JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2020
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IF 2.369
Yun Li,Yanhong You,Meng Dai,Xiaohui Chen,Jie Yang
The mixtures of propylene carbonate (PC) (1) + poly(propylene glycol) monobutyl ether with a molecular weight of 340 (PPGME340) (2) were studied as physical absorbents for CO2 absorption with different mass fractions (w1 = 0.0000, 0.2501, 0.5002, 0.7495, and 1.0000). The physical properties including densities and kinematic viscosities of these absorbents were determined and regressed by linear equation and Vogel–Fulcher–Tammann equation. CO2 absorption capacities of the absorbents under pressures up to 1300 kPa and at temperatures from 298.15 to 303.15 K were determined by the isothermal synthesis device and fitted by the extended Antoine equation. Adding PC into PPGME340 will result in a slight increase of density, dramatic decrease of kinematic viscosity, and moderate decrease of CO2 absorption capacity based on per mole absorbent. Compared with common solvents in industrial plants, PPGME340-contained absorbents show relatively high absorption capacity and kinematic viscosity. In addition, absorbent PC + PPGME340 with a mass fraction of w1 = 0.2501 shows relatively high CO2 absorption capacity and moderate kinematic viscosity, suggesting its better potential for the industrial application than pure PPGME340.
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International Journal of Greenhouse Gas Control
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2018
·
IF 4.078
Yanru Chen,Wusan Jiang,Xiao Luo,Yangqiang Huang,Bo Jin,Hongxia Gao,Wensheng Li,Zhiwu Liang
In this work, the stopped-flow technique is used to determine the kinetics data in terms of pseudo first-order rate constants ( k 0 ) for the homogenous reaction of CO 2 into aqueous solutions of 3-dimethylaminopropylamine (DMAPA) and 3-diethylaminopropylamine (DEAPA) as amine concentrations ranged from 0.05 kmol/m 3 to 0.15 kmol/m 3 and temperature ranged from 293 K to 313 K. It is found that k 0 increased with increasing temperature and with increasing amine concentration. The mechanism of the pseudo first-order chemical reaction hypothesis is applied to interpret the experimental data. The Arrhenius expressions as k 2 = 8.69 × 10 9 × exp ( − 4226.2 / T ) for DMAPA and k 2 = 7.21 × 10 12 × exp ( − 6162.9 / T ) for DEAPA are obtained. The results show that the experimental CO 2 absorption rates exhibited good agreement with predicted CO 2 absorption rates with an average relative deviation (ARD) of 2.34% and 7.53%, respectively. Finally, the interaction of tertiary amine groups with primary amine groups and the effect of molecular structure on the interaction are discussed by comparing the CO 2 absorption and desorption performances in five different systems (MEA, DEEA, MEA + DEEA, DMAPA, DEAPA). It is found that the intermolecular interaction of amino groups is stronger than that of intramolecular interaction.
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Environmental Progress & Sustainable Energy
·
2018
·Vol. 37
·期 6
·2026-2033
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IF 1.326
Ke Wang,Ji Sun,Pengfei Zhao
The development of novel Li 4 SiO 4 -based sorbents is hampered by a lack of understanding of the mechanisms governing CO 2 adsorption on the Li 4 SiO 4 surface. In this work, the adsorption of CO 2 and flue gas components (such as H 2 O and SO X (SO 2 and SO 3 )) on a simulated Li 4 SiO 4 surface was investigated using ab initio-based energetic calculations. The Li 4 SiO 4 surface was modeled by a cluster of lithium silicate, in which the atoms were unsaturated to simulate the active sites. Furthermore, Fourier transform infrared (FTIR) spectra were also analyzed. The calculated results showed that three possible configurations were determined: CO 2 weakly sorbed on the oxygen sites of Li 4 SiO 4 through physisorption; a carbonate species appeared, which was characterized by chemisorption; and a linear cluster of Li + -O = C=O formed, having the largest sorption energy. These three possible pathways were likewise in accordance with the FTIR results. Moreover, a pre-chemisorption of water on Li 4 SiO 4 resulted in promoted CO 2 capture, while the presence of competitive SO X sorption on the same active sites as CO 2 sorption showed an inhibition effect. The results clarify the complex adsorption mechanisms on the Li 4 SiO 4 surface. © 2018 American Institute of Chemical Engineers Environ Prog, 37: 1901–1907, 2018
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 7
·2300-2307
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IF 4.052
Xiao-Yan Luo,Xiao-Yan Chen,Rong-Xing Qiu,Bao-You Pei,Yi Wei,Min Hu,Jin-Qing Lin,Jing-Yang Zhang,Geng-Geng Luo
In this work, an efficient strategy for improving CO2 capture based on anion-functionalized ionic liquids (ILs) by reducing cation–anion interactions in ILs was reported. The influence of the cationic species on CO2 absorption was investigated using 2-hydroxyl pyridium anions ([2-Op]) as a probe. CO2 capture experiments indicated that the CO2 absorption capacity in [2-Op] anion-based ILs varied from 0.94 to 1.69 mol CO2 per mol IL at 30 °C and 1 atm. Spectroscopic analysis and quantum chemical calculations suggested that the increase of the CO2 absorption capacity may be ascribed to the reduction of the strength of cation–anion interactions in ILs, and stronger cation–anion interactions would make one CO2 site in the [2-Op] anion inactive. Furthermore, the effect of the cation unit on the anion was evidenced by FT-IR spectra, implying that strong interactions between ions may lead to the decrease of the IR absorption wavenumber of hydroxy pyridium and work against CO2 capture. Following this strategy, it was finally found that [Ph-C8eim][2-Op] (Ph-C8eim = 1-N-ethyl-3-N-octyl-2-phenylimidazolium) with weaker cation–anion interactions exhibited a significant increase in the CO2 uptake capacity, and extremely high capacities of 1.69 and 1.83 mol CO2 per mol IL could be achieved at 30 and 20 °C, respectively. The study presented here would be helpful for further designing novel and effective ILs for advancing CO2 capturing performance.
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PubMed
高影响因子
Analytical Methods
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2018
·Vol. 10
·期 25
·2989-2993
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IF 2.073
Bingyan Han,Ying Li,Tingting Peng,Mingbo Yu,Xixi Hu,Gaohong He
In this paper, polyethyleneimine (PEI) was applied as a carbon source for synthesizing fluorescent carbon dots (CDs) through a facile and one-step hydrothermal route. Both the N-doping and the amino-functionalization of CDs were accomplished simultaneously. The CDs exhibited strong blue fluorescence and good dispersion in aqueous solution. A large number of amino groups on the surface of CDs greatly simplified the subsequent modification steps. Through an amide reaction, glutathione-functionalized CDs were successfully applied to the selective detection of Co2+, in the linear range from 2.0 × 10−5 to 1.0 × 10−4 mol L−1.
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Nano Research
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2018
·Vol. 11
·期 5
·2450-2459
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IF 7.994
Zhang Bing,Zhao Tian-Jian,Feng Wei-Jie,Liu Yong-Xing,Wang Hong-Hui,Su Hui,Lv Li-Bing,Li Xin-Hao,Chen Jie-Sheng
The greenhouse effect and global warming are serious problems because the increasing global demand for fossil fuels has led to a rapid rise in greenhouse gas exhaust emissions in the atmosphere and disruptive changes in climate. As a major contributor, CO 2 has attracted much attention from scientists, who have attempted to convert it into useful products by electrochemical or photoelectrochemical reduction methods. Facile design of efficient but inexpensive and abundant catalysts to convert CO 2 into fuels or valuable chemical products is essential for materials chemistry and catalysis in addressing global climate change as well as the energy crisis. Herein, we show that two-dimensional fewlayer graphitic carbon nitride (g-C 3 N 4 ) can function as an efficient metal-free electrocatalyst for selective reduction of CO 2 to CO at low overpotentials with a high Faradaic efficiency of ~ 80%. The polarized surface of ultrathin g-C 3 N 4 layers (thickness: ~ 1 nm), with a more reductive conduction band, yields excellent electrochemical activity for CO 2 reduction.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Dongxing Tan,Jianling Zhang,Jinbiao Shi,Shaopeng Li,Bingxing Zhang,Xiuniang Tan,Fanyu Zhang,Lifei Liu,Dan Shao,Buxing Han
To develop photocatalysts with desirable compositions and structures for improving the efficiency and selectivity of CO2 conversion to CH4 under mild conditions is of great importance. Here, we design an effective photocatalyst of bimetal (Ag/Pd) nanoalloys supported on nitrogen-doped TiO2 nanosheet for CO2 conversion. Such a novel photocatalyst combines multiple advantages of abundant Ti3+ ions, oxygen vacancies, and substitutional nitrogen that are favorable for catalyzing CO2 reduction. It was found that CO2 could be efficiently transformed to CH4 under mild conditions, i.e., in aqueous solution and at atmospheric pressure and room temperature. The maximum production rate of CH4 can reach 79.0 μmol g–1 h–1. Moreover, the Ag/Pd bimetals supported on N-doped TiO2 nanosheet exhibit high selectivity to CH4. The as-synthesized photocatalyst can be well recycled for CO2 reduction.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2018
·Vol. 42
·期 15
·13054-13064
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IF 3.201
Qingwen Gu,Jian Fang,Zichen Xu,Wenxiu Ni,Kang Kong,Zhenshan Hou
1,8-Diazabicyclo[5.4.0]undec-7-ene (DBU) is an effective nucleophilic catalyst for the transesterification of dimethyl carbonate (DMC) with various alcohols and amines, which afforded unsymmetrical organic carbonate and carbamate. It was observed that the transesterification was accelerated under pressurized CO2 in this work. The activity is very high and the best result (89% conversion with 98% selectivity to unsymmetrical carbonate) was obtained for the DBU/alcohol/DMC/CO2 system. The addition of CO2 to DBU/ethanol generated the DBU cation salt, [DBUH][OCOOCH2CH3], which dissociated more favorably under increasing reaction temperature even under pressurized CO2. The salt could also help to activate DMC by H-bond interaction. The reaction system can be extended easily for the catalytic synthesis of carbamates from amines and DMC. After the reaction, the salt was separated from the reaction mixture and DBU can be recovered by the feasible thermal decomposition, offering a straightforward strategy for the recycling of DBU. On the basis of these results, a plausible mechanism involving the role of both DBU and CO2 has been proposed.
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Journal of CO2 Utilization
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2018
·
IF 5.503
Keng Xuan,Yanfeng Pu,Feng Li,Aixue Li,Jing Luo,Lei Li,Feng Wang,Ning Zhao,Fukui Xiao
A series of trifluoroacetic acid (TFA) modulated metal-organic frameworks UiO-66 catalysts were synthesized for the direct synthesis of dimethyl carbonate (DMC) from CO 2 and methanol in this work. Characterization results show that the surface area, pore size, pore volume as well as the amount of missing-linker defects, Lewis acid site, Lewis basic site and hydroxyl of UiO-66-X can be tuned by regulating the amount of TFA modulator. Catalytic activity assessments reveal that TFA modulation enhanced the activity of UiO-66-X. The catalytic activity improvement of the UiO-66-X could be attributed to the increased amount of active sites and the enlargement of porosity originated from TFA modulation. Moreover, a possible reaction mechanism for DMC synthesis from CO 2 and methanol over UiO-66-X was proposed based on the in situ FT-IR results.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Yunzhe Jiang,Chuanyao Liu,Jürgen Caro,Aisheng Huang
A new UiO-66-NH 2 based MOF named UiO-66-NH 2 @ICA has been prepared by grafting imidazole-2-carbaldehyde (ICA) to UiO-66-NH 2 through a post-synthesis reaction via amine condensation. FESEM , XRD , 1 H NMR, FT-IR and N 2 adsorption were used to characterize the morphology and structure of UiO-66-NH 2 @ICA. The grafted ICA mainly reduces the pore volume of UiO-66-NH 2 but increases the number of nitrogen atom as binding site of CO 2 . The UiO-66-NH 2 @ICA showed less BET surface area but a higher CO 2 /CH 4 adsorption selectivity in comparison with UiO-66-NH 2 . UiO-66-NH 2 @ICA and UiO-66-NH 2 crystals were dispersed in Matrimid ® 5218 to form mixed-matrix membranes (MMMs). Single gas permeation and mixed gas separation was carried out to investigate the effects of filler loading and feed gas pressure on the separation performances of the MMMs. The UiO-66-NH 2 @ICA/Matrimid ® MMM with 10 wt % filler showed a high CO 2 /CH 4 selectivity with a separation factor of 64.7, which is an increase by 40% in comparison with UiO-66-NH 2 /Matrimid ® MMM.
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JOURNAL OF MOLECULAR LIQUIDS
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2018
·
IF 4.513
Mingwei Zhao,Haonan He,Caili Dai,Xuepeng Wu,Yue Zhang,Yongping Huang,Chenglin Gu
This study presents the synthesis of a CO 2 -responsive surfactant namely 2‑alkyl‑1‑hydroxyethyl imidazoline (HEA n IBs n = 16, 18, 20), which exhibits satisfactory surface and adsorption properties. The micelle formation and adsorption of the above imidazoline based surfactant in aqueous solution were studied in this work. CMC , the effectiveness of surface tension reduction, the maximum surface excess concentration, the minimum area occupied per surfactant molecule at the air/water interface, and the micelle aggregation number were obtained by measuring surface tension. Dynamic light scattering indicates that when the surfactant concentration is 1.2 times the CMC, the hydrodynamic radii of the three surfactants studied were almost equal to 8 nm. Electrical conductivity measurements indicate the micellization of surfactants in aqueous solution. In addition, typical thermodynamic parameters, including Δ G m 0 , Δ G ads 0 , Δ H m 0 , Δ S m 0 , Δ H m A , Δ S m A , and Δ C p, m 0 were evaluated. The thermodynamic parameters show that micelle formation is entropy-and-enthalpy co-driven from 298 K to 318 K. We expect to elucidate the self-assembly of CO 2 -responsive surfactant in an aqueous solution.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Yunpeng Zhou,Yangqiang Huang,Bo Jin,Xiao Luo,Zhiwu Liang
Pd nanoclusters supported on Schiff base modifying graphitic carbon nitride (Pd/u-CN100) had been successfully synthesized using urea and terephthalaldehyde as precursors by an impregnation approach. The resulting sheet materials exhibited high catalytic activity that turnover frequency rose to 98.9 h–1 and stability in CO2 hydrogenation. Various factors affecting formate production including the addition amount of TPAL, reaction pressure, reaction temperature, and catalyst stability testing were studied to achieve favorable catalytic conversion. An amount of characterization methods were applied to investigate the structure–activity relationship, including TEM, XRD, XPS, FTIR, HETEM, EDS, and BET. The high activity and stability might be resulted from the electronic modification, the relatively high dispersion of noble metal nanoclusters and the formation of intensely anchored metal-carrier bonds. More concretely, the scattered Schiff base loci and multiple nitrogen species were of great significance in the efficient and durable CO2 hydrogenation system.
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