ACS Omega
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2019
·
IF 2.584
Junjie Zhu,Linbo Wu,Zhiyang Bu,Suyun Jie,Bo-Geng Li
UiO-66-NH2, a zirconium-based functional metal–organic framework (MOF), was postsynthetically modified via Schiff base reaction between aldehyde groups in glutaraldehyde and amino groups in UiO-66-NH2 and CO2-preabsorbed polyethyleneimine (PEI). The resulting PEI-modified MOFs, abbreviated as PEIC@UiO, were characterized with 1H NMR, Fourier transform infrared, powder X-ray diffraction, Brunauer–Emmett–Teller, scanning electron microscopy, and thermogravimetric analysis and evaluated as CO2 adsorbents. In comparison with pristine UiO-66-NH2, the PEIC@UiO adsorbents have reduced specific surface area (7–150 m2/g) but maintained the same crystal structure. Particularly, the PEIC96@UiO adsorbent exhibited significantly improved CO2/N2 adsorption selectivity (48 vs 25) and higher CO2 adsorption capacity (3.2 vs 2.7 mmol/g). The adsorbent also displayed moderate desorption energy (68 kJ/mol CO2), superior moisture endurance, and recyclability, which are very desirable for practical applications.
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JOURNAL OF MEMBRANE SCIENCE
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2019
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IF 7.015
Guangli Yu,Yanqin Li,Ziyang Wang,Terence Xiaoteng Liu,Guangshan Zhu,Xiaoqin Zou
Membrane separation has great potential for carbon dioxide capture. We have been developing porous organic frameworks (POFs) as a new class of nanofillers for mixed matrix membranes fabrication. A triangle monomer of melamine (MA) reacts with another linear monomer of 1, 4-piperazinedicarboxaldehyde (PDA) in a microwave system to form the POF material (designated as MAPDA). As-synthesized MAPDA possesses an open framework featured with high surface area of 548.3 m 2 g −1 and a large pore of ~1.0 nm. SEM shows that MAPDA particles are in size of ~42 nm, and adsorption measurement reveals that MAPDA is favorable for adsorbing CO 2 with an uptake of 47.0 cm 3 g −1 at 298 K and 101 kPa. Mixed matrix membranes of MAPDA/PIM-1 with different MAPDA loadings (0–20 wt%) are produced by blending nanofillers of MAPDA and soluble matrices of PIM-1. Single gas permeations demonstrate that CO 2 permeability is increased dramatically from 3694.5 to 7861.9 Barrer, meanwhile the CO 2 /N 2 selectivity is enhanced from 18.9 to 23.9 for pure PIM-1 and for a representative membrane of MAPDA/PIM-1 with 15 wt% MAPDA. High porosity and molecular affinity make the predominant contribution to the enhancements of CO 2 permeability and CO 2 /N 2 selectivity. MAPDA/PIM-1 membranes are also very selective for capturing CO 2 from gas mixtures of 50CO 2 :50N 2 and 15CO 2 :85N 2 with separation performances exceeding the latest upper bound. The good separation property and the high stability of MAPDA/PIM-1 have shed a light on next-generation membrane for CO 2 separation development.
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AICHE JOURNAL
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2019
·Vol. 65
·期 6
·e16605
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IF 3.463
Min Xiao,Wenchao Zheng,Helei Liu,Paitoon Tontiwachwuthikul,Zhiwu Liang
1-(2-Hydoxyethyl)-piperidine (1-(2HE)-PP) is a new tertiary amine with desirable properties and can be potentially used to formulate superior absorbents for CO 2 capture. The equilibrium CO 2 solubility of 1-(2HE)-PP solution is measured over temperatures from 298 to 333 K, CO 2 partial pressures from 8.1 to 101.3 kPa and initial amine concentrations from 1 to 5 M. Two thermodynamic models, namely semiempirical model and activity coefficient model are developed for the system. The activity coefficient model shows better estimation solubility with an absolute average relative deviation (AARD) of 7.6%. In the comparison between the two models, a comprehensive analysis is presented. Some suggestions are provided for the similar model development. In addition, the speciation plot of CO 2 loaded 1-(2HE)-PP solution is predicted based on the activity coefficient model. The predictive pH values agree well with experimental data with AARD of 1.0%. Finally, the potential of 1-(2-HE)PP to be an alternative amine in CO 2 capture is evaluated.
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Royal Society Open Science
·
2019
·Vol. 6
·期 3
·
IF 2.515
Fei Wang,Juangang Wang,Yunhuan Cheng
In this paper, a novel photocatalyst CNCC with excellent visible light photocatalytic performance was successfully prepared to optimize the CO2 photoreduction performance. The results showed that the methanol formation rate of CNCC was 24.7 µmol g−1 h−1, which was 1.42 times higher than that of NCC. The enhanced photoactivity is attributed to the rapid propagation of charge carriers induced by light from the constructed composite structure.
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Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 7
·1799-1812
·
IF 5.934
Xiaosong Hu,Chaoyue Zhao,Qingxin Guan,Xin Hu,Wei Li,Jun Chen
The chemical transformation of CO2 not only mitigates CO2 released into the atmosphere but also produces fuels and chemicals with important additional value. The activation of stable CO2 molecules is the key difficulty for the efficient conversion of CO2. Herein, we designed a ternary catalyst containing Cu, ZnO, and CeOx and dispersed them in SBA-15 using incipient wetness impregnation. Interestingly, the catalytic performances were improved greatly when the related active components were dispersed inside and outside the pore channels of SBA-15 using the incipient wetness impregnation method. Methanol and CO were controllably produced on the interface of Cu and metal oxides (ZnO and CeOx) due to the synergistic effects between the three active components. The metal oxides play a more important role in CO2 conversion as well as the product selectivity compared to Cu. CeO2 is more efficient than ZnO in promoting the dispersion of Cu nanoparticles and methanol generation. The suitable pore channels of SBA-15 promote the mass transfer and heat transfer while the high specific surface area is favorable to the dispersion of active components, which will facilitate the production of methanol and CO. After continuous hydrogenation evaluation for 100 h, the catalytic performance of the catalyst was still very stable. This work provides a viable strategy to prepare a supported catalyst with highly dispersed active sites, and the catalyst exhibits an efficient catalytic effect on producing methanol and CO.
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JOURNAL OF MOLECULAR LIQUIDS
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2019
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IF 4.561
Xiangrui Meng,Yijin Mi,Dongling Jia,Ning Guo,Yarui An,Yuqing Miao
Co hydroxide polymorphs (green α-Co(OH) 2 , red β-Co(OH) 2 and brown β-Co(OH) 3 ) formed at separate positions in a test-tube. Diffusion of hydrazine hydrate downward in agar gel facilitated the reaction between hydrazine and Co 2+ leading a dilatational wave of reactant concentration. The resulting periodic Liesegang bands of α-Co(OH) 2 were observed due to the diffusion hindrance of reactants. It can be deduced that the high concentration of Co 2+ causes formation of α-Co(OH) 2 while the low concentrations produce β-Co(OH) 2 . β-Co(OH) 2 is oxidized readily to form brown β-Co(OH) 3 at the upper area of agar gel with high alkali condition and O 2 distribution. This study is helpful to learn the formation of more than one product and prepare multiple materials in single chemical reaction system. In addition, the obtained α-Co(OH) 2 has been stabilized in the gel medium for at least 3 months. It may facilitate its application in many areas especially in electrochemical area since α-Co(OH) 2 typically exhibits higher conductivity and electrocatalysis than β-Co(OH) 2 while in the past its application often is limited by thermodynamically instability.
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CARBOHYDRATE POLYMERS
·
2019
·
IF 6.044
Lihua Zhang,Wentao Shi,Junqin Wang,Longming Jin,Gang Hu,Qiang Zheng,Haibo Xie,Peng Chen
Gelation and rheological behaviors of cellulose/CO 2 -based reversible ionic liquid (RIL)/DMSO solutions were investigated. The exponents of specific viscosity η sp versus concentration c were determined for wood pulp (WP) and microcrystalline cellulose (MCC) solutions. The complex viscosity acquired using oscillatory shear closely follows the steady shear viscosity, thus revealing the applicability of Cox-Merz rule. The influence of RIL content in the solvent on apparent viscosities, activation energy, intrinsic viscosities, specific viscosity-c[η] master curve, and relaxation time were also investigated. Gelation occurred in this cellulose solution system due to thermal-induced CO 2 release from the decomposition of the CO 2 -based reversible ionic liquid. The formed gel was stable in air, but re-dissolved when exposed to CO 2 , indicating the switch-on and switch-off effects of CO 2 in cellulose dissolution and gelation.
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Journal of the Taiwan Institute of Chemical Engineers
·
2019
·
IF 3.834
Yifu Li,Dongbo Wang,Guojing Yang,Xingzhong Yuan,Qiuxiang Xu,Xuran Liu,Yali Wang,Renpeng Guan,Qizi Fu,Fu Chen
A novel Co 2+ /peroxymonosulfate (PMS)/Acid pretreatment enhanced waste activated sludge (WAS) dewaterability. Experimental results showed that Co 2+ /PMS/Acid pretreatment reduced capillary suction time (CST) of WAS by 52.1% under 0.158 mmol/g TSS PMS and 0.079 mmol/g TSS Co 2+ at pH 4. In this circumstance, water content of sludge cake (WC SC ) dropped to 73.7%. The mechanisms were elucidated with a suite of macro and spectroscopic evidence. During the pretreatment, Co 2+ activated PMS to generate SO 4 •− and • OH under acidic condition, these radicals decomposed extracellular polymeric substances (EPS) and destroyed integrity of microbial cell wall. They also facilitated removal of high molecular weight biopolymers in EPS fractions. Co 2+ , its oxidative product ( i.e. , Co 3+ ), and H + reduced negative charge of EPS functional groups. Moreover, many voids were formed on sludge surface after pretreatment. Finally, the bound water content and viscosity reduced but the flocculability and amount of drainage holes of WAS increased. All these results induced the enhancement of WAS dewaterability.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2019
·Vol. 136
·期 28
·47755
·
IF 2.188
Yixuan Wang,Jiawen Fu,Qingfu Zhang,Liping Lin,Chunhai Yi,Bolun Yang
In this work, ether oxide (EO)-based multilayer composite membranes were prepared via interfacial polymerization (IP) of trimesoyl chloride (TMC) and polyetheramine (PEA) on polydimethylsiloxane precoated polysulfone support membrane. The effects of preparation parameters, such as monomer concentrations, reaction time, and heat-treatment temperature on the membrane performance were investigated. The optimal preparation parameters have been concluded. The results showed the increasing monomers concentration of both PEA and TMC can lead to the decrease of CO 2 permeance and increase of CO 2 /N 2 selectivity. The optimal monomers concentration was found. When monomer concentrations are higher than the optimal values, the CO 2 permeance decreases continually while CO 2 /N 2 selectivity only shows a very limited improvement with the further increase of monomers concentration. The reaction time has similar effects on membrane performance as the monomers concentration. The effect of heat-treatment temperature was also studied. With the increasing heat-treatment temperature, the CO 2 permeance shows a decrease tendency, while the CO 2 /N 2 selectivity shows a maximum at 80 °C. When PEA is 0.013 mol L −1 , TMC is 0.020 mol L −1 , reaction time is 3 min, and heat-treatment temperature is 80 °C, the optimum preparation conditions are achieved with CO 2 permeance of 378.3 gas permeation unit (GPU) and CO 2 /N 2 selectivity of 51.7 at 0.03 MPa. This work may help to design and fabricate gas separation membranes with desired performance. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136 , 47755.
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
·
2019
·Vol. 36
·期 9
·1900016
·
IF 4.194
Nina Jiang,Yiwei Wang,Danyang Li,Jie Niu,Shibin Wang,Aizheng Chen
Various C-doped metal oxide nanoparticles (NPs) are prepared from metal nitrates in poly-(methyl vinyl ether- co -maleic anhydride) (PVM/MA) nanoreactors. The loading of metal nitrates in the nanoreactors is realized via a process of solution-enhanced dispersion by supercritical CO 2 . When the temperature exceeds the thermal decomposition temperature of the nitrates, the nitrates-loaded nanoreactors transform into C-doped metal oxide NPs. ZnO, NiO, and Co 3 O 4 NPs as representative of the doped oxides are successfully fabricated. A precise control over the doping concentration and doping site in the lattice is achieved by changing the mass ratio between PVM/MA and metal nitrate. The controllable carbon doping avoids undesirable aggregation of carbon species and metal oxide NPs, endows the NPs with broad and strong absorption bands in the visible light region, and creates channels for separation of photo-generated electrons and holes. In this regard, the resultant C-doped metal oxide NPs exhibit excellent photocatalytic, photo-induced antibacterial, and photothermal performances.
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Journal of CO2 Utilization
·
2019
·
IF 5.189
Shanshan Chai,Yong Men,Jinguo Wang,Shuang Liu,Qiaoling Song,Wei An,Gunther Kolb
Catalytic reduction of CO 2 to methane has been recognized as one of the most important strategic reactions to produce highly valuable chemicals and for storage of renewable energy (power-to-gas). This study demonstrates a crystal facet-dependent catalytic reduction of CO 2 to CH 4 on ruthenium nanoparticles deposited over TiO 2 nanocrystal with exposed (001) and (101) facets. Compared with TiO 2 (101) nanocrystal with the same Ru loading, Ru nanoparticles supported by TiO 2 (001) exhibited a highly enhanced CO 2 conversion rate and significantly improved methanation reactivity, along with a considerable durability. The physicochemical properties of the samples were characterized by HR-TEM, XRD, BET, FT-IR, UV–vis, Raman, ICP, and temperature-programmed reaction with CO 2 , and CO 2 + H 2 . In view of the difference in catalytic activity and the physicochemical properties of the supported Ru/TiO 2 catalysts, the results uncovered that the nature of the catalyst support of Ru/TiO 2 strongly affected the dispersion of Ru species and the synergistic effect between Ru and underlying TiO 2 supporting materials due to the strong metal-support interaction, and thus affected their capability to activate CO 2 and determined the catalytic activity for CO 2 methanation. Our work demonstrated the important role of the exposed crystal facets of the underlying support and the resulting Ru particle which had a large effect on CO 2 methanation.
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APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Zhiwei Wang,Sha Li,Shaohua Xie,Yuxi Liu,Hongxing Dai,Guangsheng Guo,Jiguang Deng
Volatile organic compounds (VOCs) cause damage to atmospheric environment and human health. Supported noble metal catalysts are widely used to control VOCs emissions. The high cost, and low H 2 O-, CO 2 -, and SO 2 -resistance of such catalysts are worthy to be improved. Herein we fabricated Ce-, V-, or W-doped TiO 2 supported ultralow loading Pt catalysts via the in-situ molten salt method, and evaluated their catalytic performance for acetone (major pollutants in pharmaceutical industry) removal. Under the present reaction conditions, all the catalysts exhibited high catalytic activity and stability for acetone oxidation , with the temperature required 90% acetone conversion being of 245 °C over 0.57 wt% CeO 2 -0.05 wt% Pt/TiO 2 . The doping of Ce, V, or W enhanced the H 2 O-, CO 2 -, and SO 2 -tolerance ability of 0.05 wt% Pt/TiO 2 . More than 85 %85%, 70%, or 60% of acetone could be removed even in the presence of 20 vol% water vapor, 10 vol% CO 2 , or 100 ppm SO 2 , respectively. The improvement in SO 2 -tolerance ability was due to the inhibition of SO 2 adsorption and oxidation activity as well as Ti(SO 4 ) 2 or TiOSO 4 formation. Acetone complete oxidation over 0.57 wt% CeO 2 -0.05 wt% Pt/TiO 2 would follow the pathway: adsorbed acetone molecules → acetic acid and formic acid → carbonate species → CO 2 and H 2 O. The present supported Pt catalysts might be suitable for oxygenated VOCs removal.
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