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Scientific Papers
Publications citing the applications of openQCM (by Novaetech S.r.l.) instruments and accessories in scientific research.
The list of scientific papers published on the most important journals showing the usage of openQCM in several scientific fields, such as thin film deposition, chemical sensors, biological research and biosensors.
Because of the large number of publications, we are reorganizing everything by subject areas. This will take some time. Thank you for your patience
2024
Astier, Samuel; Johnson, Edwin C; Norvilaite, Oleta; Varlas, Spyridon; Brotherton, Emma E; Sanderson, George; Leggett, Graham J; Armes, Steven P
Controlling Adsorption of Diblock Copolymer Nanoparticles onto an Aldehyde-Functionalized Hydrophilic Polymer Brush via pH Modulation Journal Article
In: Langmuir, 2024.
Abstract | Links | BibTeX | Tags: Adsorption, Copolymers, nanoparticles, openQCM NEXT, QCM-D, Silicon, Solution chemistry
@article{astier2024controlling,
title = {Controlling Adsorption of Diblock Copolymer Nanoparticles onto an Aldehyde-Functionalized Hydrophilic Polymer Brush via pH Modulation},
author = {Samuel Astier and Edwin C Johnson and Oleta Norvilaite and Spyridon Varlas and Emma E Brotherton and George Sanderson and Graham J Leggett and Steven P Armes},
url = {https://pubs.acs.org/doi/full/10.1021/acs.langmuir.3c03392},
doi = {https://doi.org/10.1021/acs.langmuir.3c03392},
year = {2024},
date = {2024-02-06},
urldate = {2024-02-06},
journal = {Langmuir},
publisher = {ACS Publications},
abstract = {Sterically stabilized diblock copolymer nanoparticles with a well-defined spherical morphology and tunable diameter were prepared by RAFT aqueous emulsion polymerization of benzyl methacrylate at 70 °C. The steric stabilizer precursor used for these syntheses contained pendent cis-diol groups, which means that such nanoparticles can react with a suitable aldehyde-functional surface via acetal bond formation. This principle is examined herein by growing an aldehyde-functionalized polymer brush from a planar silicon wafer and studying the extent of nanoparticle adsorption onto this model substrate from aqueous solution at 25 °C using a quartz crystal microbalance (QCM). The adsorbed amount, Γ, depends on both the nanoparticle diameter and the solution pH, with minimal adsorption observed at pH 7 or 10 and substantial adsorption achieved at pH 4. Variable-temperature QCM studies provide strong evidence for chemical adsorption, while scanning electron microscopy images recorded for the nanoparticle-coated brush surface after drying indicate mean surface coverages of up to 62%. This fundamental study extends our understanding of the chemical adsorption of nanoparticles on soft substrates.},
keywords = {Adsorption, Copolymers, nanoparticles, openQCM NEXT, QCM-D, Silicon, Solution chemistry},
pubstate = {published},
tppubtype = {article}
}
Sterically stabilized diblock copolymer nanoparticles with a well-defined spherical morphology and tunable diameter were prepared by RAFT aqueous emulsion polymerization of benzyl methacrylate at 70 °C. The steric stabilizer precursor used for these syntheses contained pendent cis-diol groups, which means that such nanoparticles can react with a suitable aldehyde-functional surface via acetal bond formation. This principle is examined herein by growing an aldehyde-functionalized polymer brush from a planar silicon wafer and studying the extent of nanoparticle adsorption onto this model substrate from aqueous solution at 25 °C using a quartz crystal microbalance (QCM). The adsorbed amount, Γ, depends on both the nanoparticle diameter and the solution pH, with minimal adsorption observed at pH 7 or 10 and substantial adsorption achieved at pH 4. Variable-temperature QCM studies provide strong evidence for chemical adsorption, while scanning electron microscopy images recorded for the nanoparticle-coated brush surface after drying indicate mean surface coverages of up to 62%. This fundamental study extends our understanding of the chemical adsorption of nanoparticles on soft substrates.
2023
Wood, Amelia C; Johnson, Edwin C; Prasad, Ram RR; Sullivan, Mark V; Turner, Nicholas W; Armes, Steven P; Staniland, Sarah S; Foster, Jonathan A
Phage display against two-dimensional metal-organic nanosheets as a new route to highly selective biomolecular recognition surfaces Journal Article
In: 2023.
Abstract | Links | BibTeX | Tags: Biopanning, Metal-organic framwork nanosheets (MONs), openQCM NEXT, peptide, Phage display, Sensing, two-dimensional materials
@article{wood2023phage,
title = {Phage display against two-dimensional metal-organic nanosheets as a new route to highly selective biomolecular recognition surfaces},
author = {Amelia C Wood and Edwin C Johnson and Ram RR Prasad and Mark V Sullivan and Nicholas W Turner and Steven P Armes and Sarah S Staniland and Jonathan A Foster},
url = {https://chemrxiv.org/engage/chemrxiv/article-details/6570ea7c29a13c4d47ce600d},
doi = {https://doi.org/10.26434/chemrxiv-2023-6dhn7},
year = {2023},
date = {2023-12-08},
urldate = {2023-12-08},
abstract = {Peptides are important biomarkers for a range of diseases, however distinguishing different amino-acid sequences using artificial receptors remains a major challenge in biomedical sensing. Here we present a new approach to creating highly selective recognition surfaces using phage display biopanning against metal-organic nanosheets (MONs) and demonstrate their use as the next-generation of biomolecular recognition surfaces. Three MONs (ZIF-7, ZIF-7-NH2 and Hf-BTB-NH2) were chosen as initial targets to demonstrate how simple synthetic modifications can enhance selectivity towards specific amino acid sequences. Each MON system was added to a solution containing every possible combination of 7-residue peptides attached to bacteriophage hosts and the highest affinity binding peptides for each system was identified via successive biopanning rounds. In each case only a single peptide sequence was isolated (YNYRNLL – ZIF-7, NNWWAPA – ZIF-7-NH2 and FTVRDLS – Hf-BTB-NH2). This indicates that these MONs are highly selective, which is attributed to their 2D nanosheet structure. Zeta potential and contact angle measurements were conducted on each MON and combined with calculated properties for the peptide sequences and binding studies to provide insights into the relative importance of electrostatic, hydrophobic and co-ordination bonding interactions. A quartz crystal microbalance (QCM) was used to model phage binding and the Hf-BTB-NH2 MON coated QCM produced a 5-fold higher signal for FTVRDLS functionalised phage compared to phage with generic peptide sequences. Further studies focusing on Hf-BTB-NH2 confirmed that the VRDL sequence was highly conserved, and on-target binding exhibited equilibrium dissociation constants that are comparable to natural recognition materials. Surface plasmon resonance (SPR) studies indicated a 4600-fold higher equilibrium dissociation constant (KD) for FTVRDLS compared to those obtained for off-target sequences, comparable to those of antibodies (KD = 4 x10-10). We anticipate that the highly tunable nature of MONs will enhance our understanding of binding interactions and enable molecular recognition of biomedically important peptides.},
keywords = {Biopanning, Metal-organic framwork nanosheets (MONs), openQCM NEXT, peptide, Phage display, Sensing, two-dimensional materials},
pubstate = {published},
tppubtype = {article}
}
Peptides are important biomarkers for a range of diseases, however distinguishing different amino-acid sequences using artificial receptors remains a major challenge in biomedical sensing. Here we present a new approach to creating highly selective recognition surfaces using phage display biopanning against metal-organic nanosheets (MONs) and demonstrate their use as the next-generation of biomolecular recognition surfaces. Three MONs (ZIF-7, ZIF-7-NH2 and Hf-BTB-NH2) were chosen as initial targets to demonstrate how simple synthetic modifications can enhance selectivity towards specific amino acid sequences. Each MON system was added to a solution containing every possible combination of 7-residue peptides attached to bacteriophage hosts and the highest affinity binding peptides for each system was identified via successive biopanning rounds. In each case only a single peptide sequence was isolated (YNYRNLL – ZIF-7, NNWWAPA – ZIF-7-NH2 and FTVRDLS – Hf-BTB-NH2). This indicates that these MONs are highly selective, which is attributed to their 2D nanosheet structure. Zeta potential and contact angle measurements were conducted on each MON and combined with calculated properties for the peptide sequences and binding studies to provide insights into the relative importance of electrostatic, hydrophobic and co-ordination bonding interactions. A quartz crystal microbalance (QCM) was used to model phage binding and the Hf-BTB-NH2 MON coated QCM produced a 5-fold higher signal for FTVRDLS functionalised phage compared to phage with generic peptide sequences. Further studies focusing on Hf-BTB-NH2 confirmed that the VRDL sequence was highly conserved, and on-target binding exhibited equilibrium dissociation constants that are comparable to natural recognition materials. Surface plasmon resonance (SPR) studies indicated a 4600-fold higher equilibrium dissociation constant (KD) for FTVRDLS compared to those obtained for off-target sequences, comparable to those of antibodies (KD = 4 x10-10). We anticipate that the highly tunable nature of MONs will enhance our understanding of binding interactions and enable molecular recognition of biomedically important peptides.
Milsom, Adam; Qi, Shaojun; Mishra, Ashmi; Berkemeier, Thomas; Zhang, Zhenyu; Pfrang, Christian
In: EGUsphere, vol. 23, iss. 19, pp. 10835–10843, 2023.
Abstract | Links | BibTeX | Tags: aerosol, Dissipation Monitoring, films, openQCM NEXT, Ozone, pollutants, pollution, QCM, QCM-D, Quartz Crystal Microbalance
@article{milsom2023situ,
title = {In-situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a Quartz Crystal Microbalance with Dissipation monitoring (QCM-D)},
author = {Adam Milsom and Shaojun Qi and Ashmi Mishra and Thomas Berkemeier and Zhenyu Zhang and Christian Pfrang},
url = {https://acp.copernicus.org/articles/23/10835/2023/},
doi = {https://doi.org/10.5194/acp-23-10835-2023},
year = {2023},
date = {2023-10-04},
urldate = {2023-10-04},
journal = {EGUsphere},
volume = {23},
issue = {19},
pages = {10835–10843},
publisher = {Copernicus Publications Göttingen, Germany},
abstract = {Aerosols and films are found in indoor and outdoor environments. How they interact with pollutants, such as ozone, has a direct impact on our environment via cloud droplet formation and the chemical persistence of toxic aerosol constituents. The chemical reactivity of aerosol emissions is typically measured spectroscopically or by techniques such as mass spectrometry, directly monitoring the amount of material during a chemical reaction. We present a study which indirectly measures oxidation kinetics in a common cooking aerosol proxy using a low-cost quartz crystal microbalance with dissipation monitoring (QCM-D). We validated this approach by comparison with kinetics measured both spectroscopically and with high-intensity synchrotron radiation. Using microscopy, we found that the film morphology changed and film rigidity increased during oxidation. There was evidence of surface crust formation on oxidised particles, though this was not consistent for all experiments. Crucially, our kinetic modelling of these experimental data confirmed that the oleic acid decay rate is in line with previous literature determinations, which demonstrates that performing such experiments on a QCM-D does not alter the underlying mechanism. There is clear potential to take this robust and low-cost but sensitive method to the field for in situ monitoring of reactions outdoors and indoors.},
keywords = {aerosol, Dissipation Monitoring, films, openQCM NEXT, Ozone, pollutants, pollution, QCM, QCM-D, Quartz Crystal Microbalance},
pubstate = {published},
tppubtype = {article}
}
Aerosols and films are found in indoor and outdoor environments. How they interact with pollutants, such as ozone, has a direct impact on our environment via cloud droplet formation and the chemical persistence of toxic aerosol constituents. The chemical reactivity of aerosol emissions is typically measured spectroscopically or by techniques such as mass spectrometry, directly monitoring the amount of material during a chemical reaction. We present a study which indirectly measures oxidation kinetics in a common cooking aerosol proxy using a low-cost quartz crystal microbalance with dissipation monitoring (QCM-D). We validated this approach by comparison with kinetics measured both spectroscopically and with high-intensity synchrotron radiation. Using microscopy, we found that the film morphology changed and film rigidity increased during oxidation. There was evidence of surface crust formation on oxidised particles, though this was not consistent for all experiments. Crucially, our kinetic modelling of these experimental data confirmed that the oleic acid decay rate is in line with previous literature determinations, which demonstrates that performing such experiments on a QCM-D does not alter the underlying mechanism. There is clear potential to take this robust and low-cost but sensitive method to the field for in situ monitoring of reactions outdoors and indoors.
Zholdassov, Yerzhan
Kinetics of Photochemical and Mechanochemical Organic Reactions on Surface Journal Article
In: 2023.
Abstract | Links | BibTeX | Tags: mechanochemistry, openQCM, openQCM NEXT, photochemistry, QCM-D, surface chemistry
@article{zholdassov2023kinetics,
title = {Kinetics of Photochemical and Mechanochemical Organic Reactions on Surface},
author = {Yerzhan Zholdassov},
url = {https://academicworks.cuny.edu/gc_etds/5476/},
year = {2023},
date = {2023-09-01},
urldate = {2023-09-01},
abstract = {Solvents used in traditional chemical processes account for a large percentage of reaction mass and waste and can pose significant environmental and health risks. The environmentally friendly nature of mechanochemistry, in addition to other benefits, makes it a promising approach for sustainable chemistry over traditional solvent-based methods. However, it is still not a widely adopted method for performing chemical reactions on an industrial scale. This is partially due to the significant challenge associated with understanding the reaction kinetics under mechanochemical conditions. Many variations of scanning probe lithography (SPL) techniques are able to manipulate the organic molecules with precise control over force and position on surfaces, which offer unique opportunity to investigate the mechanochemical reactions at molecular level. Chapter 1 gives a review on recent advances in the application of SPL techniques in studying fundamental questions in mechanochemistry.
Polymer brushes, defined as thin polymer coatings in which individual polymer chains are tethered by one chain end to a solid interface. They are considered as the most powerful tools to interface properties. Potential applications of polymer brush patterns span a wide range from organic light emitting diodes (OLEDs) to membranes for desalination and gas separation, from tissue engineering to protein adsorption, controlled surface wettability and the study of fundamentals of cell biology. A number of controlled/“living” polymerization techniques, in particular those based on radical chemistry have been applied to generate such coatings on various types of substrates. It enables the grafting density, the thickness, and the chemistry of the coating to be manipulated very readily without altering the bulk mechanical properties of biomaterials. Responsive polymer brushes are a category of polymer brushes that are capable of conformational and chemical changes in response to external stimuli. They offer unique opportunities for the control of surface properties due to the precise control of chemical and structural parameters such as the brush thickness, density, chemistry, and architecture. In Chapter 2 we will discuss multiplexed stimuli responsive polymer brushes patterns that contain hidden information within the same area.
In Chapter 3 we apply novel printing platform to investigate the mechanosusceptibility of molecules to the applied mechanical energy. Mechanochemical solvent-free reactions by milling, grinding or other types of mechanical action have emerged as a viable alternative to solution chemistry. Mechanochemistry offers not only a possibility to eliminate the need for bulk solvent use, and reduce the generation of waste, but it also unlocks the door to a different reaction environment in which synthetic strategies, reactions and molecules previously not accessible in solution, can be achieved. We have used elastomeric tip arrays to precisely control the time and force applied between dienes and dienophiles on a surface to determine rate constants, activation energies and activation volumes for four reaction systems.},
key = {surface chemistry, mechanochemistry, photochemistry, openQCM, openQCM NEXT, QCM-D},
keywords = {mechanochemistry, openQCM, openQCM NEXT, photochemistry, QCM-D, surface chemistry},
pubstate = {published},
tppubtype = {article}
}
Solvents used in traditional chemical processes account for a large percentage of reaction mass and waste and can pose significant environmental and health risks. The environmentally friendly nature of mechanochemistry, in addition to other benefits, makes it a promising approach for sustainable chemistry over traditional solvent-based methods. However, it is still not a widely adopted method for performing chemical reactions on an industrial scale. This is partially due to the significant challenge associated with understanding the reaction kinetics under mechanochemical conditions. Many variations of scanning probe lithography (SPL) techniques are able to manipulate the organic molecules with precise control over force and position on surfaces, which offer unique opportunity to investigate the mechanochemical reactions at molecular level. Chapter 1 gives a review on recent advances in the application of SPL techniques in studying fundamental questions in mechanochemistry.
Polymer brushes, defined as thin polymer coatings in which individual polymer chains are tethered by one chain end to a solid interface. They are considered as the most powerful tools to interface properties. Potential applications of polymer brush patterns span a wide range from organic light emitting diodes (OLEDs) to membranes for desalination and gas separation, from tissue engineering to protein adsorption, controlled surface wettability and the study of fundamentals of cell biology. A number of controlled/“living” polymerization techniques, in particular those based on radical chemistry have been applied to generate such coatings on various types of substrates. It enables the grafting density, the thickness, and the chemistry of the coating to be manipulated very readily without altering the bulk mechanical properties of biomaterials. Responsive polymer brushes are a category of polymer brushes that are capable of conformational and chemical changes in response to external stimuli. They offer unique opportunities for the control of surface properties due to the precise control of chemical and structural parameters such as the brush thickness, density, chemistry, and architecture. In Chapter 2 we will discuss multiplexed stimuli responsive polymer brushes patterns that contain hidden information within the same area.
In Chapter 3 we apply novel printing platform to investigate the mechanosusceptibility of molecules to the applied mechanical energy. Mechanochemical solvent-free reactions by milling, grinding or other types of mechanical action have emerged as a viable alternative to solution chemistry. Mechanochemistry offers not only a possibility to eliminate the need for bulk solvent use, and reduce the generation of waste, but it also unlocks the door to a different reaction environment in which synthetic strategies, reactions and molecules previously not accessible in solution, can be achieved. We have used elastomeric tip arrays to precisely control the time and force applied between dienes and dienophiles on a surface to determine rate constants, activation energies and activation volumes for four reaction systems.
Polymer brushes, defined as thin polymer coatings in which individual polymer chains are tethered by one chain end to a solid interface. They are considered as the most powerful tools to interface properties. Potential applications of polymer brush patterns span a wide range from organic light emitting diodes (OLEDs) to membranes for desalination and gas separation, from tissue engineering to protein adsorption, controlled surface wettability and the study of fundamentals of cell biology. A number of controlled/“living” polymerization techniques, in particular those based on radical chemistry have been applied to generate such coatings on various types of substrates. It enables the grafting density, the thickness, and the chemistry of the coating to be manipulated very readily without altering the bulk mechanical properties of biomaterials. Responsive polymer brushes are a category of polymer brushes that are capable of conformational and chemical changes in response to external stimuli. They offer unique opportunities for the control of surface properties due to the precise control of chemical and structural parameters such as the brush thickness, density, chemistry, and architecture. In Chapter 2 we will discuss multiplexed stimuli responsive polymer brushes patterns that contain hidden information within the same area.
In Chapter 3 we apply novel printing platform to investigate the mechanosusceptibility of molecules to the applied mechanical energy. Mechanochemical solvent-free reactions by milling, grinding or other types of mechanical action have emerged as a viable alternative to solution chemistry. Mechanochemistry offers not only a possibility to eliminate the need for bulk solvent use, and reduce the generation of waste, but it also unlocks the door to a different reaction environment in which synthetic strategies, reactions and molecules previously not accessible in solution, can be achieved. We have used elastomeric tip arrays to precisely control the time and force applied between dienes and dienophiles on a surface to determine rate constants, activation energies and activation volumes for four reaction systems.
Hunter, Saul J; Elella, Mahmoud H Abu; Johnson, Edwin C; Taramova, Laura; Brotherton, Emma E; Armes, Steven P; Khutoryanskiy, Vitaliy V; Smallridge, Mark J
Mucoadhesive Pickering Nanoemulsions via Dynamic Covalent Chemistry Journal Article
In: Journal of Colloid and Interface Science, 2023.
Abstract | Links | BibTeX | Tags: Aldehyde-Functionalized Nanoparticles, Mucoadhesive Drug, Nanoemulsions, openQCM NEXT, QCM-D, Quartz Crystal Microbalance
@article{hunter2023mucoadhesive,
title = {Mucoadhesive Pickering Nanoemulsions via Dynamic Covalent Chemistry},
author = {Saul J Hunter and Mahmoud H Abu Elella and Edwin C Johnson and Laura Taramova and Emma E Brotherton and Steven P Armes and Vitaliy V Khutoryanskiy and Mark J Smallridge},
url = {https://www.sciencedirect.com/science/article/pii/S0021979723014200},
doi = {https://doi.org/10.1016/j.jcis.2023.07.162},
year = {2023},
date = {2023-07-27},
urldate = {2023-07-27},
journal = {Journal of Colloid and Interface Science},
publisher = {Elsevier},
abstract = {Hypothesis. Submicron oil droplets stabilized using aldehyde-functionalized nanoparticles should adhere to the primary amine groups present at the surface of sheep nasal mucosal tissue via Schiff base chemistry. Experiments. Well-defined sterically-stabilized diblock copolymer nanoparticles of 20 nm diameter were prepared in the form of concentrated aqueous dispersions via reversible addition-fragmentation chain transfer (RAFT) aqueous emulsion polymerization of 2,2,2-trifluoroethyl methacrylate (TFEMA) using a water-soluble methacrylic precursor bearing cis-diol groups. Some of these hydroxyl-functional nanoparticles were then selectively oxidized using an aqueous solution of sodium periodate to form a second batch of nanoparticles bearing pendent aldehyde groups within the steric stabilizer chains. Subjecting either hydroxyl- or aldehyde-functional nanoparticles to high-shear homogenization with a model oil (squalane) produced oil-in-water Pickering macroemulsions of 20-30 µm diameter. High-pressure microfluidization of such macroemulsions led to formation of the corresponding Pickering nanoemulsions with a mean droplet diameter of around 200 nm. Quartz crystal microbalance (QCM) experiments were used to examine adsorption of both nanoparticles and oil droplets onto a model planar substrate bearing primary amine groups, while a fluorescence microscopy-based mucoadhesion assay was developed to assess adsorption of the oil droplets onto sheep nasal mucosal tissue. Findings. Squalane droplets coated with aldehyde-functional nanoparticles adhered significantly more strongly to sheep nasal mucosal tissue than those coated with the corresponding hydroxyl-functional nanoparticles. This difference was attributed to the formation of surface imine bonds via Schiff base chemistry and was also observed for the two types of nanoparticles alone in QCM studies. Preliminary biocompatibility studies using planaria indicated only mild toxicity for these new mucoadhesive Pickering nanoemulsions, suggesting potential applications for the localized delivery of hydrophobic drugs.},
keywords = {Aldehyde-Functionalized Nanoparticles, Mucoadhesive Drug, Nanoemulsions, openQCM NEXT, QCM-D, Quartz Crystal Microbalance},
pubstate = {published},
tppubtype = {article}
}
Hypothesis. Submicron oil droplets stabilized using aldehyde-functionalized nanoparticles should adhere to the primary amine groups present at the surface of sheep nasal mucosal tissue via Schiff base chemistry. Experiments. Well-defined sterically-stabilized diblock copolymer nanoparticles of 20 nm diameter were prepared in the form of concentrated aqueous dispersions via reversible addition-fragmentation chain transfer (RAFT) aqueous emulsion polymerization of 2,2,2-trifluoroethyl methacrylate (TFEMA) using a water-soluble methacrylic precursor bearing cis-diol groups. Some of these hydroxyl-functional nanoparticles were then selectively oxidized using an aqueous solution of sodium periodate to form a second batch of nanoparticles bearing pendent aldehyde groups within the steric stabilizer chains. Subjecting either hydroxyl- or aldehyde-functional nanoparticles to high-shear homogenization with a model oil (squalane) produced oil-in-water Pickering macroemulsions of 20-30 µm diameter. High-pressure microfluidization of such macroemulsions led to formation of the corresponding Pickering nanoemulsions with a mean droplet diameter of around 200 nm. Quartz crystal microbalance (QCM) experiments were used to examine adsorption of both nanoparticles and oil droplets onto a model planar substrate bearing primary amine groups, while a fluorescence microscopy-based mucoadhesion assay was developed to assess adsorption of the oil droplets onto sheep nasal mucosal tissue. Findings. Squalane droplets coated with aldehyde-functional nanoparticles adhered significantly more strongly to sheep nasal mucosal tissue than those coated with the corresponding hydroxyl-functional nanoparticles. This difference was attributed to the formation of surface imine bonds via Schiff base chemistry and was also observed for the two types of nanoparticles alone in QCM studies. Preliminary biocompatibility studies using planaria indicated only mild toxicity for these new mucoadhesive Pickering nanoemulsions, suggesting potential applications for the localized delivery of hydrophobic drugs.
Malhotra, Jaskaran Singh; Kubus, Mariusz; Pedersen, Kasper Steen; Andersen, Simon Ivar; Sundberg, Jonas
Room-temperature monitoring of CH4 and CO2 using a metal-organic framework-based QCM sensor showing inherent analyte discrimination Journal Article
In: 2023.
Abstract | Links | BibTeX | Tags: carbon dioxide, CH4, CO2, Dissipation, metal-organic frameworks, methane, openQCM NEXT, QCM, QCM-D, Quartz Crystal Microbalance, sensors
@article{malhotra2023room,
title = {Room-temperature monitoring of CH4 and CO2 using a metal-organic framework-based QCM sensor showing inherent analyte discrimination},
author = {Jaskaran Singh Malhotra and Mariusz Kubus and Kasper Steen Pedersen and Simon Ivar Andersen and Jonas Sundberg},
url = {https://chemrxiv.org/engage/chemrxiv/article-details/646b938eccabde9f6e2fd280},
doi = {https://doi.org/10.26434/chemrxiv-2023-djhp2},
year = {2023},
date = {2023-05-24},
urldate = {2023-05-24},
abstract = {The detection of methane and carbon dioxide is of growing importance due to their negative impact on global warming. This is true both for environmental monitoring, as well as leak detection in industrial processes. Although solid-state sensors are technologically mature, they have limitations that prohibit their use in certain situations, e.g., explosive atmospheres. Thus, there is a need to develop new types of sensor materials. Herein, we demonstrate a simple, low-cost metal-organic framework-based gas leak detection sensor. The system is based on gravimetric sensing using a quartz crystal microbalance. The quartz crystal is functionalized by layer-by-layer growth of a thin metal-organic framework film. This film shows selective uptake of methane or carbon dioxide under atmospheric conditions. The hardware has low cost, simple operation, and theoretically high sensitivity. Overall, the sensor is characterized by simplicity and high robustness. Furthermore, by exploiting the different adsorption kinetics as measured by multiple harmonics analyses, it is possible to discriminate whether the response is due to methane or carbon dioxide. In summary, we demonstrate data relevant towards new applications of metal-organic frameworks and microporous hybrid materials in sensing applications.},
keywords = {carbon dioxide, CH4, CO2, Dissipation, metal-organic frameworks, methane, openQCM NEXT, QCM, QCM-D, Quartz Crystal Microbalance, sensors},
pubstate = {published},
tppubtype = {article}
}
The detection of methane and carbon dioxide is of growing importance due to their negative impact on global warming. This is true both for environmental monitoring, as well as leak detection in industrial processes. Although solid-state sensors are technologically mature, they have limitations that prohibit their use in certain situations, e.g., explosive atmospheres. Thus, there is a need to develop new types of sensor materials. Herein, we demonstrate a simple, low-cost metal-organic framework-based gas leak detection sensor. The system is based on gravimetric sensing using a quartz crystal microbalance. The quartz crystal is functionalized by layer-by-layer growth of a thin metal-organic framework film. This film shows selective uptake of methane or carbon dioxide under atmospheric conditions. The hardware has low cost, simple operation, and theoretically high sensitivity. Overall, the sensor is characterized by simplicity and high robustness. Furthermore, by exploiting the different adsorption kinetics as measured by multiple harmonics analyses, it is possible to discriminate whether the response is due to methane or carbon dioxide. In summary, we demonstrate data relevant towards new applications of metal-organic frameworks and microporous hybrid materials in sensing applications.
Maity, Tanmoy; Malik, Pratibha; Bawari, Sumit; Ghosh, Soumya; Mondal, Jagannath; Haldar, Ritesh
Chemically routed interpore molecular diffusion in metal-organic framework thin films Journal Article
In: Nature Communications, vol. 14, no. 1, pp. 2212, 2023.
Abstract | Links | BibTeX | Tags: molecular diffusion, Nanoporous channels, openQCM NEXT, QCM, QCM-D, Quartz Crystal Microbalance
@article{maity2023chemically,
title = {Chemically routed interpore molecular diffusion in metal-organic framework thin films},
author = {Tanmoy Maity and Pratibha Malik and Sumit Bawari and Soumya Ghosh and Jagannath Mondal and Ritesh Haldar},
url = {https://pubmed.ncbi.nlm.nih.gov/37072404/},
doi = {https://doi.org/10.1038/s41467-023-37739-8},
year = {2023},
date = {2023-04-18},
urldate = {2023-04-18},
journal = {Nature Communications},
volume = {14},
number = {1},
pages = {2212},
publisher = {Nature Publishing Group UK London},
abstract = {Transport diffusivity of molecules in a porous solid is constricted by the rate at which molecules move from one pore to the other, along the concentration gradient, i.e. by following Fickian diffusion. In heterogeneous porous materials, i.e. in the presence of pores of different sizes and chemical environments, diffusion rate and directionality remain tricky to estimate and adjust. In such a porous system, we have realized that molecular diffusion direction can be orthogonal to the concentration gradient. To experimentally determine this complex diffusion rate dependency and get insight of the microscopic diffusion pathway, we have designed a model nanoporous structure, metal-organic framework (MOF). In this model two chemically and geometrically distinct pore windows are spatially oriented by an epitaxial, layer-by-layer growth method. The specific design of the nanoporous channels and quantitative mass uptake rate measurements have indicated that the mass uptake is governed by the interpore diffusion along the direction orthogonal to the concentration gradient. This revelation allows chemically carving the nanopores, and accelerating the interpore diffusion and kinetic diffusion selectivity.},
keywords = {molecular diffusion, Nanoporous channels, openQCM NEXT, QCM, QCM-D, Quartz Crystal Microbalance},
pubstate = {published},
tppubtype = {article}
}
Transport diffusivity of molecules in a porous solid is constricted by the rate at which molecules move from one pore to the other, along the concentration gradient, i.e. by following Fickian diffusion. In heterogeneous porous materials, i.e. in the presence of pores of different sizes and chemical environments, diffusion rate and directionality remain tricky to estimate and adjust. In such a porous system, we have realized that molecular diffusion direction can be orthogonal to the concentration gradient. To experimentally determine this complex diffusion rate dependency and get insight of the microscopic diffusion pathway, we have designed a model nanoporous structure, metal-organic framework (MOF). In this model two chemically and geometrically distinct pore windows are spatially oriented by an epitaxial, layer-by-layer growth method. The specific design of the nanoporous channels and quantitative mass uptake rate measurements have indicated that the mass uptake is governed by the interpore diffusion along the direction orthogonal to the concentration gradient. This revelation allows chemically carving the nanopores, and accelerating the interpore diffusion and kinetic diffusion selectivity.
Qi, Shaojun; Kiratzis, Ioannis; Adoni, Pavan; Tuekprakhon, Aekkachai; Hill, Harriet James; Stamataki, Zania; Nabi, Aneesa; Waugh, David; Rodriguez, Javier Rodriguez; Clarke, Stuart Matthew; others,
Porous Cellulose Thin Films as Sustainable and Effective Antimicrobial Surface Coatings Journal Article
In: ACS Applied Materials & Interfaces, 2023.
Abstract | Links | BibTeX | Tags: antimicrobial, cellulose, evaporation, film, openQCM NEXT, QCM, QCM-D, Quartz Crystal Microbalance, robustness, SARS-CoV-2
@article{qi2023porous,
title = {Porous Cellulose Thin Films as Sustainable and Effective Antimicrobial Surface Coatings},
author = {Shaojun Qi and Ioannis Kiratzis and Pavan Adoni and Aekkachai Tuekprakhon and Harriet James Hill and Zania Stamataki and Aneesa Nabi and David Waugh and Javier Rodriguez Rodriguez and Stuart Matthew Clarke and others},
url = {https://pubs.acs.org/doi/full/10.1021/acsami.2c23251},
doi = {https://doi.org/10.1021/acsami.2c23251},
year = {2023},
date = {2023-03-29},
urldate = {2023-01-01},
journal = {ACS Applied Materials & Interfaces},
publisher = {ACS Publications},
abstract = {In the present work, we developed an effective antimicrobial surface film based on sustainable microfibrillated cellulose. The resulting porous cellulose thin film is barely noticeable to human eyes due to its submicrometer thickness, of which the surface coverage, porosity, and microstructure can be modulated by the formulations and the coating process. Using goniometers and a quartz crystal microbalance, we observed a threefold reduction in water contact angles and accelerated water evaporation kinetics on the cellulose film (more than 50% faster than that on a flat glass surface). The porous cellulose film exhibits a rapid inactivation effect against SARS-CoV-2 in 5 min, following deposition of virus-loaded droplets, and an exceptional ability to reduce contact transfer of liquid, e.g., respiratory droplets, to surfaces such as an artificial skin by 90% less than that from a planar glass substrate. It also shows excellent antimicrobial performance in inhibiting the growth of both Gram-negative and Gram-positive bacteria (Escherichia coli and Staphylococcus epidermidis) due to the intrinsic porosity and hydrophilicity. Additionally, the cellulose film shows nearly 100% resistance to scraping in dry conditions due to its strong affinity to the supporting substrate but with good removability once wetted with water, suggesting its practical suitability for daily use. Importantly, the coating can be formed on solid substrates readily by spraying, which requires solely a simple formulation of a plant-based cellulose material with no chemical additives, rendering it a scalable, affordable, and green solution as antimicrobial surface coating. Implementing such cellulose films could thus play a significant role in controlling future pan- and epidemics, particularly during the initial phase when suitable medical intervention needs to be developed and deployed.},
key = {cellulose, film, antimicrobial, evaporation, SARS-CoV-2, robustness},
keywords = {antimicrobial, cellulose, evaporation, film, openQCM NEXT, QCM, QCM-D, Quartz Crystal Microbalance, robustness, SARS-CoV-2},
pubstate = {published},
tppubtype = {article}
}
In the present work, we developed an effective antimicrobial surface film based on sustainable microfibrillated cellulose. The resulting porous cellulose thin film is barely noticeable to human eyes due to its submicrometer thickness, of which the surface coverage, porosity, and microstructure can be modulated by the formulations and the coating process. Using goniometers and a quartz crystal microbalance, we observed a threefold reduction in water contact angles and accelerated water evaporation kinetics on the cellulose film (more than 50% faster than that on a flat glass surface). The porous cellulose film exhibits a rapid inactivation effect against SARS-CoV-2 in 5 min, following deposition of virus-loaded droplets, and an exceptional ability to reduce contact transfer of liquid, e.g., respiratory droplets, to surfaces such as an artificial skin by 90% less than that from a planar glass substrate. It also shows excellent antimicrobial performance in inhibiting the growth of both Gram-negative and Gram-positive bacteria (Escherichia coli and Staphylococcus epidermidis) due to the intrinsic porosity and hydrophilicity. Additionally, the cellulose film shows nearly 100% resistance to scraping in dry conditions due to its strong affinity to the supporting substrate but with good removability once wetted with water, suggesting its practical suitability for daily use. Importantly, the coating can be formed on solid substrates readily by spraying, which requires solely a simple formulation of a plant-based cellulose material with no chemical additives, rendering it a scalable, affordable, and green solution as antimicrobial surface coating. Implementing such cellulose films could thus play a significant role in controlling future pan- and epidemics, particularly during the initial phase when suitable medical intervention needs to be developed and deployed.
