MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Xiaoli Ding,Yongfu Tang,Hongyong Zhao,Qingping Xin,Yuzhong Zhang
Hollow SAPO-34 with an average particle size of ca .370 nm was synthesized by selective etching its precursor under the controlled alkaline condition. Subsequently, freestanding mixed matrix membranes were synthesized by UV-induced in-situ polymerization of the mixture of hollow SAPO-34, the fluorinated monomer , and the trifunctional cross-linker. The structure and the physical characteristic of hollow SAPO-34 and membranes were characterized by scan electron microscope, wide-angle X-ray diffraction, etc. The effect of the hollow SAPO-34 loading amount on the gas permeation-separation performance of mixed matrix membranes was investigated. The results showed that hollowing out SAPO-34 improved the N 2 /CH 4 sorption selectivity and converted the crystals from preferential adsorption of N 2 to preferential adsorption of CH 4 , the incorporation of hollow SAPO-34 into membranes increased the N 2 /CH 4 solubility selectivity and the permeability. The optimal membrane exhibited a 39-fold increase in N 2 permeability from 6.9 × 10 −13 to 2.7 × 10 −11 cm 3 (STP)cm·cm −2 ·s −1 ·Pa −1 at 0.2 MPa and 35 °C without the loss of N 2 /CH 4 permselectivity, which exceeded the 2008 Robeson upper bound.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Ke Chen,Linhan Ni,Hao Zhang,Chengming Xiao,Li Li,Xin Guo,Junwen Qi,Chaohai Wang,Xiuyun Sun,Jiansheng Li
Rational design of fillers and polymers is of great importance to fabricate mixed matrix membranes (MMMs) with high performance. In this work, fluorinated metal-organic frameworks (KAUST-7 (also referred as NbOFFIVE-1-Ni)) were adopted as nanofillers to prepare MMMs through physically blending into the polymer of intrinsic microporosity (PIM-1). Benefiting from the features of porous KAUST-7, including well CO 2 affinity, distinctive pore characteristics (size, shape, and functionality) and strong intermolecular interactions with PIM-1, the achieved MMMs demonstrated increased CO 2 /CH 4 separation performance and improved anti-physical aging property. Specifically, with the assistance of KAUST-7, the CO 2 permeability and CO 2 /CH 4 (30:70 vol%) selectivity of the optimized MMMs increased up to 5928 Barrer and 23.5, corresponding to improvements of 50% of and 88% of the permeability and selectivity compared with the pristine membranes, respectively. Importantly, 100-h continuous separation test results confirmed the satisfying long-term stability of the prepared MMMs. Notably, the MMMs maintained 91% of the initial CO 2 permeability after 150 days (decreased only 539 Barrer), implying that the CO 2 permeability decrement is about 5-fold lower than that of the control PIM-1 membrane. These results suggest that the fabricated MMMs are promising candidates for CO 2 separation in practical applications.
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ENERGY
·
2022
·
IF 8.857
Haorui Liu,Shuoyu Wang,Xiaoqiong Wang,XiaoJing Feng,Shuixia Chen
A novel stable porous solid amine adsorbent with three-dimensional interpenetrating network structure was prepared by polymerization of divinylbenzene using high internal phase emulsion (HIPE) template method , and followed by further introducing polyethyleneimine (PEI) by impregnation-crosslinking method. Fixed bed dynamic adsorption experiment proved that under wet condition, the former exhibited not only a higher capacity of 6.22 mmol/g but also a better adsorption kinetics process with faster adsorption rate and longer lag in breakthrough point, which makes it potential to be used in gas separation. In CO 2 /CH 4 separation experiment, PolyHIPE-PE30-4 showed a CO 2 /CH 4 separation selectivity of 253 at 298 K and 1 bar, and meanwhile exhibited an extra-high operating capacity. The pure methane productivity of PolyHIPE-PE30-4 was 24.1 mmol/g from CO 2 /CH 4 (80:20, v/v) mixed gas, 4.5 times to that of PE30-4 gel (5.36 mmol/g). Significantly, PolyHIPE-PE30-4 could maintain an excellent regeneration performance after at least 7 cycles, while PolyHIPE-P30 exhibited a remarkably decrease in adsorption capacity after only three adsorption-desorption process in wet condition, demonstrating the advantage of impregnation-crosslinking method for amine functionalization. The superior CO 2 adsorption capacity and regeneration stability, combined with its superior adsorption kinetics property make it a broad prospect in the field of CO 2 /CH 4 separation.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 17
·5048-5057
·
IF 5
Fengyun Su,Zhishuai Wang,Mengzhen Tian,Kecheng Liu,Haiquan Xie,Wenguang Tu,Yezhen Zhang,Xiang Li,Xiaoli Jin,Xin Ying Kong
The photocatalytic reduction of carbon dioxide (CO2) into renewable fuels holds great promise as a sustainable energy production approach, addressing both the imminent energy crisis and global warming simultaneously. However, the poor CO2 adsorption and rapid recombination of photogenerated charge carriers on semiconductors greatly limit the CO2 conversion efficiency along with poor selectivity towards the desired product. Herein, we propose that the construction of a homojunction in a crystalline–amorphous photocatalyst can greatly enhance its photocatalytic performance. In this study, we developed a hydrated niobium pentoxide (HNBO) homojunction with co-existing crystalline and amorphous structures through a facile hydrothermal method. The resulting crystalline–amorphous HNBO demonstrated exceptional photocatalytic activity for CO2 reduction into methane (CH4) and carbon monoxide (CO), in which the selectivity for CH4 reached 85.7%. The superior performance of HNBO can be attributed to the following factors: (i) the presence of a large specific surface area (355 m2 g−1) due to the aggregation of HNBO nanoparticles with abundant “ink bottle” mesopores, (ii) the abundant OH− groups on HNBO promoting the adsorption and activation of CO2, (iii) the enhanced separation of charge carriers resulting from the crystalline–amorphous homojunction interface, and (iv) a narrowed bandgap along with an elevated conduction band potential to give strong reduction power. This work presents a remarkable instance of a solitary crystalline–amorphous material for CO2 photoreduction into CH4 with superior activity and high selectivity. Notably, this was achieved without the need for any dopants or co-catalysts, underscoring the elegance of this photocatalyst.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Wenjie Xiong,Mingzhen Shi,Lingling Peng,Xiaomin Zhang,Xingbang Hu,Youting Wu
CO 2 and H 2 S are considered impurities in natural gas that moderate the pace of environmental health. Developing highly efficient and cost-effective absorbents is of significance for sweetening natural gas. Herein, four superbase protic ionic liquids (SPILs) were prepared in this study. Typical physical properties (density, viscosity, and decomposition temperature) were also examined at ambient pressure. These SPILs show low viscosity values at ranging from 5.1 cP to 18.3 cP at 313.2 K. The solubility of H 2 S (0–1.0 bar), CO 2 (0–1.0 bar), and CH 4 (0–5.0 bar) was systematically measured at temperatures in the range of 298.2 K to 333.2 K. Impressively, the absolute solubility of H 2 S under 0.1 bar was found to be located at 4.31–5.15 mol/kg at 313.2 K, which is the highest value obtained among the reported results in the literature. The ideal selectivity of H 2 S/CH 4 and CO 2 /CH 4 (H 2 S or CO 2 solubility at 0.1 bar vs CH 4 solubility at 1 bar) at 313.2 K are in the ranges of 367–653 and 92.4–240, respectively. The interaction mechanism we explored was characterized by NMR and FT-IR spectroscopy. Thermodynamic parameters, such as enthalpy, Gibbs free energy, and entropy of dissolution were calculated from the temperature dependent solubility using the “deactivated model”. These SPILs are promising alternative candidates for the simultaneous removal of H 2 S and CO 2 in natural gas upgrading.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yingying Wang,Qixin Zhou,Yongfa Zhu,Dongsheng Xu
Solar-energy-driven CO 2 and H 2 O conversion into value-added chemical fuel holds great potential in solving the greenhouse effect problem and the energy crisis. Herein, the novel lead-free perovskite Cs 3 Sb 2 I 9 photocatalyst was developed to realize high efficiency reduction of CO 2 to CO and CH 4 by photothermal synergistic catalysis. The production rate of the novel catalytic system is 95.7 μmol g −1 h -1 without any sacrificial agents or cocatalysts, which are 87-fold and 5.2-fold higher than that of pure photocatalysis and pure thermal catalysis respectively, and an order of magnitude higher compared to previous literatures. Through the obtained evidence of the formate active intermediates, defects active sites produced in reaction process and photogenerated charge enhanced activity driven by built-in electric field, it is revealed that the defects active sites produced by the thermal excitation of Cs 3 Sb 2 I 9 photocatalyst can adsorb and activate CO 2 , while the plentiful electrons excited by light can provide the CO 2 reduction capacity, the synergistic effect of them enhance the activity of CO 2 reduction reaction. This work firstly reports the novel Sb-based perovskite material was developed as photocatalyst for artificial synthetic CO 2 and H 2 O into solar energy fuels and provides new insights on photothermal synergistic catalysis.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Yingqian Wang,Jihong Sun,Tallat Munir,Bingying Jia,Anadil Gul
Clinoptilolite (CP) with various morphologies, such as spherical, flower, cylindrical, and disc-shape, were successfully synthesized in the presence of alcohol solvents with different carbon chain lengths. The structural and textural properties of the resultant CPs were characterized via XRD, SEM, TG-DSC profiles, TEM, NMR, FT-IR spectra, and N 2 sorption isotherms. The effect of the additive amount of various alcohol solvents on the induction (nucleation) periods and growth stages of synthetic CPs were detailed investigated. Their activation energies of induction ( E n ) and growth ( E g ) periods during crystallization intervals were calculated according to the Arrhenius equation, where the former being larger than the latter, indicating that nucleation is the key step during the whole synthesis of CPs. Particularly, the E n value gradually increased as the increasing chain-length of the used alcohol, but smaller than that without additive alcohols. These demonstrations implied that the presence of alcohol solvents is beneficial to promote the nucleation process of synthetic CP. Furthermore, their CH 4 and N 2 adsorption capacity and selectivity were preliminary explored, showing the highest selective factor of 5.58 at 0 °C for CH 4 /N 2 separation using flower-like CP as an adsorbent. These results suggested a promising adsorbent for wide applications in gas separation.
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Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 8
·2043-2049
·
IF 5.934
Di Liu,Guangsheng Pang,Zhiyong Tang,Shouhua Feng
Interfacial engineering has demonstrated a significant effect on fabricating highly efficient membranes for gas separation. Herein, we introduced a new way to prepare a soft MOF membrane with a modified interface using polyelectrolyte branched polyethyleneimine (PEI) as the joint material. Assembled with layered graphene oxide (GO) and zeolitic imidazolate framework-8 (ZIF-8) nanocrystals, branched PEI not only functions as a soft coat onto the ZIF-8 surface to overcome the rigid nature but also well connects with GO nanosheets via electrostatic attraction, thus preventing the fracture of the membrane. When employed as the gas separation membrane for H2/CH4, the long gas diffusion pathway determined by layered GO and the accurate sieving effect endowed by ZIF-8 enable the remarkable permeance and selectivity. Furthermore, by simply altering the content of GO nanosheets and ZIF-8 nanocrystals in the composite membrane, one can easily adjust the permeance and selectivity toward the separation of H2/CH4 gas mixture.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Daofei Lv,Renfeng Shi,Yongwei Chen,Yang Chen,Houxiao Wu,Xin Zhou,Hongxia Xi,Zhong Li,Qibin Xia
A water resistant zirconium–porphyrin metal–organic framework PCN-222 was synthesized for selectively separating CO2/CH4 and CO2/N2. Isotherms of CO2, CH4, and N2 on PCN-222 at low and high pressures were respectively measured. At 298 K, CO2 uptakes at 100 and 3000 kPa were 1.16 and 13.67 mmol/g, respectively. At 298 K and 100 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities separately reached 4.3 and 73.7. At 298 K and 3000 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities were 4.7 and 32.8, respectively. Importantly, breakthrough experiments confirmed that PCN-222 could achieve the effective separation of CO2/CH4 (both 50:50 and 10:90) and CO2/N2 (both 50:50 and 15:85) gas mixtures. The dynamic regeneration experiments showed that PCN-222 maintained its initial CO2 adsorption capacity after five cycles of CO2 adsorption–desorption. This work suggested that PCN-222 was a potential candidate for selectively separating CO2/N2 and CO2/CH4.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2013
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IF 3.548
Zebao Rui,Danyan Feng,Huayao Chen,Hongbing Ji
Highly-ordered TiO 2 nanotube array (TiNT) was prepared by an electrochemical anodization method and used as the support for Ni and Ni–M (M = Ru, Pt and Rh) bimetallic catalysts . Ni/TiNT and Ni–M/TiNT were then applied to the combination reactions of the partial oxidation of methane reaction (POM) with the carbon dioxide reforming with methane reaction (CRM) for the syngas production . The results show that Ni/TiNT suffers from the formation of NiO and NiTiO 3 , and the coke deposition. The superior catalytic performance and the enhanced resistance ability against carbon formation are obtained over a small amount of noble metal modified Ni bimetallic catalysts, which are ranked as Ni/TiNT < Ni–Ru/TiNT < Ni–Pt/TiNT < Ni–Rh/TiNT. The interaction of Ni–M, i.e., enhanced reducibility of NiO and the maintenance of metallic Ni species even in the presence of oxygen, over Ni bimetallic catalysts is regarded as an important reason. Much short distance between the exothermic and the endothermic zones over Ni–M/TiNT catalysts bed can be realized, and a flat temperature profile in the catalyst bed is expected, which in turn can relieve the hot-spot and NiTiO 3 formation to some extent.
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RSC Advances
·
2016
·Vol. 6
·期 55
·50138-50143
·
IF 3.289
D. Li,W. B. Li,J. S. Shi,F. W. Xin
Hexagonally packed mesoporous silica (HMS) was used as a kind of template-like material to prepare heteroatom doped porous carbons from the polymerization reactions of resorcinol and formaldehyde in the HMS pore channels. Different acids (HNO3, H2SO4, H3PO4) were used to catalyze the polymerization reactions to obtain N-doped, S-doped, and P-doped porous carbons, respectively. The adsorption properties of H2, CH4, and CO2 were investigated on these doped carbon materials systematically. For the hydrogen adsorption, the adsorption amount was 11.8%, 21.1%, and 33.3% higher on N-doped, S-doped, and P-doped porous carbons, respectively, than the carbon sample without doping, and the highest hydrogen uptake reached 14.88 mmol g−1 on the P-doped sample; regarding the CO2 adsorption, the adsorption amount reached 3.60 mmol g−1 and 3.16 mmol g−1 on the S-doped sample and N-doped sample, respectively, which is 39.5% and 22.5% higher than the sample without doping; it also shows that methane uptake amount was significantly increased by 27.1% on the S-doped sample as compared to the sample without doping, i.e., 3.52 mmol g−1 of CH4. Therefore, it is predicted that these doped carbon materials with high specific surface area are of great potential for the gas adsorption of H2, CH4, and CO2.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Yating Xie,Nicui Yuan,Hongyang Liu,Lukai Luo,Jun Gong,Xiping Yin,Tengfei Li,Yonghua Zhou
Defect engineering by creating oxygen vacancies (OVs) and heterogeneous frustrated Lewis acid-base pairs (FLPs) emerged as an efficient strategy to enhance the selective conversion CO 2 to CH 4 . Considering the intrinsic FLPs contained in UiO-66-NH 2 (UNH for abbreviation), in this paper, the OVs was introduced therein by fabricating the Ce-doped UNH (denoted as UNH(Ce/Zr)) via one-step solvothermal route. The as-prepared UNH(Ce/Zr) catalyst exhibited the CH 4 yield of 31.02 μmol·g −1 ·h −1 accompanied with the CH 4 selectivity of 93 % and satisfying recycling stability. The XRD, SEM, FT-IR, XPS, TG, TPD and NH 3 in situ DRIFTS and in situ FT-IR characterization results justified that the UNH(Ce/Zr) possess the obviously increased OVs sites and enhanced Lewis acidic and basic properties. Additionally, the photoelectrochemical characterization results showed that UNH(Ce/Zr)−0.014 efficiently improved photogenerated electron-hole separation efficiency and charge transfer rate. It could be concluded that it was the cooperative action of OVs and FLPs that led to the high CH 4 selectivity and CH 4 yield.
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