openQCM – Powered by Novaetech S.r.l
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
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}
}
Okur, Salih; Hashem, Tawheed; Bogdanova, Evgenia; Hodapp, Patrick; Heinke, Lars; Bräse, Stefan; Wöll, Christof
Optimized Detection of Volatile Organic Compounds Utilizing Durable and Selective Arrays of Tailored UiO-66-X SURMOF Sensors Journal Article
In: ACS sensors, 2024.
Abstract | Links | BibTeX | Tags: Adsorption, Liquids, Metal organic frameworks, openQCM Q-1, QCM-D, sensors, Volatile organic compounds
@article{okur2024optimized,
title = {Optimized Detection of Volatile Organic Compounds Utilizing Durable and Selective Arrays of Tailored UiO-66-X SURMOF Sensors},
author = {Salih Okur and Tawheed Hashem and Evgenia Bogdanova and Patrick Hodapp and Lars Heinke and Stefan Bräse and Christof Wöll},
url = {https://pubs.acs.org/doi/abs/10.1021/acssensors.3c01575},
doi = {https://doi.org/10.1021/acssensors.3c01575},
year = {2024},
date = {2024-02-06},
urldate = {2024-01-01},
journal = {ACS sensors},
publisher = {ACS Publications},
abstract = {Metal–organic frameworks (MOFs), with their well-defined and highly flexible nanoporous architectures, provide a material platform ideal for fabricating sensors. We demonstrate that the efficacy and specificity of detecting and differentiating volatile organic compounds (VOCs) can be significantly enhanced using a range of slightly varied MOFs. These variations are obtained via postsynthetic modification (PSM) of a primary framework. We alter the original MOF’s guest adsorption affinities by incorporating functional groups into the MOF linkers, which yields subtle changes in responses. These responses are subsequently evaluated by using machine learning (ML) techniques. Under severe conditions, such as high humidity and acidic environments, sensor stability and lifespan are of utmost importance. The UiO-66-X MOFs demonstrate the necessary durability in acidic, neutral, and basic environments with pH values ranging from 2 to 11, thus surpassing most other similar materials. The UiO-66-NH2 thin films were deposited on quartz-crystal microbalance (QCM) sensors in a high-temperature QCM liquid cell using a layer-by-layer pump method. Three different, highly stable surface-anchored MOFs (SURMOFs) of UiO-66-X obtained via the PSM approach (X: NH2, Cl, and N3) were employed to fabricate arrays suitable for electronic nose applications. These fabricated sensors were tested for their capability to distinguish between eight VOCs. Data from the sensor array were processed using three distinct ML techniques: linear discriminant (LDA), nearest neighbor (k-NN), and neural network analysis methods. The discrimination accuracies achieved were nearly 100% at high concentrations and over 95% at lower concentrations (50–100 ppm).},
keywords = {Adsorption, Liquids, Metal organic frameworks, openQCM Q-1, QCM-D, sensors, Volatile organic compounds},
pubstate = {published},
tppubtype = {article}
}
Chen, Xie
QCM anal`yza nanočástic a molekul Masters Thesis
České vysoké učen'i technické v Praze. Vypočetn'i a informačn'i centrum., 2024.
Abstract | Links | BibTeX | Tags: Cortisol, nanodiamonds, nanoparticles, openQCM Q-1, QCM-D, Quartz Crystal Microbalance
@mastersthesis{chen2024qcm,
title = {QCM anal`yza nanočástic a molekul},
author = {Xie Chen},
url = {https://dspace.cvut.cz/handle/10467/113400},
year = {2024},
date = {2024-01-22},
urldate = {2024-01-22},
school = {České vysoké učen'i technické v Praze. Vypočetn'i a informačn'i centrum.},
abstract = {Sensors based on quartz crystal microbalances (QCM) have dominated research in recent years. They have produced excellent laboratory results in analyzing the mass as well as the conformation of nanoparticles and molecules. The technology is constantly developed and widely used in various fields of chemistry, physics and biology. Here, we investigated a novel concept based on the use of nanodiamonds on QCM and explored the performance of nanodiamonds on QCM sensors, which helps in expanding the application of nanodiamonds in biosensing and exploring their effectiveness in QCM setups. We established a procedure and suitable parameters for the QCM sensor measurement. 5 MHz opensource QCM sensor system was used for building up the sensor assay for detection of cortisol via antigen (Ag)-antibody (Ab) reactions. Optical pictures after each functionalization step as well as scanning electron microscopy (SEM) pictures before and after the experiment were observed and compared. The values of amplitude, phase, resonance frequency, and dissipation were acquired in dry and water environment. The main evaluated QCM parameters were changes in resonance frequency (Δf) and simultaneous changes in QCM energy dissipation (ΔD), corresponding to changes in mass and morphology of the investigated sensor structure. Thereby we identified sensor assay build up, its functioning in dry and water conditions as well as potential issues such as partial release of nanodiamonds during the chemical treatments.
Sensors based on quartz crystal microbalances (QCM) have dominated research in recent years. They have produced excellent laboratory results in analyzing the mass as well as the conformation of nanoparticles and molecules. The technology is constantly developed and widely used in various fields of chemistry, physics and biology. Here, we investigated a novel concept based on the use of nanodiamonds on QCM and explored the performance of nanodiamonds on QCM sensors, which helps in expanding the application of nanodiamonds in biosensing and exploring their effectiveness in QCM setups. We established a procedure and suitable parameters for the QCM sensor measurement. 5 MHz opensource QCM sensor system was used for building up the sensor assay for detection of cortisol via antigen (Ag)-antibody (Ab) reactions. Optical pictures after each functionalization step as well as scanning electron microscopy (SEM) pictures before and after the experiment were observed and compared. The values of amplitude, phase, resonance frequency, and dissipation were acquired in dry and water environment. The main evaluated QCM parameters were changes in resonance frequency (Δf) and simultaneous changes in QCM energy dissipation (ΔD), corresponding to changes in mass and morphology of the investigated sensor structure. Thereby we identified sensor assay build up, its functioning in dry and water conditions as well as potential issues such as partial release of nanodiamonds during the chemical treatments.},
keywords = {Cortisol, nanodiamonds, nanoparticles, openQCM Q-1, QCM-D, Quartz Crystal Microbalance},
pubstate = {published},
tppubtype = {mastersthesis}
}
Stuart, Daniel David
Advancing Label Free Detection Techniques Through Surface Based Sensing and Machine Learning PhD Thesis
University of California, Riverside, 2023.
Abstract | Links | BibTeX | Tags: openQCM, openQCM Q-1, QCM, QCM sensor, QCM-D, SARS-CoV-2
@phdthesis{stuart2023advancing,
title = {Advancing Label Free Detection Techniques Through Surface Based Sensing and Machine Learning},
author = {Daniel David Stuart},
url = {https://escholarship.org/uc/item/2cr290xf},
year = {2023},
date = {2023-12-01},
urldate = {2023-12-01},
school = {University of California, Riverside},
abstract = {High-performing sensors have played a pivotal role in expanding our understanding of biological systems, disease diagnosis, environmental monitoring, and national security. The technical capability they provide has enabled us to obtain in-depth information and insights towards improving human health. One area of sensing that exemplifies this progress is the development of label free sensors which allow direct analysis of molecular interactions. Among these methods surface plasmon resonance (SPR) has emerged as a powerful, real-time detection technique for studies of biological interactions, drug discovery, and other important aspects that lead to new disease diagnosis. Through the implementation of new materials and methods SPR and other label-free sensors have expanded the range of analytes tested. This Dissertation aims to establish improvements in materials and methodologies through technology advancement for solving current sensor limitations. The work focuses on enhancing sensing signal while limiting the impact of nonspecific interactions on label-free methods, providing expanded molecular identity information, and overcoming challenges encountered when detecting small molecules. Chapters 2, 3, and 4 demonstrate advancements in unique biomimetic surfaces to enable the exploration of new biological systems as well as block nonspecific interactions. Chapter 2 focuses on a tethered membrane system to promote incorporation of relevant constituents into lipid bilayers without compromising membrane mobility property and drug delivery interactions. Chapter 3 employs a charged membrane to suppress nonspecific interactions and explores the working mechanism. Chapter 4 expands the capabilities of label-free sensing systems through development of curved membrane platforms that mitigate the decay limits through modeling of lipid distribution in vesicles. Chapter 5 exploits the plasmonic properties of SPR chips to enhance signals in matrix assisted laser desorption ionization mass spectrometry (MALDI-MS) , which is further facilitated with development of machine learning models to identify bacterial species. In Chapter 6, the limitation of small molecule analysis with SPR is tackled by taking advantage of pressure effects to provide specific gas sensing. Each of these Chapters provides novel advancements in sensing capabilities by addressing performance-impairing limitations in label-free sensors. Research goals are achieved both from improvements to SPR systems and incorporation of other methodologies to augment SPR results.},
keywords = {openQCM, openQCM Q-1, QCM, QCM sensor, QCM-D, SARS-CoV-2},
pubstate = {published},
tppubtype = {phdthesis}
}
Forinová, Michala; Seidlová, Anna; Pilipenco, Alina; Jr, N Scott Lynn; Obořilová, Radka; Farka, Zdeněk; Skládal, Petr; Saláková, Alena; Spasovová, Monika; Houska, Milan; others,
In: Current Research in Biotechnology, pp. 100166, 2023.
Abstract | Links | BibTeX | Tags: Antifouling coating, biosensors, Cultivation-based methods, openQCM Q-1, QCM-D, Quartz Crystal Microbalance, S. aureus
@article{forinova2023comparative,
title = {A Comparative Assessment of a Piezoelectric Biosensor Based on a New Antifouling Nanolayer and Cultivation Methods: Enhancing S. aureus Detection in Fresh Dairy Products},
author = {Michala Forinová and Anna Seidlová and Alina Pilipenco and N Scott Lynn Jr and Radka Obořilová and Zdeněk Farka and Petr Skládal and Alena Saláková and Monika Spasovová and Milan Houska and others},
url = {https://www.sciencedirect.com/science/article/pii/S2590262823000485},
doi = {https://doi.org/10.1016/j.crbiot.2023.100166},
year = {2023},
date = {2023-11-23},
urldate = {2023-11-23},
journal = {Current Research in Biotechnology},
pages = {100166},
publisher = {Elsevier},
abstract = {Ensuring dairy product safety demands rapid and precise Staphylococcus aureus (S. aureus) detection. Biosensors show promise, but their performance is often demonstrated in model samples using non-native pathogens and has never been studied towards S. aureus detection in naturally contaminated samples. This study addresses the gap by directly comparing results taken with a novel piezoelectric biosensor, capable of one-step detection, with four conventional cultivation-based methods. Our findings reveal that this biosensor, based on an antifouling nanolayer-coated biochip, exhibits exceptional resistance to biofouling from unprocessed dairy products and is further capable of specific S. aureus detection. Notably, it performed comparably to Petrifilm and Baird-Parker methods but delivered results in only 30 min, bringing a substantial reduction from the 24 h required by cultivation-based techniques. Our study also highlights differences in the performance of cultivation methods when analyzing artificially spiked versus naturally contaminated foods. These findings underline the potential of antifouling biosensors as efficient reliable tools for rapid, cost-effective, point-of-care testing, enhancing fresh dairy product safety and S. aureus detection.},
keywords = {Antifouling coating, biosensors, Cultivation-based methods, openQCM Q-1, QCM-D, Quartz Crystal Microbalance, S. aureus},
pubstate = {published},
tppubtype = {article}
}
Khoirudin, Hanif; Aflaha, Rizky; Arsetiyani, Eldiana Rully; Nugraheni, Ari Dwi; Nurputra, Dian Kesumapramudya; Triyana, Kuwat; Kusumaatmaja, Ahmad
Influence of the SMN antibody on quartz crystal microbalance with dissipation (QCM-D) surface as an SMN protein biosensor Journal Article
In: MRS Communications, pp. 1–7, 2023.
Abstract | BibTeX | Tags: antibody detection, Nanofiber, Nanofibers, neuron, openQCM, protein, QCM-D, Quartz Crystal Microbalance, SEM
@article{khoirudin2023influence,
title = {Influence of the SMN antibody on quartz crystal microbalance with dissipation (QCM-D) surface as an SMN protein biosensor},
author = {Hanif Khoirudin and Rizky Aflaha and Eldiana Rully Arsetiyani and Ari Dwi Nugraheni and Dian Kesumapramudya Nurputra and Kuwat Triyana and Ahmad Kusumaatmaja},
year = {2023},
date = {2023-11-06},
urldate = {2023-01-01},
journal = {MRS Communications},
pages = {1--7},
publisher = {Springer},
abstract = {The lack of survival motor neuron (SMN) protein levels can lead to spinal muscular atrophy (SMA) disease. In this study, an SMN protein biosensor based on quartz crystal microbalance with dissipation (QCM-D) was developed. The sensor was coated with polyvinyl alcohol (PVA) nanofiber and doped with SMN antibodies to increase the sensitivity. Scanning electron microscope (SEM) images showed that the nanofiber was undamaged after doping the SMN antibody. The sensitivity of the QCM-D sensor was 21.2 Hz/% after doping SMN antibodies and had good stability for 3 days. Moreover, the sensor has been validated using western blot. Thus, the fabricated QCM-D-based biosensor has excellent potential in detecting SMN levels in human blood plasma.},
key = {QCM-D, openQCM, Quartz Crystal Microbalance, neuron, protein, antibodies, nanofiber, SEM},
keywords = {antibody detection, Nanofiber, Nanofibers, neuron, openQCM, protein, QCM-D, Quartz Crystal Microbalance, SEM},
pubstate = {published},
tppubtype = {article}
}
Armutcu, Canan; Karasu, Tunca; Pişkin, Sena; Özgür, Erdoğan; Uzun, Lokman
Selective Aptasensor for Trinitrotoluene Detection: Comparison of the Detecting Performances from Liquid and Vapor Phases Journal Article
In: Colloids and Surfaces A: Physicochemical and Engineering Aspects, pp. 132258, 2023.
Abstract | Links | BibTeX | Tags: aptasensor, explosive detection, openQCM Q-1, openQCM sensors, QCM-D, TNT
@article{armutcu2023selective,
title = {Selective Aptasensor for Trinitrotoluene Detection: Comparison of the Detecting Performances from Liquid and Vapor Phases},
author = {Canan Armutcu and Tunca Karasu and Sena Pişkin and Erdoğan Özgür and Lokman Uzun},
url = {https://www.sciencedirect.com/science/article/abs/pii/S0927775723013420},
doi = {https://doi.org/10.1016/j.colsurfa.2023.132258},
year = {2023},
date = {2023-11-05},
urldate = {2023-11-05},
journal = {Colloids and Surfaces A: Physicochemical and Engineering Aspects},
pages = {132258},
publisher = {Elsevier},
abstract = {In general, chromatographic and sensor analyses have been utilized for explosive detection. The main interest on those systems is to develop a method to selectively detect explosives at a single step as well as from vapor phase if possible. Moreover, on-site and real-time detection with portable systems is another challenge for the researchers. On the other hand, the detection of 2,4,6-trinitrotoluene (TNT) vapor at the crime scene, preferably before the explosion is highly demanded in order to prevent the negative effects of terrorism and to ensure the safety of the civilian population. In this study, initially, Quartz Crystal Microbalance (QCM) sensor was prepared for real-time monitoring of TNT in aqueous solution, through the attachment of TNT peptide aptamer on the gold surface of QCM sensor. Secondly, after providing optimum conditions, TNT detection was investigated even from vapor phase through the QCM aptasensor. According to results, the selectivity coefficient of QCM-based aptasensor was calculated as 6.78 for TNT in respect to DNT whereas that was calculated as 9.02 for TNT in respect to TNB. In addition, the evaluation of the reusability and storage stability emphasized that the sensor could be used repeatedly without significant reduction in dissipation (∆D) values. The linearity coefficient (R2) was found to be 0.9965. The limit of detection (LOD) and the limit of quantitation (LOQ) were determined as 0.0238 and 0.0739 nM, respectively. The studies demonstrated that the portable QCM sensor decorated with the aptamer selective for TNT molecules could be classified as a promising alternative, selective, cost-friendly, easy-to-prepare, ready-to-use, and applicable for on-site and real-time explosive measurements (even from vapor phase).},
key = {openQCM Q-1, QCM-D, openQCM sensors, explosive detection, TNT, aptasensor},
keywords = {aptasensor, explosive detection, openQCM Q-1, openQCM sensors, QCM-D, TNT},
pubstate = {published},
tppubtype = {article}
}
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}
}
Neville, George M; Dobre, Ana-Maria; Smith, Gavin J; Micciulla, Samantha; Brooks, Nick J; Arnold, Thomas; Welton, Tom; Edler, Karen J
Interactions of Choline and Geranate (CAGE) and Choline Octanoate (CAOT) Deep Eutectic Solvents with Lipid Bilayers Journal Article
In: Advanced Functional Materials, pp. 2306644, 2023.
Abstract | Links | BibTeX | Tags: Choline, Choline Octanoate, geranic acid, openQCM Q-1, QCM, QCM-D
@article{neville2023interactions,
title = {Interactions of Choline and Geranate (CAGE) and Choline Octanoate (CAOT) Deep Eutectic Solvents with Lipid Bilayers},
author = {George M Neville and Ana-Maria Dobre and Gavin J Smith and Samantha Micciulla and Nick J Brooks and Thomas Arnold and Tom Welton and Karen J Edler},
url = {https://onlinelibrary.wiley.com/doi/full/10.1002/adfm.202306644},
doi = {https://doi.org/10.1002/adfm.202306644},
year = {2023},
date = {2023-10-02},
urldate = {2023-10-02},
journal = {Advanced Functional Materials},
pages = {2306644},
publisher = {Wiley Online Library},
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.},
key = {Choline, Choline Octanoate, geranic acid, openQCM Q-1, QCM, QCM-D},
keywords = {Choline, Choline Octanoate, geranic acid, openQCM Q-1, QCM, QCM-D},
pubstate = {published},
tppubtype = {article}
}
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}
}
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}
}
Wang, Xinati; Lamantia, Angelo; Jay, Michael; Sadeghi, Hatef; Lambert, Colin J; Kolosov, Oleg V; Robinson, Benjamin
Determination of electric and thermoelectric properties of molecular junctions by AFM in peak force tapping mode Journal Article
In: Nanotechnology, 2023.
Abstract | Links | BibTeX | Tags: Functional Theory (DFT) Calculations, Molecular Thin Films, openQCM, openQCM Q-1, QCM, QCM-D, Self-Assembled Monolayers (SAMs)
@article{wang2023determination,
title = {Determination of electric and thermoelectric properties of molecular junctions by AFM in peak force tapping mode},
author = {Xinati Wang and Angelo Lamantia and Michael Jay and Hatef Sadeghi and Colin J Lambert and Oleg V Kolosov and Benjamin Robinson},
url = {https://iopscience.iop.org/article/10.1088/1361-6528/acdf67/meta},
doi = {https://doi.org/10.1088/1361-6528/acdf67},
year = {2023},
date = {2023-06-19},
urldate = {2023-06-19},
journal = {Nanotechnology},
abstract = {Molecular thin films, such as self-assembled monolayers (SAMs), offer the possibility of translating the optimised thermophysical and electrical properties of high-Seebeck-coefficient single molecules to scalable device architectures. However, for many scanning probe-based approaches attempting to characterise such SAMs, there remains a significant challenge in recovering single-molecule equivalent values from large-area films due to the intrinsic uncertainty of the probe-sample contact area coupled with film damage caused by contact forces. Here we report a new reproducible non-destructive method for probing the electrical and thermoelectric properties of small assemblies (10 – 103) of thiol-terminated molecules arranged within a SAM on a gold surface, and demonstrate the successful and reproducible measurements of the equivalent single-molecule electrical conductivity and Seebeck values. We have used a modified thermal-electric force microscopy (TEFM) approach, which integrates the conductive-probe atomic force microscope, a sample positioned on a temperature-controlled heater, and a probe-sample peak-force feedback that interactively limits the normal force across the molecular junctions. The experimental results are interpreted by density functional theory calculations allowing quantification the electrical quantum transport properties of both single molecules and small clusters of molecules. Significantly, this approach effectively eliminates lateral forces between probe and sample, minimising disruption to the SAM while enabling simultaneous mapping of the SAMs nanomechanical properties, as well as electrical and/or thermoelectric response, thereby allowing correlation of the film properties.},
keywords = {Functional Theory (DFT) Calculations, Molecular Thin Films, openQCM, openQCM Q-1, QCM, QCM-D, Self-Assembled Monolayers (SAMs)},
pubstate = {published},
tppubtype = {article}
}
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}
}
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}
}
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}
}
György, Dr. Csilla; Kirkman, Dr. Paul M.; Neal, Dr. Thomas J.; Chan, Dr. Derek H. H.; Williams, Megan; Smith, Dr. Timothy; Growney, Dr. David J.; Armes, Prof. Steven P.
Enhanced Adsorption of Epoxy-Functional Nanoparticles onto Stainless Steel Significantly Reduces Friction in Tribological Studies Journal Article
In: Angewandte Chemie International Edition, 2023.
Abstract | Links | BibTeX | Tags: epoxy-functional noparticles, nanoparticles, polymerization, polymerization-induced, QCM-D, Quartz Crystal Microbalance, RAFT, self-assembly, stainless steel
@article{armesenhanced,
title = {Enhanced Adsorption of Epoxy-Functional Nanoparticles onto Stainless Steel Significantly Reduces Friction in Tribological Studies},
author = {Dr. Csilla György and Dr. Paul M. Kirkman and Dr. Thomas J. Neal and Dr. Derek H. H. Chan and Megan Williams and Dr. Timothy Smith and Dr. David J. Growney and Prof. Steven P. Armes},
url = {https://onlinelibrary.wiley.com/doi/10.1002/anie.202218397},
doi = {https://doi.org/10.1002/anie.202218397},
year = {2023},
date = {2023-01-18},
urldate = {2023-01-18},
journal = {Angewandte Chemie International Edition},
publisher = {Wiley Online Library},
abstract = {Epoxy-functional sterically-stabilized diblock copolymer nanoparticles (~27 nm) are prepared via RAFT dispersion polymerization in mineral oil. Nanoparticle adsorption onto stainless steel is examined using a quartz crystal microbalance. Incorporating epoxy groups within the steric stabilizer chains results in a near two-fold increase in the adsorbed amount, Γ, at 20 °C (7.6 mg m-2) compared to epoxy-core functional nanoparticles (3.7 mg m-2) or non-functional nanoparticles (3.8 mg m-2). A larger difference in Γ is observed at 40 °C; this suggests chemical adsorption of the nanoparticles rather than merely physical adsorption. A remarkable near five-fold increase in Γ is observed for larger (~50 nm) epoxy-functional nanoparticles compared to non-functional nanoparticles (31.3 vs. 6.4 mg m-2, respectively). Tribological studies conducted at 60-120 °C confirm that the adsorption of epoxy-functional nanoparticles leads to a significant reduction in the friction coefficient.},
key = {QCM-D, nanoparticles},
keywords = {epoxy-functional noparticles, nanoparticles, polymerization, polymerization-induced, QCM-D, Quartz Crystal Microbalance, RAFT, self-assembly, stainless steel},
pubstate = {published},
tppubtype = {article}
}
Avila-Sierra, Alejandro; Moreno, Jose A; Goode, Kylee; Zhu, Taotao; Fryer, Peter J; Taylor, Alan; Zhang, Zhenyu J
Effects of structural and chemical properties of surface coatings on the adsorption characteristics of proteins Journal Article
In: Surface and Coatings Technology, pp. 129054, 2022.
Abstract | Links | BibTeX | Tags: absorption, AFM, Functionalized coatings, protein, Protein adsorption, QCM-D, Structured surfaces
@article{avila2022effects,
title = {Effects of structural and chemical properties of surface coatings on the adsorption characteristics of proteins},
author = {Alejandro Avila-Sierra and Jose A Moreno and Kylee Goode and Taotao Zhu and Peter J Fryer and Alan Taylor and Zhenyu J Zhang},
url = {https://www.sciencedirect.com/science/article/pii/S0257897222009756},
doi = {https://doi.org/10.1016/j.surfcoat.2022.129054},
year = {2022},
date = {2022-01-01},
urldate = {2022-01-01},
journal = {Surface and Coatings Technology},
pages = {129054},
publisher = {Elsevier},
abstract = {Using Quartz Crystal Microbalance with Dissipation (QCM-D) and Atomic Force Microscopy (AFM), a series of functional surface coatings were investigated to establish the effects of surface structural and chemical properties on the adsorption characteristics of two model proteins, β-Lactoglobulin (β-Lg) and Bovine Serum Albumin (BSA). We show that a free contact scenario, e.g., droplet, that is widely used to evaluate surface energy, is not always equivalent to biofouling conditions where the liquid phase is continuous - releasing the entrapped air from surface geometries could influence the interfacial adsorption process of biomolecules. We observed that surface structuration favoured adsorption of both proteins, especially for the protein of smaller size (β-Lg) as larger amounts of molecules would be required to fill surface geometries. Compact proteinaceous adlayers were observed on the coatings without structure, particularly those containing -CF3 ligands, suggesting stronger adhesion mechanisms due to conformational reorientations of both proteins to facilitate surface binding, especially BSA. In contrast, surface structure led to the formation of soft adlayers as the filling of surface cavities might affect protein conformation and favour protein superposition, hindering removal. We demonstrate how protein-surface binding affinity and packaging density of adsorbed proteins can be modulated as a synergistic effect of surface chemistry and structure, which is of especially importance to the development of anti-fouling coatings.},
key = {Protein adsorption, Functionalized coatings, Structured surfaces, QCM-D, AFM},
keywords = {absorption, AFM, Functionalized coatings, protein, Protein adsorption, QCM-D, Structured surfaces},
pubstate = {published},
tppubtype = {article}
}
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