Multifunctional composite hydrogels for bacterial capture, growth/elimination, and sensing applications

Hydrogels are cross-linked networks of hydrophilic polymer chains with a three-dimensional structure. Owing to their unique features, the application of hydrogels for bacterial/antibacterial studies and bacterial infection management has grown in importance in recent years. This trend is likely to continue due to the rise in bacterial infections and antimicrobial resistance. By exploiting their physicochemical characteristics and inherent nature, hydrogels have been developed to achieve bacterial capture and detection, bacterial growth or elimination, antibiotic delivery, or bacterial sensing. Traditionally, the development of hydrogels for bacterial/antibacterial studies has focused on achieving a single function such as antibiotic delivery, antibacterial activity, bacterial growth, or bacterial detection. However, recent studies demonstrate the fabrication of multifunctional hydrogels, where a single hydrogel is capable of performing more than one bacterial/antibacterial function, or composite hydrogels consisting of a number of single functionalized hydrogels, which exhibit bacterial/antibacterial function synergistically. In this review, we first highlight the hydrogel features critical for bacterial studies and infection management. Then, we specifically address unique hydrogel properties, their surface/network functionalization, and their mode of action for bacterial capture, adhesion/growth, antibacterial activity, and bacterial sensing, respectively. Finally, we provide insights into different strategies for developing multifunctional hydrogels and how such systems can help tackle, manage, and understand bacterial infections and antimicrobial resistance. We also note that the strategies highlighted in this review can be adapted to other cell types and are therefore likely to find applications beyond the field of microbiology

Cell-Free Artificial Photosynthesis System

The objective of this research is to create a cell-free artificial platform for harvesting light energy and transforming the energy to organic compounds. In order to achieve this objective, we took the approach of mimicking the photosynthetic processes of a plant leaf and integrating them into a compact system using microfabrication technology. Photosynthesis consists of two parts: light reaction and dark reaction. During the light reaction, light energy is transformed to chemical energy in ATP that is a biological energy source, while during the dark reaction. Carbon dioxide is absorbed and used to synthesize organic compounds such as glucose and fructose. Many scientists had tried to realize artificial photosynthesis for energy harvesting for decades. However, most of the previous systems were simply based on light reaction and produced less desirable energy sources, such as explosive hydrogen gas and unstable electricity. Other works had been reported that combined both light and dark reactions to produce useful organic compounds, but they were all based on utilizing living cells that were difficult to maintain and were not reusable. We developed a cell-free artificial platform conducting both light and dark reactions. To the best of our knowledge, such a device had not been reported so far. This device was able to harvest light energy and transform the energy to organic compounds, mimicking a plant leaf. We envision integrating the "artificial leaves" to create a compact energy harvesting system with a promising efficiency. In order to create an artificial photosynthesis device, we had come up with four specific parts as follows. Part 1: Light reaction was realized in a microfluidic platform that consists of two fluid chambers separated by a planar membrane with embedded proteins that convert light energy into ATP. Four different materials were investigated as potential membrane materials and the optimal (most stable) material was identified through impedance spectroscopy. Since these membrane materials were very soft, it was challenging to integrate them in a microfluidic platform. Diverse support materials and fabrication techniques were investigated to identify the optimal fabrication process. Once the best membrane material was identified and a microfluidic platform was constructed, we would have light-converting proteins embedded in the membrane followed by the evaluation its light reaction performance. Part 2: Dark reaction was realized in another microfluidic platform porous PDMS cubes as gas-liquid interface media. We used porous PDMS as a gas-liquid interface between microfluidic channels to create a "one-way" diffusion path for carbon dioxide. The CO2 transport was evaluated based on pH change and successful CO2 transport would produce precursors (C3 compounds) for glucose production. Part 3: Glucose synthesis and storage unit was developed by mimicking sponge mesophyll found in a leaf (dicotyledons leaf). Chitosan porous structures with interconnected pores were used for this purpose and they were fabricated by lyophilization after casting or 3D printing. Part 4: The circuits for an integrated light reaction platform was designed and simulated. The digital encode/decode of microchip array was simulated. A high-resolution, low-speed analog-to-digital converter was also designed and simulated for ion channel monitoring purpose. While carrying out this research, the following scientific contributions were also made. First, electrochemical property database of planar membranes made of different biomaterials were established. Second, a novel gas-liquid interface was developed for microfluidic platforms using porous PDMS and its performance was thoroughly investigated by on-chip pH measurement. Third, during the study on 3D printing of chitosan porous structure, a mathematical model was established for identifying optimal operational parameters for printing non-Newtonian fluids with a pneumatic printer. This research brought together expertise in advanced manufacturing (MEMS and additive manufacturing), biochemistry and biomaterials, and system control and integration. We envisioned integrating the "artificial leaves" to create a compact energy harvesting system with high efficiency.Ph.D., Mechanical Engineering and Mechanics -- Drexel University, 201

Integration of biologicals and value added nano-materials in seed treatment: aiming for sustainable agriculture / by Rita Choudhary

&nbsp;In order to contribute to the sustainable agricultural systems; the work carried out in this thesis encompasses developing a novel formulation and strategies for seed coating. Optimization and validations of a formulation having various vital components such as biologicals, polymers, fungicides, and nano-nutrients, which may help in building better practices towards sustainable agriculture.<br /

Wearable chemo/bio-sensors for sweat sensing in sports applications: combining micro-fluidics and novel materials

In the last decade, we have witnessed an exponential growth in the area of clinical diagnostic but surprisingly little has been done on the development of wearable chemo/bio-sensors in the field of sports science. In particular, the use of wearable wireless sensors capable of analysing sweat during physical exercise can provide access to new information sources that can be used to optimise and manage athletes’ performance. Lab-on-a-Chip technology provides a fascinating opportunity for the development of such wearable sensors. In this thesis two different colorimetric wearable microfluidic devices for real- time pH sensing were developed and used during athlete training activity. In one case a textile-based microfluidic platform employing cotton capillarity to drive sweat toward the pH sensitive area is presented that avoids the use of bulky fluid handling apparatus, i.e. pumps. The second case presents a wearable micro-fluidic device based on the use of pH responsive ionogels to obtain real-time sweat pH measurements through photo analysis of their colour variation. The thesis also presents the first example of sweat lactate sensing using an organic electrochemical transistor incorporating an ionogel as solid-state electrolyte. In this chapter, optimization of the lactate oxidase stability when dissolved in number of hydrated ionic liquids is investigated. Finally, a new fabrication protocol for paper-based microfluidic technology is presented, which may have important implications for future applications such as low-cost diagnostics and chemical sensing technologies

Development of novel tools for assisted reproductive technologies based on electrically switchable surfaces

A variety of stimuli have been explored in the last few decades to develop dynamic interfaces with biotechnological and biomedical applications, such as biosensors, point of care devices, cell behaviour control and tissue engineering. In this work, the use of an electrical stimulus was explored for the development of a smart switchable surface with the ability to, in an on-demand fashion, expose and conceal progesterone - an ovarian steroid hormone which plays a crucial role as a modulator of sperm function. In this system, an electric potential drives a conformational change in the surface bound peptide moiety with fast response time. Focus was given to the design of a device that could be used in assisted reproductive treatments and grown into a commercially marketable product. Whilst being developed for assessment of sperm quality and fertilizing potential, the application of this system can be widely extended as this approach can be applied to other relevant antigen-antibody systems, which have so far only been evaluated in static conditions. Fabrication of a micropatterned surface was performed and a novel method for orthogonal functionalisation of gold and glass was developed, where gold was functionalised with a polyethylene glycol thiol self-assembled monolayer (SAM) and glass was functionalised with a covalently bound poly-d-lysine layer for sperm cell attachment. In addition to the investigations on SAMs and mixed SAMs formed on gold, silicon and glass substrates, studies with fluospheres were also undertaken. These tools are aimed to be used for further studies with cells, namely the investigation of their response in terms of Ca2+ signalling, a key player in the regulation of sperm function

Synthesis, postsynthetic modification, and investigation of metal-organic frameworks for environmental and biological applications

2018 Fall.Includes bibliographical references.Metal-organic frameworks (MOFs) are unique porous coordination polymers having record-high surface areas, and tunability at both the organic linkers and metal ions. As such, MOFs are advantageous for various applications including electronics, gas adsorption, and separations amongst others. Despite the advantages associated with MOFs, there are several key challenges that must be addressed in order to broadly expand the practicality of these materials. Such challenges include synthetic pitfalls, structural instability, selectivity, and inefficient heterogeneous catalysis. For instance, most MOFs are not stable in moisture-rich environments, which leads to structural collapse even in the open atmosphere. This instability poses a serious limitation for useful applications. In addition, the synthesis of MOF-related ligands is underdeveloped, which can lead to costly or inaccessible materials. To overcome these challenges, one goal of this research is to develop a solution to enhance the kinetic stability of MOFs to water and another is to execute an efficient and cost-effective synthetic strategy to generate the MOFs used herein. CuBTC (copper benzene-1,3,5-tricarboxylate), a commercially available MOF that has been well-studied and designated as having great potential for many applications, undergoes rapid degradation in humid atmospheres. Therefore, a novel synthetic approach was developed to efficiently access NH2BTC on gram-scale. Postsynthetic modification to the amine of the MOF powder material enhances the kinetic stability of the MOF to water. A distinct linear relationship between the number of carbons in the modification and observed water contact angle is described for the first time. This facilitates the first report of reliable access to mixed-ligand frameworks with predictable, calculated wettability and tunable kinetic stability to water. This work is also the first report of functionalizing copper MOFs as well as MOFs containing a benzene-1,3,5-tricarboxylate ligand to alter hydrophobic characteristics. That initial work inspired further exploration of CuNH2BTC as an antibacterial surface when synthetically grown on the surface of carboxymethylated cotton. The resultant material is capable of tunable Cu2+ ion release (via postsynthetic modification) and exceeds current industry standards for antibacterial agents, exhibiting a log-3 or greater reduction in bacteria both on the surface and in solution. As the scientific community continues to explore and understand MOFs, the implementation of these materials for various applications is dramatically increasing. As such, the second part of this research was devoted to applying and manipulating MOFs to better understand the interactions of MOFs with small molecules and ions. The photophysical properties of CuNH2BTC were investigated and specific interactions between anions and metal ions with MOFs were identified, encouraging the strategic design of MOFs to detect target-analytes via changing fluorescence emission properties in dimethylformamide (quenching or enhancing emission intensity or changing emission wavelength). This work provides a prerequisite study towards the development of improved next-generation MOF chemosensors. In addition, the open coordination site of thermodynamically stable porphyrin-based MOFs was exploited for simultaneous heavy metal detection and metal ion removal from aqueous solutions. Lastly, to better understand heterogenous catalysis with MOFs in biologically relevant media water, a 1HNMR method with solvent suppression was implemented and allows for kinetic and mechanistic studies of biologically relevant MOF-catalyzed decomposition of GSNO with thermodynamically stable MOF CuBTTri in H2O and eventually in blood. As a whole this research provides valuable insights as to how MOFs may be strategically designed, manipulated, and utilized for sensing, catalysis, and antibacterial applications

Sewage sludge heavy metal analysis and agricultural prospects for Fiji

Insoluble residues produced in Waste Water Treatment Plants (WWTP) as by products are known as sewage sludge (SS). Land application of SS, particularly in agricultural lands, is becoming an alternative disposal method in Fiji. However, currently there is no legislative framework governing its use. SS together with its high nutrient and organic matter contents, constitutes some undesired pollutants such as heavy metals, which may limit its extensive use. The focus of this study therefore was to determine the total concentrations of Pb, Zn, Cd, Cu, Cr, Ni and Mn in the SS produced at the Kinoya WWTP (Fiji) and in the non-fertile soil amended with the SS at 20, 40, 60, 80% application rates and in the control (100% Soil). The bioavailable heavy metals were also determined as it depicts the true extent of metal contamination. The treatment mixtures were then used to cultivate cabbage plants in which the total heavy metal uptake was investigated. Total Zn (695.6 mg/kg) was present in the highest amounts in the 100% SS (control), followed by Pb (370.9 mg/kg), Mn (35.0 mg/kg), Cu (65.5 mg/kg), Cr (20.5 mg/kg) and finally Cd (13.5 mg/kg) and hence a similar trend was seen in all treatment mixtures. The potential mobility of sludgeborne heavy metals can be classified as Ni > Cu > Cd > Zn > Mn > Cr > Pb. Total metal uptake in plant leaves and stems showed only the bioavailable metals Cu, Cd, Zn and Mn, with maximum uptake occurring in the leaves. Ni, despite being highly mobile was not detected, due to minute concentrations in the SS treatments. Optimum growth occurred in the 20 and 40% SS treatments. However maximum Cu and Mn uptake occurred in the 40% SS treatment thereby making the 20% treatment the most feasible. Furthermore the total and bioavailable metal concentrations observed were within the safe and permitted limits of the EEC and USEPA legislations

The Chemistry of Reticular Framework Nanoparticles: MOF, ZIF, and COF Materials

Nanoparticles have become a vital part of a vast number of established processes and products;they are used as catalysts, in cosmetics, and even by the pharmaceutical industry. Despite this, however, the reliable and reproducible production of functional nanoparticles for specific applications remains a great challenge. In this respect, reticular chemistry provides methods for connecting molecular building blocks to nanoparticles whose chemical composition, structure, porosity, and functionality can be controlled and tuned with atomic precision. Thus, reticular chemistry allows for the translation of the green chemistry principle of atom economy to functional nanomaterials, giving rise to the multifunctional efficiency concept. This principle encourages the design of highly active nanomaterials by maximizing the number of integrated functional units while minimizing the number of inactive components. State-of-the-art research on reticular nanoparticles-metal-organic frameworks, zeolitic imidazolate frameworks, and covalent organic frameworks-is critically assessed and the beneficial features and particular challenges that set reticular chemistry apart from other nanoparticle material classes are highlighted. Reviewing the power of reticular chemistry, it is suggested that the unique possibility to efficiently and straightforwardly synthesize multifunctional nanoparticles should guide the synthesis of customized nanoparticles in the future

Organic Bioelectronics Development in Italy: A Review

In recent years, studies concerning Organic Bioelectronics have had a constant growth due to the interest in disciplines such as medicine, biology and food safety in connecting the digital world with the biological one. Specific interests can be found in organic neuromorphic devices and organic transistor sensors, which are rapidly growing due to their low cost, high sensitivity and biocompatibility. This trend is evident in the literature produced in Italy, which is full of breakthrough papers concerning organic transistors-based sensors and organic neuromorphic devices. Therefore, this review focuses on analyzing the Italian production in this field, its trend and possible future evolutions

Diagnosis and Detection of Viruses Infecting ICRISAT Mandate Crops

Methods for the diagnosis and detection of plant viruses are described in this manual with particular emphasis on detection of important virus diseases of ICRISAT mandate crops. These include protein-based (ELISA and Western immunoblotting) and nucleic acid-based (PCR, RT-PCR and dot-blot hybridization) techniques, and methods for studying plant-virus vector interactions. Though the technology may appear complicated to beginners, every effort has been made to simplify the procedures by providing technical details in a step-wise manner, with description of underlying principles. The techniques described are applicable for the detection of any plant virus in general, albeit suitable modifications made to optimize the performance as per the needs