Publications
82 results found
Ghalei B, Sakurai K, Kinoshita Y, et al., 2017, Enhanced selectivity in mixed matrix membranes for CO2 capture through efficient dispersion of amine-functionalized MOF nanoparticles, Nature Energy, Vol: 2, Pages: 1-9, ISSN: 2058-7546
Mixed matrix membranes (MMMs) for gas separation applications have enhanced selectivity when compared with the pure polymer matrix, but are commonly reported with low intrinsic permeability, which has major cost implications for implementation of membrane technologies in large-scale carbon capture projects. High-permeability polymers rarely generate sufficient selectivity for energy-efficient CO2 capture. Here we report substantial selectivity enhancements within high-permeability polymers as a result of the efficient dispersion of amine-functionalized, nanosized metal–organic framework (MOF) additives. The enhancement effects under optimal mixing conditions occur with minimal loss in overall permeability. Nanosizing of the MOF enhances its dispersion within the polymer matrix to minimize non-selective microvoid formation around the particles. Amination of such MOFs increases their interaction with thepolymer matrix, resulting in a measured rigidification and enhanced selectivity of the overall composite. The optimal MOF MMM performance was verified in three different polymer systems, and also over pressure and temperature ranges suitable for carbon capture.
Song Q, Wang A, Zhang TH, et al., 2017, Polymer Membranes of Intrinsic Microporosity for Molecular Separations, 13th International Conference on Materials Chemistry (MC13)
Zeng D, Patzschke C, Fennell P, et al., 2017, Nanostructured Iron-based Mixed Metal Oxides for Efficient H2 Production via Thermochemical Water Splitting, 13th International Conference on Materials Chemistry (MC13)
Song Q, 2017, Multifunctional Porous Materials and Membranes for Energy and Sustainability, 13th International Conference on Materials Chemistry (MC13)
Song Q, Liu TY, Jelfs KE, et al., 2017, Advanced Microporous Membranes for Molecular Separations, British Zeolite Association 40th Annual Meeting
Song Q, 2017, Functional Microporous Membranes for Energy and Environmental Applications, ChemEngDay UK 2017
Rong Y, Song Q, Mathwig K, et al., 2016, pH-Induced Reversal of Ionic Diode Polarity in 300 nm Thin Membranes Based on a Polymer of Intrinsic Microporosity, Electrochemistry Communications, Vol: 69, Pages: 41-45, ISSN: 1873-1902
“Ionic diode” (or current rectification) effects are potentially important for a range of applications including water purification. In this preliminary report, we observe novel ionic diode behaviour of thin (300 nm) membranes based on a polymer of intrinsic microporosity (PIM-EA-TB) supported on a poly-ethylene-terephthalate (PET) film with a 20 μm diameter microhole, and immersed in aqueous electrolyte media. Current rectification effects are observed for half-cells with the same electrolyte solution on both sides of the membrane for cases where cation and anion mobility differ (HCl, other acids, NaOH, etc.) but not for cases where cation and anion mobility are more alike (LiCl, NaCl, KCl, etc.). A pH-dependent reversal of the ionic diode effect is observed and discussed in terms of tentatively assigned mechanisms based on both (i) ion mobility within the PIM-EA-TB nano-membrane and (ii) a possible “mechanical valve effect” linked to membrane potential and electrokinetic movement of the membrane as well as hydrostatic pressure effects.
Jimenez-Solomon M, Song Q, Jelfs K, et al., 2016, Polymer nanofilms with enhanced microporosity by interfacial polymerization, Nature Materials, Vol: 15, Pages: 760-767, ISSN: 1476-4660
Highly permeable and selective membranes are desirable for energy-efficient gas and liquid separations.Microporous organic polymers have attracted significant attention in this respect owing to their highporosity, permeability, and molecular selectivity. However, it remains challenging to fabricate selectivepolymer membranes with controlled microporosity which are stable in solvents. Here we report a newapproach to designing crosslinked, rigid polymer nanofilms with enhanced microporosity bymanipulating the molecular structure. Ultra-thin polyarylate nanofilms with thickness down to 20 nmwere formed in-situ by interfacial polymerisation. Enhanced microporosity and higher interconnectivityof intermolecular network voids, as rationalised by molecular simulations, are achieved by utilisingcontorted monomers for the interfacial polymerisation. Composite membranes comprising polyarylatenanofilms with enhanced microporosity fabricated in-situ on crosslinked polyimide ultrafiltrationmembranes show outstanding separation performance in organic solvents, with up to two orders ofmagnitude higher solvent permeance than membranes fabricated with nanofilms made from noncontortedplanar monomers.
Song Q, Jiang S, Hasell T, et al., 2016, Molecular Sieves: Porous Organic Cage Thin Films and Molecular-Sieving Membranes (Adv. Mater. 13/2016), Advanced Materials, Vol: 28, Pages: 2652-2652, ISSN: 0935-9648
Song Q, Jiang S, Hasell T, et al., 2016, Porous organic cage thin films and molecular-sieving membranes, Advanced Materials, Vol: 28, Pages: 2629-2637, ISSN: 1521-4095
Porous organic cage molecules are fabricated into thin films and molecular-sieving membranes. Cage molecules are solution cast on various substrates to form amorphous thin films, with the structures tuned by tailoring the cage chemistry and processing conditions. For the first time, uniform and pinhole-free microporous cage thin films are formed and demonstrated as molecular-sieving membranes for selective gas separation.
Song Q, Cao S, Pritchard RH, et al., 2016, Nanofiller-tuned microporous polymer molecular sieves for energy and environmental processes, Journal of Materials Chemistry A, Vol: 4, Pages: 270-279, ISSN: 2050-7496
Microporous polymers with molecular sieving properties are promising for a wide range of applications in gas storage, molecular separations, catalysis, and energy storage. In this study, we report highly permeable and selective molecular sieves fabricated from crosslinked polymers of intrinsic microporosity (PIMs) incorporated with highly dispersed nanoscale fillers, including nonporous inorganic nanoparticles and microporous metal-organic framework (MOF) nanocrystals. We demonstrate that the combination of covalent crosslinking of microporous polymers via controlled thermal oxidation and tunable incorporation of nanofillers results in high performance membranes with substantially enhanced permeability and molecular sieving selectivity, as demonstrated in separation of gas molecules, for example, air separation (O2/N2), CO2 separation from natural gas (CH4) or flue gas (CO2/N2), and H2 separation from N2 and CH4. After ageing over two years, these nanofiller-tuned molecular sieves became more selective and less permeable but maintained permeability levels that are still two orders of magnitude higher than conventional gas separation membranes.
Jimenez-Solomon MF, Song Q, Jelfs KE, et al., 2016, Polymer nanofilms with enhanced microporosity by interfacial polymerisation for molecular separations
Song Q, 2015, Crosslinked polymer, method for producing the same, molecular sieve composition and material separation membranes
Song Q, Liu W, Cao S, et al., 2015, Nanostructured metal oxides for chemical looping processes, Publisher: AMER CHEMICAL SOC, ISSN: 0065-7727
Song Q, Cao S, Jiang S, et al., 2015, Advanced Molecular sieve Membranes, 250th ACS National Meeting & Exposition
Perera DHN, Song Q, Qiblawey H, et al., 2015, Regulating the aqueous phase monomer balance for flux improvement in polyamide thin film composite membranes, Journal of Membrane Science, Vol: 487, ISSN: 1873-3123
Polyamide thin film composite (PA TFC) membranes are synthesized from interfacial polymerization using two amines in the aqueous phase. The conventional monomer, m-phenelynediamine (MPD), is partially replaced by a linear monomer, 1,3–diamino-2-hydroxypropane (DAHP). The water permeability of the membranes improves by around 22% (to 2.67±0.09 L m−2 h−1 bar−1) while keeping the same high salt rejection (96–98%) at an optimum DAHP/MPD ratio of 12.8%. While developing the control PA TFC membrane we introduce a washing step and show that the support surface should be free from surface protective coatings to achieve high water flux (2.18±0.08 L m−2 h−1 bar−1). Incorporating DAHP units into the polyamide network improves the water flux through the membranes fabricated on both original and washed supports. The surface morphologies of polyamide films change significantly with introduction of DAHP, from large ridge-and-valley structure to enlarged nodular structures. High resolution SEM images show an ultrathin polyamide thin film with a thickness that is reduced with addition of DAHP. These influences of DAHP, namely a reduction in the selective layer thickness, an alteration in surface morphology, changes in internal molecular packing and hydrophilicity, are suggested as factors behind the improved water permeability.
Perera DHN, Song Q, Qiblawey H, et al., 2015, Regulating the aqueous phase monomer balance for flux improvement in polyamide thin film composite membranes, Journal of Membrane Science, ISSN: 1873-3123
Di D, Musselman KP, Li G, et al., 2015, Size-Dependent Photon Emission from Organometal Halide Perovskite Nanocrystals Embedded in an Organic Matrix, JOURNAL OF PHYSICAL CHEMISTRY LETTERS, Vol: 6, Pages: 446-450, ISSN: 1948-7185
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- Citations: 146
Solomon MFJ, Song Q, Munoz-Ibanez M, et al., 2015, TFC membranes with intrinsic microporosity by interfacial polymerization for organic solvent nanofiltration, Pages: 679-680
Song Q, Cao S, Pritchard RH, et al., 2014, Controlled thermal oxidative crosslinking of polymers of intrinsic microporosity towards tunable molecular sieve membranes, NATURE COMMUNICATIONS, Vol: 5, ISSN: 2041-1723
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- Citations: 217
Roussenova M, Hughes DJ, Enrione J, et al., 2014, Free Volume, Molecular Mobility and Polymer Structure: Towards the Rational Design of Multi-Functional Materials, 41st Polish Seminar on Positron Annihilation (PSPA), Publisher: POLISH ACAD SCIENCES INST PHYSICS, Pages: 801-805, ISSN: 0587-4246
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- Citations: 11
Song Q, Cao S, Zavala-Rivera P, et al., 2013, Photo-oxidative enhancement of polymeric molecular sieve membranes, Nature Communications, Vol: 4, ISSN: 2041-1723
High-performance membranes are attractive for molecular-level separations in industrial-scale chemical, energy and environmental processes. The next-generation membranes for these processes are based on molecular sieving materials to simultaneously achieve high throughput and selectivity. Membranes made from polymeric molecular sieves such as polymers of intrinsic microporosity (pore size<2 nm) are especially interesting in being solution processable and highly permeable but currently have modest selectivity. Here we report photo-oxidative surface modification of membranes made of a polymer of intrinsic microporosity. The ultraviolet light field, localized to a near-surface domain, induces reactive ozone that collapses the microporous polymer framework. The rapid, near-surface densification results in asymmetric membranes with a superior selectivity in gas separation while maintaining an apparent permeability that is two orders of magnitude greater than commercially available polymeric membranes. The oxidative chain scission induced by ultraviolet irradiation also indicates the potential application of the polymer in photolithography technology.
Song Q, Liu W, Bohn CD, et al., 2013, A high performance oxygen storage material for chemical looping processes with CO2 capture, Energy & Environmental Science, Vol: 6, Pages: 288-298, ISSN: 1754-5692
Nataraj SK, Song Q, Al-Muhtaseb SA, et al., 2013, Thin, Flexible Supercapacitors Made from Carbon Nanofiber Electrodes Decorated at Room Temperature with Manganese Oxide Nanosheets, JOURNAL OF NANOMATERIALS, Vol: 2013, ISSN: 1687-4110
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- Citations: 12
Song Q, Al-Muhtaseb SA, Sivaniah E, 2012, Nanocomposite membrane of a polymer of intrinsic microporosity and zeolitic imidazolate frameworks for gas separation
A series of composite membrane were fabricated from solution casting of the PIM-1/ZIF-8 solution with loading of ZIF-8 ≤ up to ∼ 40 wt %. The nanocomposite membranes were treated with various techniques, e.g., methanol treatment, thermal treatment, and photochemical modification, to improve the permeability or selectivity. For the nanocomposite membrane without methanol treatment, the gas permeability decreased with the loading of ZIF-8 nanoparticles, while the selectivity was maintained without significant loss. After methanol treatment, the permeability of nanocomposite membrane increased with the loading of ZIF-8 nanocrystals and surpassed the Robeson's upper bound. For the pure polymer membranes annealed at ≤ 300°C, the gas permeability slightly decreased while the selectivity was stable. For the PIM-1/ZIF-8 nanocomposite membranes, the gas permeability decreased with the annealing temperature. For the composite membrane with 20 wt % loading of ZIF-8 annealed at 300°C, the CO2 permeability could reach ≈ 1000 Barrer with selectivity of both CO2/N2 and CO2/CH4 as high as 30. The ideal selectivity of other gas pairs, e.g., O2/N2, H2/N2, and H2/CH4, were all enhanced surpassing the Robeson's upper bound. as sorption properties of these nanocomposites were also studied with various types of gases, so their potential as adsorbents or gas storage materials were also evaluated. This is an abstract of a paper presented at the AIChE Annual Meeting (Pittsburgh, PA 10/28/2012-11/2/2012).
Zhang S, Xiao R, Yang YC, et al., 2012, Experimental study of desulfurization of chemical-loping combustion of coal with calcium-based oxygen carrier, Kung Cheng Je Wu Li Hsueh Pao/Journal of Engineering Thermophysics, Vol: 33, Pages: 525-528, ISSN: 0253-231X
In the process of chemical-looping combustion of coal with calcium-based oxygen carrier, large amount of SO 2 was released due to the side reactions occurred between CaSO4 oxygen carrier and coal gasification products. In this work, desulfurization experiments were conducted using MAC iron ore, CaO and limestone as desulfurizers in a laboratory scale pressurized fixed-bed reactor. The influencing factors of temperature, pressure and Ca/S ratio on the removal of SO 2 gas were analyzed. The results showed that the outlet concentration of SO 2 increased with the increase of temperature in the presence of only CaSO 4 oxygen carrier. Adding MAC iron ore into the reactor could reduce the concentration of SO 2 released from the reactor due to the catalytic effect of Fe 2O 3 on suppressing the decomposition of CaSO 4. The desulfurization efficiency of both CaO and limestone showed an increased trend with the increase of temperature, pressure and Ca/S ratio, and CaO showed a better performance than limestone under the same experimental conditions.
Song Q, Nataraj SK, Roussenova MV, et al., 2012, Zeolitic imidazolate framework (ZIF-8) based polymer nanocomposite membranes for gas separation, Energy and Environmental Science, Vol: 5, Pages: 8359-8369, ISSN: 1754-5692
Kotrappanavar NS, Zavala-Rivera P, Song Q, et al., 2012, High performance ordered nanoporous membranes from block copolymers, Euromembrane Conference, Publisher: ELSEVIER SCIENCE BV, Pages: 632-633, ISSN: 1877-7058
Xiao R, Song Q, 2011, Characterization and kinetics of reduction of CaSO<sub>4</sub> with carbon monoxide for chemical-looping combustion, COMBUSTION AND FLAME, Vol: 158, Pages: 2524-2539, ISSN: 0010-2180
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- Citations: 53
Zhang S, Xiao R, Yang YC, et al., 2011, Pressurized chemical-looping combustion of coal with iron-based industrial wastes as oxygen carrier, Kung Cheng Je Wu Li Hsueh Pao/Journal of Engineering Thermophysics, Vol: 32, Pages: 1073-1076, ISSN: 0253-231X
In this study, pressurized chemical-looping combustion of coal with iron-based industrial wastes and the cyclic durability of the iron-based industrial wastes were investigated in a laboratory fixed bed reactor. The results showed that the pressurized condition suppressed the initial coal pyrolysis process while enhanced the gasification process of coal char and the reaction between gasification products and oxygen carrier. With the increase of pressure, higher concentration of CO2 and carbon conversion and lower concentrations of CO and CH4 were obtained, also the conversion of the oxygen carrier was higher under higher pressure. With the increase of mass ratio of coal to oxygen carrier, the concentration of CO2 and fuel conversion decreased due to the limited oxygen capacity of oxygen carrier, which is not favorable for CO2 capture and the efficient use of energy. The cyclic experiments showed that the reactivity of the oxygen carrier increased with the increase of number of cycles, the conversions of volatile gases and gasification products of coal char increased as well as the fuel conversion.
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