Imperial College London

Prof Andrew G. Livingston

Faculty of EngineeringDepartment of Chemical Engineering

Visiting Professor
 
 
 
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Contact

 

+44 (0)20 7594 5582a.livingston Website

 
 
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Assistant

 

Miss Jessica Baldock +44 (0)20 7594 5699

 
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Location

 

413ACE ExtensionSouth Kensington Campus

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Summary

 

Publications

Publication Type
Year
to

412 results found

Oxley A, Livingston AG, 2024, Effect of polymer molecular weight on the long-term process stability of crosslinked polybenzimidazole organic solvent nanofiltration (OSN) membranes, Journal of Membrane Science, Vol: 689, ISSN: 0376-7388

The importance of polymer molecular weight on the long-term performance of polybenzimidazole (PBI) membranes in organic solvents was investigated. PBI membranes were manufactured from two different polymer molecular weights: the standard molecular weight of PBI polymer, used almost universally across literature for organic solvent stable membranes (∼27,000 g mol-1), and an untested ∼ two-fold higher molecular weight (∼60,000 g mol-1). After crosslinking, all PBI membranes were chemically and mechanically stable. However, during continuous long-term pressurised filtration in DMF, the standard molecular weight PBI membranes suffered slow permeance decline over time. This was attributed to rearrangement of the crosslinked polymer chains. Increasing the extent of crosslinking reduced the rate of membrane permeance decline but did not provide a fully process stable membrane. Using a higher molecular weight PBI, and a similar extent of crosslinking, resulted in a membrane with constant permeance and excellent process stability, even during continuous DMF filtration at 120 °C. This was attributed to the increased interchain interactions and entanglement in the high molecular weight polymer, which reduced the rate of chain rearrangement and compaction. This work demonstrates the importance of polymer molecular weight for reducing membrane compaction and providing process stability in organic solvents.

Journal article

Burke DW, Jiang Z, Livingston AG, Dichtel WRet al., 2024, 2D Covalent Organic Framework Membranes for Liquid-Phase Molecular Separations: State of the Field, Common Pitfalls, and Future Opportunities., Adv Mater, Vol: 36

2D covalent organic frameworks (2D COFs) are attractive candidates for next-generation membranes due to their robust linkages and uniform, tunable pores. Many publications have claimed to achieve selective molecular transport through COF pores, but reported performance metrics for similar networks vary dramatically, and in several cases the reported experiments are inadequate to support such conclusions. These issues require a reevaluation of the literature. Published examples of 2D COF membranes for liquid-phase separations can be broadly divided into two categories, each with common performance characteristics: polycrystalline COF films (most >1 µm thick) and weakly crystalline or amorphous films (most <500 nm thick). Neither category has demonstrated consistent relationships between the designed COF pore structure and separation performance, suggesting that these imperfect materials do not sieve molecules through uniform pores. In this perspective, rigorous practices for evaluating COF membrane structures and separation performance are described, which will facilitate their development toward molecularly precise membranes capable of performing previously unrealized chemical separations. In the absence of this more rigorous standard of proof, reports of COF-based membranes should be treated with skepticism. As methods to control 2D polymerization improve, precise 2D polymer membranes may exhibit exquisite and energy efficient performance relevant for contemporary separation challenges.

Journal article

Oxley A, Livingston AG, 2022, Anti-fouling membranes for organic solvent nanofiltration (OSN) and organic solvent ultrafiltration (OSU): graft modified polybenzimidazole (PBI), JOURNAL OF MEMBRANE SCIENCE, Vol: 662, ISSN: 0376-7388

Journal article

Li S, Dong R, Musteata V-E, Kim J, Rangnekar ND, Johnson JR, Marshall BD, Chisca S, Xu J, Hoy S, McCool BA, Nunes SP, Jiang Z, Livingston AGet al., 2022, Hydrophobic polyamide nanofilms provide rapid transport for crude oil separation, SCIENCE, Vol: 377, Pages: 1555-+, ISSN: 0036-8075

Journal article

Jiang Z, Dong R, Evans AM, Biere N, Ebrahim MA, Li S, Anselmetti D, Dichtel WR, Livingston AGet al., 2022, Aligned macrocycle pores in ultrathin films for accurate molecular sieving, NATURE, Vol: 609, Pages: 58-+, ISSN: 0028-0836

Journal article

Foglia F, Frick B, Nania M, Livingston A, Cabral Jet al., 2022, Multimodal confined water dynamics in reverse osmosis polyamide membranes, Nature Communications, Vol: 13, ISSN: 2041-1723

While polyamide (PA) membranes are widespread in water purification and desalination by reverse osmosis, a molecular-level understanding of the dynamics of both confined water and polymer matrix remains elusive. Despite the dense hierarchical structure of PA membranes formed by interfacial polymerization, previous studies suggest that water diffusion remains largely unchanged with respect to bulk water. Here, we employ neutron spectroscopy to investigate PA membranes under precise hydration conditions, and a series of isotopic contrasts, to elucidate water transport and polymer relaxation, spanning ps-ns timescales, and Å-nm lengthscales. We experimentally resolve, for the first time, the multimodal diffusive nature of water in PA membranes: in addition to (slowed down) translational jump-diffusion, we observe a long-range and a localized mode, whose geometry and timescales we quantify. The PA matrix is also found to exhibit rotational relaxations commensurate with the nanoscale confinement observed in water diffusion. This comprehensive ‘diffusion map’ can anchor molecular and nanoscale simulations, and enable the predictive design of PA membranes with tuneable performance.

Journal article

Oxley A, Gaffney PRJ, Kim D, Marchetti PG, Livingston Aet al., 2022, Graft modification of polybenzimidazole membranes for organic solvent ultrafiltration with scale up to spiral wound modules, JOURNAL OF MEMBRANE SCIENCE, Vol: 647, ISSN: 0376-7388

Journal article

He A, Jiang Z, Wu Y, Hussain H, Rawle J, Briggs ME, Little MA, Livingston AG, Cooper AIet al., 2022, A smart and responsive crystalline porous organic cage membrane with switchable pore apertures for graded molecular sieving, Nature Materials, Vol: 21, Pages: 463-470, ISSN: 1476-1122

Membranes with high selectivity offer an attractive route to molecular separations, where technologies such as distillation and chromatography are energy intensive. However, it remains challenging to fine tune the structure and porosity in membranes, particularly to separate molecules of similar size. Here, we report a process for producing composite membranes that comprise crystalline porous organic cage films fabricated by interfacial synthesis on a polyacrylonitrile support. These membranes exhibit ultrafast solvent permeance and high rejection of organic dyes with molecular weights over 600 g mol-1. The crystalline cage film is dynamic, and its pore aperture can be switched in methanol to generate larger pores that provide increased methanol permeance and higher molecular weight cut-offs (1,400 g mol-1). By varying the water/methanol ratio, the film can be switched between two phases that have different selectivities, such that a single, 'smart' crystalline membrane can perform graded molecular sieving. We exemplify this by separating three organic dyes in a single-stage, single-membrane process.

Journal article

Buzzard K, Hughes C, Lau K, Livingston A, Mir RF, Morrison Set al., 2021, Schemes in Lean, Experimental Mathematics, Vol: 31, Pages: 355-363, ISSN: 1058-6458

We tell the story of how schemes were formalized in three different ways in the Lean theorem prover.

Journal article

Butler EL, Reid B, Luckham PF, Guldin S, Livingston AG, Petit Cet al., 2021, Interparticle Forces of a Native and Encapsulated Metal-Organic Framework and Their Effects on Colloidal Dispersion, ACS APPLIED MATERIALS & INTERFACES, Vol: 13, Pages: 45898-45906, ISSN: 1944-8244

Journal article

Yeo J, Peeva L, Chung S, Gaffney P, Kim D, Luciani C, Tsukanov S, Seibert K, Kopach M, Albericio F, Livingston Aet al., 2021, Liquid Phase Peptide Synthesis via One‐Pot Nanostar Sieving (PEPSTAR), Angewandte Chemie, Vol: 133, Pages: 7865-7874, ISSN: 0044-8249

<jats:title>Abstract</jats:title><jats:p>Herein, a one‐pot liquid phase peptide synthesis featuring iterative addition of amino acids to a “nanostar” support, with organic solvent nanofiltration (OSN) for isolation of the growing peptide after each synthesis cycle is reported. A cycle consists of coupling, Fmoc removal, then sieving out of the reaction by‐products via nanofiltration in a reactor‐separator, or synthesizer apparatus where no phase or material transfers are required between cycles. The three‐armed and monodisperse nanostar facilitates both efficient nanofiltration and real‐time reaction monitoring of each process cycle. This enabled the synthesis of peptides more efficiently while retaining the full benefits of liquid phase synthesis. PEPSTAR was validated initially with the synthesis of enkephalin‐like model penta‐ and decapeptides, then octreotate amide and finally octreotate. The crude purities compared favorably to vendor produced samples from solid phase synthesis.</jats:p>

Journal article

Yeo J, Peeva L, Chung S, Gaffney P, Kim D, Luciani C, Tsukanov S, Seibert K, Kopach M, Albericio F, Livingston Aet al., 2021, Liquid phase peptide synthesis via one‐pot nanostar sieving (PEPSTAR), Angewandte Chemie International Edition, Vol: 60, Pages: 7786-7795, ISSN: 1433-7851

Herein, a one‐pot liquid phase peptide synthesis featuring iterative addition of amino acids to a ‘nanostar’ support, with organic solvent nanofiltration (OSN) for isolation of the growing peptide after each synthesis cycle is reported. A cycle consists of coupling, Fmoc removal, then sieving out of the reaction by‐products via nanofiltration in a reactor‐separator, or synthesizer apparatus where no phase or material transfers are required between cycles. The three‐armed and monodisperse nanostar facilitates both efficient nanofiltration and real‐time reaction monitoring of each process cycle. This enabled the synthesis of peptides more efficiently while retaining the full benefits of liquid phase synthesis. PEPSTAR was validated initially with the synthesis of enkephalin‐like model penta‐ and decapeptides, then octreotate amide and finally octreotate. The crude purities compared favorably to vendor produced samples from solid phase synthesis.

Journal article

Murray K, Livingston A, 2021, TRANSFORMING OLIGONUCLEOTIDE MANUFACTURING, Chimica Oggi/Chemistry Today, Vol: 39, Pages: 32-34, ISSN: 0392-839X

Oligonucleotides, which have already shown success in the treatment of rare diseases, are now being used to treat conditions with much larger patient populations. However, limitations associated with the current state-of-the-art solid-phase manufacturing technology – namely high costs and low capacity – inhibit their true potential. Despite this, oligonucleotide-based drugs are still moving through the R&D pipeline, but their progress will be hindered without an overhaul of the current manufacturing process. An exciting academic, government and industry collaboration is investigating the potential of a novel liquid-phase synthesis technique. This technique – referred to as Nanostar Sieving – circumvents many of the limitations associated with solid-phase oligonucleotide manufacturing, offering a more cost-effective and environmentally sustainable method of manufacturing oligonucleotides at a larger scale.

Journal article

Kim JH, Cook M, Peeva L, Yeo JIN, Bolton LW, Lee YM, Livingston Aet al., 2020, Low energy intensity production of fuel-grade bio-butanol enabled by membrane-based extraction, Energy and Environmental Science, Vol: 13, Pages: 4862-4871, ISSN: 1754-5692

Widespread use of biofuels is inhibited by the significant energy burden of recovering fuel products from aqueous fermentation systems. Here, we describe a membrane-based extraction (perstraction) system for the recovery of fuel-grade biobutanol from fermentation broths which can extract n-butanol with high purity (>99.5%) while using less than 25% of the energy of current technology options. This is achieved by combining a spray-coated thin-film composite membrane with 2-ethyl-1-hexanol as an extractant. The membrane successfully protects the micro-organisms from the extractant, which, although ideal in other respects, is a metabolic inhibitor. In contrast to water, the extractant does not form a heterogeneous azeotrope with n-butanol, and the overall energy consumption of for n-butanol production is 3.9 MJ kg-1, substantially less than other recovery processes (17.0 – 29.4 MJ kg-1). By (a) extracting n-butanol from the fermentation broth without a phase change, (b) breaking the heterogeneous azeotrope relationship (less energy consumption for distillation), and (c) utilizing a small volume ratio of extractant : fermentation broth (1:100, v/v), the need for high energy intensity processes such as pervaporation, gas stripping or liquid-liquid extraction is avoided. The application of this perstraction system to continuous production of higher alcohols is developed and shown to be highly favourable.

Journal article

Thompson KA, Mathias R, Kim D, Kim J, Rangnekar N, Johnson JR, Hoy SJ, Bechis I, Tarzia A, Jelfs KE, McCool BA, Livingston A, Lively RP, Finn MGet al., 2020, N-Aryl-linked spirocyclic polymers for membrane separations of complex hydrocarbon mixtures, Science, Vol: 369, Pages: 310-315, ISSN: 0036-8075

The fractionation of crude-oil mixtures through distillation is a large-scale, energy-intensive process. Membrane materials can avoid phase changes in such mixtures and thereby reduce the energy intensity of these thermal separations. With this application in mind, we created spirocyclic polymers with N-aryl bonds that demonstrated noninterconnected microporosity in the absence of ladder linkages. The resulting glassy polymer membranes demonstrated nonthermal membrane fractionation of light crude oil through a combination of class- and size-based “sorting” of molecules. We observed an enrichment of molecules lighter than 170 daltons corresponding to a carbon number of 12 or a boiling point less than 200°C in the permeate. Such scalable, selective membranes offer potential for the hybridization of energy-efficient technology with conventional processes such as distillation.

Journal article

McGilvery CM, Abellan P, Klosowski MM, Livingston AG, Cabral JT, Ramasse QM, Porter AEet al., 2020, Nanoscale chemical heterogeneity in aromatic polyamide membranes for reverse osmosis applications, ACS Applied Materials & Interfaces, Vol: 12, Pages: 19890-19902, ISSN: 1944-8244

Reverse osmosis membranes are used within the oil and gas industry for seawater desalination on off-shore oilrigs. The membranes consist of three layers of material: a polyester backing layer, a polysulfone support and a polyamide (PA) thin film separating layer. It is generally thought that the PA layer controls ion selectivity within the membrane but little is understood about its structure or chemistry at the molecular scale. This active polyamide layer is synthesized by interfacial polymerization at an organic/aqueous interface between m-phenylenediamine and trimesoyl chloride, producing a highly cross-linked PA polymer. It has been speculated that the distribution of functional chemistry within this layer could play a role in solute filtration. The only technique potentially capable of probing the distribution of functional chemistry within the active PA layer with sufficient spatial and energy resolution is scanning transmission electron microscopy combined with electron energy-loss spectroscopy (STEM-EELS). Its use is a challenge because organic materials suffer beam-induced damage at relatively modest electron doses. Here we show that it is possible to use the N K-edge to map the active layer of a PA film using monochromated EELS spectrum imaging. The active PA layer is 12 nm thick, which supports previous neutron reflectivity data. Clear changes in the fine structure of the C K-edge across the PA films are measured and we use machine learning to assign fine structure at this edge. Using this method, we map highly heterogeneous intensity variations in functional chemistry attributed to N—C═C bonds within the PA. Similarities are found with previous molecular dynamics simulations of PA showing regions with a higher density of amide bonding as a result of the aggregation process at similar length scales. The chemical pathways that can be deduced may offer a clearer understanding of the transport mechanisms through the membrane.

Journal article

Jiang Z, Karan S, Livingston AG, 2020, Membrane Fouling: Does Microscale Roughness Matter?, INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, Vol: 59, Pages: 5424-5431, ISSN: 0888-5885

Journal article

Casanova S, Liu T-Y, Chew Y-MJ, Livingston A, Mattia Det al., 2020, High flux thin-film nanocomposites with embedded boron nitride nanotubes for nanofiltration, JOURNAL OF MEMBRANE SCIENCE, Vol: 597, ISSN: 0376-7388

Journal article

Livingston AG, Jiang Z, 2020, Proteins tailor pore geometry, NATURE MATERIALS, Vol: 19, Pages: 257-258, ISSN: 1476-1122

Journal article

Butler EL, Petit C, Livingston AG, 2020, Poly(piperazine trimesamide) thin film nanocomposite membrane formation based on MIL-101: Filler aggregation and interfacial polymerization dynamics, JOURNAL OF MEMBRANE SCIENCE, Vol: 596, ISSN: 0376-7388

Journal article

Abdulsalam Ebrahim M, Karan S, Livingston AG, 2020, On the influence of salt concentration on the transport properties of reverse osmosis membranes in high pressure and high recovery desalination, Journal of Membrane Science, Vol: 594, ISSN: 0376-7388

In this work, we investigate the effect of varying the concentration of sodium chloride up to 70 g L−1 - equivalent to a recovery of approximately 50% in seawater desalination-on the transport properties of different reverse osmosis membranes. The study was performed using five commercial thin film composite (TFC) membranes and an analogue TFC membrane fabricated via the interfacial reaction of m-phenylenediamine and trimesoyl chloride. The surface properties of the membranes as measured by atomic force microscopy (AFM), zeta potential, and X-ray photoelectron spectroscopy (XPS) are presented. The solution diffusion model coupled with film theory was used to calculate the permeance of water and salt through the membranes, to account for the effect of concentration polarisation. The mass transfer coefficient in the test cells was estimated independently using the dissolution rate of benzoic acid; and was found to be approximately . A linear reduction in salt permeance was observed in some of the RO membranes, while it remained constant for other membranes, including the analogue membrane. All the tested membranes maintained constant water permeance below 45 g L−1 NaCl. However, when the salt concentration at the membrane surface exceeded 45 g L−1, water permeance either increased, remained constant or decreased. The results demonstrate the dependence of water and salt transport on the concentration of sodium chloride at the membrane surface.

Journal article

Livingston A, Trout BL, Horvath IT, Johnson MD, Vaccaro L, Coronas J, Babbitt CW, Zhang X, Pradeep T, Drioli E, Hayler JD, Tam KC, Kappe CO, Fane AG, Szekely Get al., 2020, Challenges and Directions for Green Chemical Engineering-Role of Nanoscale Materials, SUSTAINABLE NANOSCALE ENGINEERING: FROM MATERIALS DESIGN TO CHEMICAL PROCESSING, Editors: Szekely, Livingston, Publisher: ELSEVIER SCIENCE BV, Pages: 1-18, ISBN: 978-0-12-814681-1

Book chapter

Corcos AR, Levato GA, Jiang Z, Evans AM, Livingston AG, Marinas BJ, Dichtel WRet al., 2019, Reducing the Pore Size of Covalent Organic Frameworks in Thin-Film Composite Membranes Enhances Solute Rejection, ACS MATERIALS LETTERS, Vol: 1, Pages: 440-446

Journal article

Szekely G, Livingston A, 2019, Sustainable nanoscale engineering: From materials design to chemical processing, ISBN: 9780128146811

Sustainable Nanoscale Engineering: From Materials Design to Chemical Processing presents the latest on the design of nanoscale materials and their applications in sustainable chemical production processes. The newest achievements of materials science, in particular nanomaterials, opened new opportunities for chemical engineers to design more efficient, safe, compact and environmentally benign processes. These materials include metal-organic frameworks, graphene, membranes, imprinted polymers, polymers of intrinsic microporosity, nanoparticles, and nanofilms, to name a few. Topics discussed include gas separation, CO2 sequestration, continuous processes, waste valorization, catalytic processes, bioengineering, pharmaceutical manufacturing, supercritical CO2 technology, sustainable energy, molecular imprinting, graphene, nature inspired chemical engineering, desalination, and more.

Book

Sultan Z, Graça I, Li Y, Lima S, Peeva LG, Kim D, Ebrahim MAA, Rinaldi R, Livingston Aet al., 2019, Membrane fractionation of liquors from lignin-first biorefining, ChemSusChem, Vol: 12, Pages: 1203-1212, ISSN: 1864-5631

For the purposing of each lignin fraction in the lignin liquors, the development of separation strategies to fractionate the lignin streams by MW ranges constitutes a timely challenge to be tackled. Herein, membrane separation was applied to the refining of lignin streams obtained from a lignin-first biorefining process based on H-transfer reactions catalyzed by Raney Ni, using 2-propanol as a part of the lignin extraction liquor and as an H-donor. A two-stage membrane cascade was considered to separate and concentrate the monophenol-rich fraction from the CUB liquor. Building on the experimental results, an economic evaluation of the potential of membrane separation for the refining of lignin streams was undertaken. The membrane performance represents the bottleneck of the costs associated with the separation process. Accordingly, we present a detailed analysis of future developments in the performance required to debottleneck the utilization of membrane separation for lignin refining.

Journal article

Dong R, Liu R, Gaffney P, Schaepertoens M, Marchetti P, Williams C, Chen R, Livingston Aet al., 2019, Sequence-defined multifunctional polyethers via liquid-phase synthesis with molecular sieving, Nature Chemistry, Vol: 11, Pages: 136-145, ISSN: 1755-4330

Synthetic chemists have devoted tremendous effort towards the production of precision synthetic polymers with defined sequences and specific functions. However, the creation of a general technology that enables precise control over monomer sequence, with efficient isolation of the target polymers, is highly challenging. Here, we report a robust strategy for the production of sequence-defined synthetic polymers through a combination of liquid-phase synthesis and selective molecular sieving. The polymer is assembled in solution with real-time monitoring to ensure couplings proceed to completion, on a three-armed star-shaped macromolecule to maximize efficiency during the molecular sieving process. This approach is applied to the construction of sequence-defined polyethers, with side-arms at precisely defined locations that can undergo site-selective modification after polymerization. Using this versatile strategy, we have introduced structural and functional diversity into sequence-defined polyethers, unlocking their potential for real-life applications in nanotechnology, healthcare and information storage.

Journal article

Dong R, Liu R, Gaffney PRJ, Schaepertoens M, Marchetti P, Williams CM, Chen R, Livingston AGet al., 2019, Author Correction: Sequence-defined multifunctional polyethers via liquid-phase synthesis with molecular sieving, Nature Chemistry, Vol: 11, Pages: 184-184, ISSN: 1755-4330

Correction to: Nature Chemistry https://doi.org/10.1038/s41557-018-0169-6, published online 3 December 2018.

Journal article

Peeva L, Livingston A, 2019, Nanofiltration in the Pharmaceutical and Biopharmaceutical Technology, CURRENT TRENDS AND FUTURE DEVELOPMENTS ON (BIO-) MEMBRANES: MEMBRANE PROCESSES IN THE PHARMACEUTICAL AND BIOTECHNOLOGICAL FIELD, Editors: Basile, Charcosset, Publisher: ELSEVIER SCIENCE BV, Pages: 97-121, ISBN: 978-0-12-813606-5

Book chapter

Butler E, Reid B, Petit C, Luckham P, Livingston A, Guldin Set al., 2018, Extended DLVO interactions of a metal-organic framework: Implications on colloidal dispersion, 256th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nanoscience, Nanotechnology and Beyond, Publisher: AMER CHEMICAL SOC, ISSN: 0065-7727

Conference paper

Dong R, Chen R, Livingston A, 2018, Iterative synthesis of sequence-defined, multifunctional, biocompatible PEGs for biomedical applications, 256th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nanoscience, Nanotechnology and Beyond, Publisher: AMER CHEMICAL SOC, ISSN: 0065-7727

Conference paper

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