IONICS
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2018
·Vol. 25
·期 4
·1921-1927
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IF 2.347
Shen Feng-xia,Shi Jin,Shi Feng,Chen Tian-you,Li Yun-fei,Li Qing-yuan,Dai Yong-nian,Yang Bin,Qu Tao
Electro-reduction of carbon dioxide (CO 2 ) to carbon monoxide (CO) has been extensively studied on metal and alloy electrodes for many decades. However, owing to their disadvantages of low current density and high over-potential, the practical application of these electrodes has been limited. Hence, it is highly desirable to explore new and high efficient electrode for CO 2 reduction to CO. Ag 2 S has been widely studied as electrode material in electrochemistry due to its unique properties, such as high conductivity, chemical stability, and easy to be prepared. In this work, we have fabricated an Ag 2 S electrode via electro-oxidation of Ag in aqueous solution. X-ray diffraction (XRD) and scanning electron microscope (SEM) confirm that Ag 2 S has been modified on Ag foil, which made the electrode surface roughness. And then, we have evaluated the performance of Ag 2 S electrode as the cathode for CO 2 reduction in propylene carbonate/tetrabutylammonium perchlorate. The cathodic current density reaches to 9.85 mA/cm 2 , with the faradic efficiency for CO formation remaining stable at 92% during 4 h long-term electrolysis.
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Nanoscale
·
2015
·Vol. 8
·期 2
·1140-1146
·
IF 7.394
Chunmei Gao,Shaoyu Lü,Mingzhu Liu,Can Wu,Yun Xiong
The synthesis and properties of CO2 responsive and fluorescent dendritic polymers, poly(amido amine)/Pluronic F127 (PAMAM/F127), are reported in this paper. The morphologies and sizes of PAMAM/F127 dendritic polymers were investigated by dynamic light scattering (DLS) and transmission electron microscopy (TEM). PAMAM/F127 dendritic polymers showed unimolecular micelle morphologies at low concentrations, and changed to multimolecular micelles at higher concentrations. Additionally, fluorescence spectra and confocal laser scanning microscopy images showed that PAMAM/F127 dendritic polymers exhibited a fluorescent enhancement response to the presence of CO2. Apart from that, the release behavior of PAMAM/F127 gels under simulated body fluids was investigated by choosing curcumin as the hydrophobic drug. The results indicated that PAMAM/F127 dendritic polymers can be used to improve the solubility of curcumin, and the drug released faster in the presence of CO2. Such CO2 responsive fluorescent dendritic polymers are potentially applicable in cellular imaging or drug controlled release.
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PubMed
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Polymer Chemistry
·
2014
·Vol. 5
·期 24
·7109-7120
·
IF 5.368
Ning Che,Saina Yang,Hongliang Kang,Ruigang Liu,Zhuang Li,Zhijing Liu,Pingping Li,Xiaozhong Qu,Yong Huang
Dextran graft poly((N-amidino)hexyl methacrylamide) (Dex-g-PAHMA) copolymers were synthesized by free radical polymerization in aqueous solution and characterized. Dex-g-PAHMA copolymers can self-assemble into micelles with the PAHMA rich core and dextran rich shell in aqueous media. The CO2 sensitivity of the micelles was investigated by dynamic light scattering (DLS), conductivity and zeta potential. The results confirmed that the Dex-g-PAHMA copolymer micelles have reversible CO2 sensitivity. The micelles can be used as doxorubicin (DOX) carriers and DOX molecules are mainly located in the core of the micelles. The MTT assay indicated that the Dex-g-PAHMA graft copolymers are non-toxic to cells in the copolymer concentration range of 5–1000 μg mL−1, whereas the relative cell viability is greatly reduced with the increase of copolymer concentration for DOX-loaded micelles. The DOX-loaded micelles can be endocytosed by MCF-7 cells and the DOX can release from micelles and diffuse into the cell nucleus. The Dex-g-PAHMA copolymers have promising applications as drug carriers for cancer therapy.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2015
·
IF 2.037
Yu Zhang,Wei Su,Yan Sun,Jia Liu,Xiuwu Liu,Xiaojing Wang
MIL-101 is a promising adsorbent because of its large pore volume, high separation selectivity, easy regeneration, and good stability. MIL-101 was synthesized and characterized by X-ray diffraction, scanning electron microscopy, and nitrogen adsorption at 77 K. Adsorption isotherms of pure N2, CH4, and CO2 were measured on MIL-101 from 263 K to 313 K and at pressures up to 0.8 MPa. The Langmuir model was a good fit for the experimental isotherms and the isosteric heats of adsorption decreased in the order: CO2 > CH4 > N2. The CO2/CH4 separation selectivity was sensitive to the adsorption pressure and temperature and it varied from 3.2 to 6.3. In contrast, the CH4/N2 separation selectivity changed from 2.6 to 3.3 with temperature and pressure.
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ACS Sustainable Chemistry & Engineering
·
2015
·
IF 4.642
Lin-Bing Sun,Ying-Hu Kang,Yao-Qi Shi,Yao Jiang,Xiao-Qin Liu
Owing to their high physicochemical stability and low skeleton density, polymers are highly promising for capturing the greenhouse gas CO2. However, complicated monomers, expensive catalysts, and/or severe conditions are usually required for their synthesis, which makes the process costly, tedious, and hard to scale up. In this paper, a facile nucleophilic substitution reaction is developed to synthesize polymers from low-cost monomers, namely chloromethylbenzene and various diamines. Due to the appropriate reactivity of monomers, the polymerization takes place at a low temperature of about 60 °C in the absence of any catalysts. A series of polymers containing plentiful secondary amines are successfully fabricated; these secondary amines provide a proper adsorbate–adsorbent interaction from the viewpoints of selective capture of CO2 and energy-efficient regeneration of adsorbents. Moreover, the materials possess well-defined micropores with the dimension close to the size of adsorbate molecules and subsequently, exhibit the molecule sieving effect. As a result, these materials are active in selective adsorption of CO2 and show high CO2/N2 and CO2/CH4 selectivities. More importantly, the adsorbents can be completely regenerated under mild conditions, and no loss in activity is detected after eight cycles.
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ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Zhenkang Li,Zhiping Wang,Qiwei Yang,Zhiguo Zhang,Yiwen Yang,Qilong Ren,Huabin Xing
Ionic liquid (IL)-mediated extraction methods have drawn much attention due to their reduced environmental impact and improved extraction efficiencies compared to traditional separation methods. However, one long-standing challenge in the application of IL-based extraction processes is the difficulty in recovering high-boiling solutes from the IL phase due to the negligible vapor pressure of ILs and the strong interaction between solutes and ILs. In this study, a new CO2-assisted back-extraction method was developed for the recovery of high-boiling solutes from the IL phase based on the reversible chemical absorption and/or strong physical interaction of CO2 with ILs. We found the distribution coefficient (D) of the typical solute δ-tocopherol in the [P4444][Pro]/DMSO–hexane biphasic system significantly decreased from 10.38 to 2.42 after the introduction of CO2, which greatly reduced the required solvent consumption and the number of back-extractions required for tocopherol recovery. For example, the number of back-extractions required for the recovery of 90% of the tocopherols from the [P4444][Pro]/DMSO–hexane biphasic phase decreased from 24 to 5 with the aid of CO2 absorption, along with a decrease in solvent consumption by approximately 80%. The effects of the structure of the IL, the loading of CO2, the type of cosolvents, and the temperature of the CO2-assisted back-extraction processes were investigated in this study. This proof-of-concept study demonstrates the great potential of CO2-assisted back-extraction as a green method for the efficient recovery of high-boiling solutes from the IL phase.
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Journal of CO2 Utilization
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2017
·
IF 4.292
Changsheng Cao,Zhenhai Wen
Cu-based composites with different compositions and construction can seriously influence its electrocatalytic performance toward CO 2 reduction reaction (CO 2 RR). Herein, we report a microwave-assistant route to prepare Cu nanoparticles decorating reduced graphene oxide (CuNPs/rGO) nanohybrids, which are characterized by a variety of techniques, demonstrating that Cu nanoparticles coupling with Cu x O nanoparticles were uniformly anchored on the surface of rGO, as well as the existence of grain boundaries. The CuNPs/rGO composites are studied as electrocatalyst for CO 2 RR and show a favorable electrocatalytic activity toward CO 2 RR with an onset potential of −0.9 V, corresponding to about only 190 mv overpotential for CO generation. Besides with a small amount of HCOOH (<5%), H 2 and CO are the main CO 2 reduction products with a tunable ratio of from 1.16:1 to 6.38:1 by changing the applied potentials. The gaseous products with various ratio of H 2 to CO can be potentially used as syngas to produce more valuable products in industry. This work demonstrates a simple, facile and effective way to improve the electrocatalytic CO 2 RR performance of Cu-based composites.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2017
·
IF 2.726
Yue Zhao,Shufeng Shen,Yangyang Bian,Ya-nan Yang,Ujjal Ghosh
In this work, CO 2 solubility in aqueous potassium lysinate solutions has been measured for the concentrations of (1.25–3.28) mol·kg −1 and at temperatures of (313–343) K. The vapour-liquid equilibrium data were correlated using a Soft model and a semi-empirical (SE) model. The proposed models can match well with the experimental data with AAD within 20%. The heat of absorption for LysK was estimated as about (55–70) kJ·mol −1 CO 2 absorbed from the solubility data. The lower heat of absorption, compared with that of 30 mass% MEA, will be beneficial for the reduction of regeneration energy.
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LUMINESCENCE
·
2017
·Vol. 32
·期 8
·1448-1455
·
IF 1.509
Jing Li,Shuhua Han
A novel chemosensor TrisRh based on tris(2-aminoethyl)amine and rhodamine 6G is designed and synthesized as a fluorescence turn-on probe for Co 2+ ions that is paramagnetic with a property of quenching fluorescence. Rhodamine spirolactam forms are nonfluorescent, whereas, ring-opening of corresponding spirocyclic induced by Co 2+ results in strong fluorescence emission. Upon the addition of Co 2+ ions, TrisRh can display significant enhancements in absorbance and fluorescence intensity as well as evident colorific transformation, which can be perceived by the naked eye. The association stoichiometry of TrisRh to Co 2+ ions was inferred to be 1:1 through Job's plot and electrospray ionization mass spectrometry analysis. The binding model was speculated from Fourier transform infrared spectra and 1 H–nuclear magnetic resonance technologies. Significantly, the limit of detection was determined to be as low as 1.22 nmol. Furthermore, TrisRh can exhibit robust anti-jamming ability against other interference metal ions.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2016
·Vol. 134
·期 10
·
IF 1.866
Yuanyuan Liu,Xueqin Li,Yun Qin,Ruili Guo,Jianshu Zhang
Novel facilitated-transport mixed-matrix membrane (MMM) were prepared through the incorporation of polydopamine (PDA) microspheres into a poly(amide- b -ethylene oxide) (Pebax MH 1657) matrix to separate CO 2 –CH 4 gas mixtures. The Pebax–PDA microsphere MMMs were characterized by Fourier transform infrared spectroscopy, scanning electron microcopy, X-ray diffraction, differential scanning calorimetry, and thermogravimetric analysis. The PDA microspheres acted as an adhesive filler and generated strong interfacial interactions with the polymer matrix; this generated a polymer chain rigidification region near the polymer–filler interface. Polymer chain rigidification usually results in a larger resistance to the transport of gas with a larger molecular diameter and a higher CO 2 –CH 4 selectivity. In addition, the surface of PDA microspheres contained larger numbers of amine, imine, and catechol groups; these were beneficial to the improvement of the CO 2 separation performance. Compared with the pristine Pebax membrane, the MMM with a 5 wt % PDA microsphere loading displayed a higher gas permeability and selectivity; their CO 2 permeability and CO 2 –CH 4 selectivity were increased by 61 and 60%, respectively, and surpassed the 2008 Robeson upper bound line. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 44564.
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Nano Energy
·
2024
·
IF 16.8
Shanyong Chen,Tao Luo,Xiaoqing Li,Kejun Chen,Qiyou Wang,Junwei Fu,Kang Liu,Chao Ma,Ying-Rui Lu,Hongmei Li,Kishan S. Menghrajani,Changxu Liu,Stefan A. Maier,Ting-Shan Chan,Min Liu
Metal-nitrogen-carbon single-atom catalysts (SACs) have emerged as promising candidates for electrocatalytic CO 2 reduction reaction. However, the perpendicular d z 2 orbital within planar metal site mainly interacts with *COOH, resulting in inferior CO 2 activation. Inspired by reaction-driven active configuration, here we propose to upshift nickel single-atom away from nitrogen-carbon substrate, prominently promoting the interaction between CO 2 and other d orbitals besides d z 2 . Theoretical and experimental analyses reveal that upshifting nickel site away substrate induces d xz , d yz , and d z 2 to hybridize with CO 2 , expediting CO 2 conversion to *COOH. The planar and out-of-plane Ni-N sites are formed on carbon nanosheet (Ni 1 -N/C NS ) and curved nanoparticle (Ni 1 -N/C NP ), respectively, which is verified by X-ray absorption fine structure spectroscopy. Impressively, the Ni 1 -N/C NP presents CO Faradaic efficiency of 96.4 % at 500 mA cm −2 and energy conversion efficiency of 79.8 % in flow cell, outperforming Ni 1 -N/C NS and most SACs. This work highlights the simulation of reaction-driven active sites for efficient electrocatalysis .
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2024
·
IF 2.2
Jing Xia,Zhigao Sun
Thermodynamic inhibitors may be used to inhibit hydrate formation in industry. Alcohol substances, due to their hydrophilic hydroxyl groups in their molecular structure, are prone to form hydrogen bond with water molecules to inhibit hydrate formation. In this work, sec -butyl alcohol is chosen to study the effects on CO 2 hydrate dissociation equilibrium conditions, where the step-heating method is utilized to obtain hydrate equilibrium conditions. The equilibrium curve of carbon dioxide hydrate dissociation moves to the region of lower temperatures or higher pressures. The higher mass fraction of sec -butyl alcohol, the better effect of inhibiting hydrate formation. Sec-butyl alcohol can be used as a thermodynamic hydrate inhibitor.
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