ChemSusChem
·
2016
·Vol. 9
·期 17
·2351-2357
·
IF 7.116
Mingguang Pan,Ningning Cao,Wenjun Lin,Xiaoyan Luo,Kaihong Chen,Siying Che,Haoran Li,Congmin Wang
Graphical Dual-tuning method : Through the introduction of a large π-conjugated structure into the anion, a dual-tuning approach to improve CO 2 capture by anion-functionalized ionic liquids (ILs) results in high capacities of up to 0.96 ; and excellent reversibility. Quantum chemical calculations, spectroscopic investigations, and thermogravimetric analysis indicate that the increased capacity is a result of stronger dynamic covalent bonds. The strong chemisorption of CO 2 is always accompanied by a high absorption enthalpy, and traditional methods to reduce the absorption enthalpy lead to decreased CO 2 capacities. Through the introduction of a large π-conjugated structure into the anion, a dual-tuning approach for the improvement of CO 2 capture by anion-functionalized ionic liquids (ILs) resulted in a high capacity of up to 0.96 mol and excellent reversibility. The increased capacity and improved desorption were supported by quantum chemical calculations, spectroscopic investigations, and thermogravimetric analysis. The increased capacity may be a result of the strengthened dynamic covalent bonds in these π-electron-conjugated structures through anion aggregation upon the uptake of CO 2 , and the improved desorption originates from the charge dispersion of interaction sites through the large π-electron delocalization. These results provide important insights into effective strategies for CO 2 capture.
✓ 已验证
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2016
·Vol. 18
·期 12
·3567-3576
·
IF 8.506
Xu Jiang,Faliang Gou,Fengjuan Chen,Huanwang Jing
A series of innovative bisimidazole-functionalized porphyrin cobalt(III) complexes have been devised, synthesized and characterized using NMR, MS and elemental analysis. These homogeneous catalysts were applied to the cycloaddition of epoxides and carbon dioxide without organic solvent and co-catalyst. It was found that the performance of the catalysts deeply relies on their structural features. The alkoxyl chain length of the linkage and the imidazole position relative to the phenyl rings of porphyrin evidently affects the catalyst activities. [5,15-Di(3-((8-imidazolyloctyl)oxy)phenyl)porphyrin] cobalt(III) chloride (J-m8) and [5,15-di(2-((6-imidazolylhexyl)oxy)phenyl)porphyrin] cobalt(III) chloride (J-o6) demonstrated excellent activity under optimal reaction conditions. Synchronously, a preliminary kinetic investigation of this reaction was carried out using three catalysts and illustrated the activation energies of cyclic carbonate formation. Furthermore, a tri-synergistic catalytic mechanism has been carefully proposed in light of the features of the new catalysts and experimental results.
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2016
·
IF 4.764
Zhong Ying,Chao Zhang,Shan Jiang,Qifan Wu,Bin Zhang,Yancun Yu,Minli Lan,Haiyang Cheng,Fengyu Zhao
Carbon dioxide, as a carbonyl source to replace the highly toxic isocyanate, was used to prepare a new type of polyurea with amino modified polysiloxane in this work. The formation of both the modified polysiloxane and polyureas were confirmed by FT-IR spectra, 1 H NMR spectrum and 13 C NMR spectrum. The thermo-stability, solubility as well as the hydrophilicity was examined; the polysiloxane could be soluble in several polar solvents like acetone, THF, ethanol and so on. The polyureas are stable at temperature lower than 150 °C, and the synthesized polyureas are hydrophobic as they have a water contact angles larger than 90°. Moreover, the polyurea containing high urea linkage content presented excellent absorption for some organic solvents, such as C 2 H 3 Cl 3 , thus it is expected to have an application in removing organic pollutants on river.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2016
·
IF 7.145
Haiyang Zhang,Ruili Guo,Jinpeng Hou,Zhong Wei,Xueqin Li
In this study, a carbon nanotubes composite coated with N-isopropylacrylamide hydrogel (NIPAM-CNTs) was synthesized. Mixed-matrix membranes (MMMs) were fabricated by incorporating NIPAM-CNTs composite filler into poly(ether-block-amide) (Pebax MH 1657) matrix for efficient CO2 separation. The as-prepared NIPAM-CNTs composite filler mainly plays two roles: (i) The extraordinary smooth one-dimensional nanochannels of CNTs act as the highways to accelerate CO2 transport through membranes, increasing CO2 permeability; (ii) The NIPAM hydrogel layer coated on the outer walls of CNTs acts as the super water absorbent to increase water content of membranes, appealing both CO2 permeability and CO2/gas selectivity. MMM containing 5 wt % NIPAM-CNTs exhibited the highest CO2 permeability of 567 barrer, CO2/CH4 selectivity of 35, and CO2/N2 selectivity of 70, transcending 2008 Robeson upper bound line. The improved CO2 separation performance of MMMs is mainly attributed to the construction of the efficient CO2 transport pathways by NIPAM-CNTs. Thus, MMMs incorporated with NIPAM-CNTs composite filler can be used as an excellent membrane material for efficient CO2 separation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Mengli Li,Lingxia Zhang,Xiangqian Fan,Meiying Wu,Min Wang,Ruolin Cheng,Linlin Zhang,Heliang Yao,Jianlin Shi
We have synthesized a series of LaPO 4 /g-C 3 N 4 core-shell nanowires via an in-situ hydrothermal growth of LaPO 4 nanorods in tubular g-C 3 N 4 and investigated their photocatalytic activity in CO 2 reduction. It was found that in the synthesized core-shell structure, the outer g-C 3 N 4 nano-shells coated on the LaPO 4 nanorod cores resulted in the enhanced light absorption and charge carrier separation/transfer ability, thus improved the room temperature photocatalytic performance of the nanocomposites in CO 2 photocatalytic reduction compared with the g-C 3 N 4 and LaPO 4 individuals. A maximum CO yield of 0.433 μmol has been obtained from CO 2 reduction within 1 h irradiation on 30 mg nanocomposite photocatalyst under the absence of any noble metal. Finally, a possible mechanism, which is featured with LaPO 4 activation due to significantly promoted separation/transfer of photo-generated charge carriers, was proposed. The encouraging performance in CO 2 photoreduction demonstrates that this novel nanocomposite will be a prospective material in environmental protection and energy conversion.
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Jibo Liu,Huijie Shi,Xiaofeng Huang,Qi Shen,Guohua Zhao
Photo/electrochemical CO 2 reduction using pyridine was feasible to produce methanol via the formation of pyridiniumformate intermediate. To improve the reduction efficiency, a pyridyl bonded ruthenium (II)-based photosensitizer catalyst (Ru-Py) was designed for photoelectrochemical CO 2 conversion. The photocurrent density on Ru-Py modified electrode in CO 2 saturated solution was 0.103 mA cm −2 higher than that without illumination. The total Faradaic efficiency (f) reached 83.1%, whereas the turnover number (TON) for methanol was 38.4 in aqueous solution after 8 h irradiation. The methanol production was 24.1 μmol which was higher than the published literatures (less than 8 μmol) in similar systems could be attributed to the efficient electron transfer between the photosensitizer and the pyridyl active site covalently linked by C-C bond, as well as the strong and wide absorption up to 610 nm resulted from the large conjugated structure of the ligands. The mechanism investigation revealed that the N atom in pyridyl as catalytic active sites played significant role in CO 2 conversion by forming the pyridiniumformate intermediate which was confirmed by the simulation reaction. Meanwhile, in order to realize the reduction process intuitively, the density functional theory (DFT) was applied to simulate the structure of Ru-Py and the pyridiniumformate intermediates.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Yebin Guan,Juanjuan Shi,Ming Xia,Jun Zhang,Zhenfeng Pang,Alessandro Marchetti,Xiaohong Wang,Jingsong Cai,Xueqian Kong
Monodispersed zeolitic imidazolate frameworks (ZIFs) were prepared with a simple method using dimethylsulfoxide (DMSO) as solvent. This method yields ZIF-8 nanoparticles with a narrow particle size distribution of 90–110 nm and the dispersion is highly stable against agglomeration. These particles have larger nanosized porosity and enhanced CO 2 adsorption capability compared to ZIF-8 prepared with different solvents such as methanol or N , N -dimethyl formamide. Their uniform size and surface chemistry also lead to superior performance in the Knoevenagel condensation reactions. The ZIF-8 nanoparticles possess high thermal stability up to 550 °C and the preparation steps are easy for scaling up which are favorable for industrial applications.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2013
·
IF 4.093
Jun Shi,Jin Shi,Chao Du,Qun Chen,Shaokui Cao
Alginate/CaCO 3 hybrid membranes with pH- and thermal-responsive drug release properties were prepared under compressed CO 2 using polyacrylic acid (PAA) as a crystal growth additive. Aliphatic poly(urethane-amine) (PUA) was employed as the thermal-responsive composition in the hybrid membranes. The hybrid membranes were characterized by scanning electron microscopy, energy dispersive X-ray spectrometer, X-ray diffraction and thermogravimetric analyzer. The interaction between PAA and aliphatic PUA contributed the formation of compact CaCO 3 microparticles and the high drug loading efficiency of the hybrid membranes. By adjusting the pressure and reaction time of the biomineralization process, sustained drug release property could be achieved from the hybrid membranes. The results indicated that the compact CaCO 3 microparticles could hinder the permeability of the encapsulated drug and reduce the drug release effectively. Moreover, the thermal-sensitivity of aliphatic PUA and pH-sensitivity of alginate matrix would preserve after the biomineralization process.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2014
·
IF 0
Yong Xie,Rui-Xia Yang,Nian-Yu Huang,Hua-Jun Luo,Wei-Qiao Deng
We reported a bifunctional material, Cr-salen implanted conjugated microporous polymer (Cr-CMP), which is able to capture excellent CO 2 amounts and has a remarkable catalytic activity towards the cycloaddition reaction of CO 2 to epoxides forming cyclic carbonates at mild conditions without additional solvents. This heterogeneous Cr-CMP catalyst has a superior catalytic activity to its related homogeneous catalyst and can be reused more than ten times without a significant decrease in catalytic activity.
✓ 已验证
产品关联
DOI
RSC Advances
·
2014
·Vol. 4
·期 52
·27176-27183
·
IF 3.708
Qinghua Wu,Shuixia Chen,Hui Liu
A high amino density of grafted solid amine adsorption fiber (PP-AM-PEI) for CO2 adsorption was prepared by grafting acrylamide (AM) onto the surface of a polypropylene (PP) fiber and subsequently modified with polyethylenimine (PEI). The grafting of AM on PP fibers was beneficial for introducing and assembling PEI onto the fibers. An examination by infrared and scanning electron microscopies confirmed that AM and PEI were successfully introduced onto the surface of PP fiber. PP-AM-PEI showed good thermo-stability, a high adsorption capacity for CO2 (5.91 mmol g−1). It also has good regeneration performance and could maintain almost the same adsorption capacity for CO2 after 5 recycle numbers. In addition, two other polypropylene-based adsorbents, PP-GMA-PEI (using glycidyl methacrylate (GMA) as the active monomer) and PP-AM-EDA (using ethylenediamine (EDA) as the functional monomer) were prepared. Compared with PP-GMA-EDA, PP-AM-PEI was more suitable for CO2 capture in the presence of moisture due to its hydrophilicity. The results also showed that the adsorption capacity of PP-AM-PEI was superior to PP-AM-EDA due to the high amino density of PEI.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
·
2014
·Vol. 32
·期 12
·1628-1638
·
IF 1.42
Xiang Yan-hui,Liu Fu,Xue Li-xin,Shen Jian-hui,Lin Hai-bo
A supercritical carbon dioxide (ScCO 2 ) assisted phase inversion was developed to produce microporous poly(vinylidene fluoride) (PVDF) membranes whose morphology characteristics arise from both liquid-liquid demixing and solid-liquid demixing (crystallization). This result was confirmed by Fourier transform infrared spectroscopy (FTIR), from which both α and β crystals were found. As revealed by contact angle experiment, the PVDF membranes prepared via ScCO 2 assisted phase inversion were more hydrophobic compared with the control membrane produced via conventional immersion-precipitation technique. In particular, the sample with 15 wt% PVDF prepared at 45 °C and 13 MPa exhibited a contact angle of 142°, which was mainly caused by the multilevel micro- and nano-structure. The effects of polyethylene glycol (PEG), polyvinyl pyrrolidone (PVP) and lithium chloride (LiCl) on the structures and crystal form were investigated. PVP promoted the formation of α phase crystal form, while PEG boosts the evolution of β phase. LiCl restrained the crystallization degree of PVDF membrane under ScCO 2 .
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2014
·Vol. 60
·期 12
·4232-4240
·
IF 2.581
Kuan Huang,Xiao-Min Zhang,Yun Xu,You-Ting Wu,Xing-Bang Hu,Yun Xu
The solubilities of H 2 S and CO 2 in four protic ionic liquids (PILs)—methyldiethanolammonium acetate, methyldiethanolammonium formate, dimethylethanolammonium acetate, and dimethylethanolammonium formate were determined at 303.2–333.2 K and 0–1.2 bar. It is shown PILs have higher absorption capacity for H 2 S than normal ionic liquids (ILs) and the Henry's law constants of H 2 S in PILs (3.5–11.5 bar at 303.2 K) are much lower than those in normal ILs. In contrast, the solubility of CO 2 in PILs is found to be a magnitude lower than that of H 2 S, implying these PILs have both higher absorption capacity for H 2 S and higher ideal selectivity of H 2 S/CO 2 (8.9–19.5 at 303.2 K) in comparison with normal ILs. The behavior of H 2 S and CO 2 absorption in PILs is further demonstrated based on thermodynamic analysis. The results illustrate that PILs are a kind of promising absorbents for the selective separation of H 2 S/CO 2 and believed to have potential use in gas sweetening. © 2014 American Institute of Chemical Engineers AIChE J 60: 4232–4240, 2014
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）