising route for the high-value utilization of greenhouse gases . Low graphitization degree of carbon materials is the limiting issue for potential applications. In the past, catalytic effect for the electrochemical conversion of CO 2 was not achieved in molten salts due to carbon coverage on heterogeneous solid electrode. A novel and feasible homogeneous catalytic strategy by soluble NaVO 3 in carbonate molten salt was proposed for the enhanced electrochemical conversion of CO 2 to carbon with high graphitization degree. It was found that graphite consisting of carbon nanotubes and sheets were more easily produced by adding NaVO 3 into molten salt. The graphitization degree of carbon products was obviously improved and I D / I G value was only 0.428. During CO 2 electrolysis, vanadate in the form of V 2 O 7 4− will be co-electroreduced to V 2 O 3 . Meanwhile, V 2 O 7 4− ions can be regenerated by the spontaneous reaction between the newly-formed V 2 O 3 and carbonate, which also accelerates the production of graphite. Therefore, a continuous homogeneous in-situ catalytic cycle was achieved for the enhanced graphitization conversion of CO 2 . It provides a novel and effective way to prepare carbon materials with high graphitization degree from CO 2 .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Meng Yuan,Ge Gao,Xiayi Hu,Xiao Luo,Yangqiang Huang,Bo Jin,Zhiwu Liang
In this work, industrial grade sepiolite (IG-SEP) was premodified with hydrochloric acid, and then premodified sepiolite (SEP) was impregnated with triethylenetetramine (TETA) to create a novel TETA functionalized SEP adsorbent. The effects of TETA loading and adsorption temperature on CO2 adsorption capacity, as well as the CO2 adsorption isotherm and cyclic regenerability were investigated. Results show that, when SEP was optimized at 30 wt % TETA (SEP-TETA-30%), the adsorbent attained a CO2 adsorption capacity as high as 1.93 mmol/g at 50 °C with fast adsorption kinetics and good regenerability. The Freundlich model was best able to fit the experimental adsorption isotherm, and the isosteric heat of adsorption at high CO2 coverage was 28 kJ/mol. The presence of moisture in simulated gas has a positive effect on the adsorption capacity, with less harm to adsorption stability. The adsorbent samples were further characterized by N2 adsorption/desorption, scanning electron microscope, X-ray diffraction, Fourier transform infrared spectroscopy, and thermogravimetric analysis. The increased surface area and pore volume of the SEP allow for effective immobilization of TETA within its channels. A kinetic study demonstrated that the experimental adsorption data for SEP-TETA-30% were well fitted by the pseudo-second-order model. More importantly, an index of cost efficiency was proposed to evaluate the practicability and competitiveness of amine-impregnated adsorbents. The cost efficiency of SEP-TETA-30% adsorbent was estimated as 0.19 mol CO2/$, which was higher than reported adsorbents, suggesting that the TETA functionalized SEP (SEP-TETA-30%) composite is a promising adsorbent for cyclic postcombustion CO2 capture processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2018
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IF 3.927
Wenji Zheng,Rui Ding,Kai Yang,Yan Dai,Xiaoming Yan,Gaohong He
Poly (ether- block -amide) (Pebax) based mixed matrix membranes (MMMs) were prepared by using size-tunable ZIF-8 nanoparticles as fillers. ZIF-8 nanoparticles with sizes of 40, 60, 90 and 110 nm (ZIF-8-40, ZIF-8-60, ZIF-8-90 and ZIF-8-110) were synthesized in microemulsion by controlling the ratio of Zn 2+ to Hmim (1:16, 1:8, 1:5, 1:2). And they were distributed uniformly in Pebax matrix without obvious agglomerations and defects at the loading of 0–20 wt.%, which was confirmed by field-emission scanning electron microscopy (FE-SEM). The incorporation of ZIF-8 resulted in a significant improvement in CO 2 permeability and the CO 2 /N 2 selectivity increased with the BET surface area of ZIF-8 increasing. The enhanced permeability is attributed to an improvement in the free volume of the polymer induced by larger sized ZIF-8, while the increased selectivity results from the high specific surface area of large sized ZIF-8, which can provide more active sites for CO 2 capture and great mass transfer resistance for N 2 . At 5 wt.% loading of ZIF-8-90, the MMM presents the best separation performance with CO 2 permeability of 99.7 Barrer and CO 2 /N 2 selectivity of 59.6, both of which are increased by about 25% by comparison to the pure Pebax membrane. The present study provides an effective way to obtain size-controlled ZIF-8 fillers and high separation performances of Pebax based MMMs.
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Catalysts
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2018
·Vol. 8
·期 5
·215
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IF 3.465
Tongyao Wang,Ming Xia,Xueqian Kong
Photocatalytic reduction of CO2into fuels is a promising route to reduce greenhouse gas emission, and it demands high-performance photocatalysts that can use visible light in the solar spectrum. Due to its broadband light adsorption, polydopamine (PDA) is considered as a promising photo-sensitization material for semiconductor photocatalysts. In this work, titanium oxides have been coated with PDA through an in-situ oxidation polymerization method to pursue CO2reduction under visible light. We have shown that the surface coated PDA with a thickness of around 1 nm can enhance the photocatalytic performance of anatase under visible light to reduce CO2into CO. Assisted with additional UV-vis adsorption and photoluminescence characterizations, we confirmed the sensitization effect of PDA on anatase. Furthermore, our study shows that thicker PDA coating might not be favorable, as PDA could decompose under both visible and UV-vis light irradiations.13C solid-state nuclear magnetic resonance showed structural differences between thin and thick PDA coatings and revealed compositional changes of PDA after light irradiation.Keywords:photocatalysis;CO2reduction;anatase;polydopamine;sensitization
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