Showing papers in "Annual Review of Chemical and Biomolecular Engineering in 2010"
TL;DR: The origins and applications of stimuli-responsive polymer systems and polymer therapeutics such as polymer-protein and polymer-drug conjugates are reviewed and the latest developments in polymers capable of molecular recognition or directing intracellular delivery are surveyed to illustrate areas of research advancing the frontiers of drug delivery.
Abstract: Polymers have played an integral role in the advancement of drug delivery technology by providing controlled release of therapeutic agents in constant doses over long periods, cyclic dosage, and tunable release of both hydrophilic and hydrophobic drugs. From early beginnings using off-the-shelf materials, the field has grown tremendously, driven in part by the innovations of chemical engineers. Modern advances in drug delivery are now predicated upon the rational design of polymers tailored for specific cargo and engineered to exert distinct biological functions. In this review, we highlight the fundamental drug delivery systems and their mathematical foundations and discuss the physiological barriers to drug delivery. We review the origins and applications of stimuli-responsive polymer systems and polymer therapeutics such as polymer-protein and polymer-drug conjugates. The latest developments in polymers capable of molecular recognition or directing intracellular delivery are surveyed to illustrate areas of research advancing the frontiers of drug delivery.
1,199 citations
TL;DR: This review presents a short delineation of the theory, the application potential and limitations of COSMO-RS, and its most important application areas.
Abstract: The conductor-like screening model for realistic solvation (COSMO-RS) method has been established as a novel way to predict thermophysical data for liquid systems and has become a frequently used alternative to force field-based molecular simulation methods on one side and group contribution methods on the other. Through its unique combination of a quantum chemical treatment of solutes and solvents with an efficient statistical thermodynamics procedure for the molecular surface interactions, it enables the efficient calculation of many properties that other methods can barely predict. This review presents a short delineation of the theory, the application potential and limitations of COSMO-RS, and its most important application areas.
451 citations
TL;DR: This review focuses on recent advances concerning underpinning points and how they affect measurable properties relevant to engineering applications and the role that particle shape plays in affecting dispersion and hence property control.
Abstract: It is well recognized that nanocomposites formed by adding nanoparticles to polymers can have significantly enhanced properties relative to the native polymer. This review focuses on three aspects that are central to the outstanding problem of realizing these promised property improvements. First, we ask if there exist general strategies to control nanoparticle spatial distribution. This is an important question because it is commonly accepted that the nanoparticle dispersion state crucially affects property improvements. Because ideas on macroscale composites suggest that optimizing different properties requires different dispersion states, we next ask if we can predict a priori the particle dispersion and organization state that can optimize one (or more) properties of the resulting nanocomposite. Finally, we examine the role that particle shape plays in affecting dispersion and hence property control. This review focuses on recent advances concerning these underpinning points and how they affect measur...
433 citations
TL;DR: Deoxygenation of biomass derivatives is a requisite step for the production of fuels and chemicals, and strategies are proposed to minimize the consumption of hydrogen from an external source during this process.
Abstract: Lignocellulosic biomass is renewable and cheap, and it has the potential to displace fossil fuels in the production of fuels and chemicals. Biomass-derived carboxylic acids are important compounds that can be used as platform molecules for the production of a variety of important chemicals on a large scale. Lactic acid, a prototypical biomass derivative, and levulinic acid, an important chemical feedstock produced by hydrolysis of waste cellulosic materials, can be upgraded using bifunctional catalysts (those containing metal and acid sites), which allows the integration of several transformations (e.g., oxygen removal and C-C coupling) in a single catalyst bed. This coupling between active sites is beneficial in that it reduces the complexity and cost of the biomass conversion processes. Deoxygenation of biomass derivatives is a requisite step for the production of fuels and chemicals, and strategies are proposed to minimize the consumption of hydrogen from an external source during this process.
322 citations
TL;DR: This review highlights specific examples of ionic liquid applications in catalysis and in separation technologies and the application of ions as working fluids in process machines is introduced.
Abstract: The development of engineering applications with ionic liquids stretches back to the mid-1990s when the first examples of continuous catalytic processes using ionic liquids and the first studies of ionic liquid-based extractions were published. Ever since, the use of ionic liquids has seen tremendous progress in many fields of chemistry and engineering, and the first commercial applications have been reported. The main driver for ionic liquid engineering applications is to make practical use of their unique property profiles, which are the result of a complex interplay of coulombic, hydrogen bonding and van der Waals interactions. Remarkably, many ionic liquid properties can be tuned in a wide range by structural modifications at their cation and anion. This review highlights specific examples of ionic liquid applications in catalysis and in separation technologies. Additionally, the application of ionic liquids as working fluids in process machines is introduced.
300 citations
TL;DR: This review discusses supercritical fluids in industrial and near-to-industry applications that have been applied to mass-transfer processes, phase-transition processes, reactive systems, materials-related processes, and nanostructured materials.
Abstract: This review discusses supercritical fluids in industrial and near-to-industry applications. Supercritical fluids are flexible tools for processing materials. Supercritical fluids have been applied to mass-transfer processes, phase-transition processes, reactive systems, materials-related processes, and nanostructured materials. Some applications are already at industrial capacity, whereas others remain under development. In addition to extraction, application areas include impregnation and cleaning, multistage countercurrent separation, particle formation, coating, and reactive systems such as hydrogenation, biomass gasification, and supercritical water oxidation. Polymers are modified with supercritical fluids, and colloids and emulsions as well as nanostructured materials exhibit interesting phenomena when in contact with supercritical fluids that can be industrially exploited. For these applications to succeed, the properties of supercritical fluids in combination with the materials processed must be clearly determined and fundamental knowledge of the complex behavior must be made readily available.
250 citations
TL;DR: Batteries have powered vehicles for more than a century, but recent advances, especially in lithium-ion (Li-ion) batteries, are bringing a new generation of electric-powered vehicles to the market.
Abstract: Batteries have powered vehicles for more than a century, but recent advances, especially in lithium-ion (Li-ion) batteries, are bringing a new generation of electric-powered vehicles to the market. Key barriers to progress include system cost and lifetime, and derive from the difficulty of making a high-energy, high-power, and reversible electrochemical system. Indeed, although humans produce many mechanical and electrical systems, the number of reversible electrochemical systems is very limited. System costs may be brought down by using cathode materials less expensive than those presently employed (e.g., sulfur or air), but reversibility will remain a key challenge. Continued improvements in the ability to synthesize and characterize materials at desired length scales, as well as to use computations to predict new structures and their properties, are facilitating the development of a better understanding and improved systems. Battery research is a fascinating area for development as well as a key enabler for future technologies, including advanced transportation systems with minimal environmental impact.
249 citations
TL;DR: Techniques developed to guide the self-assembly process in thin films, which permit varying degrees of control over the patterns formed by the microdomains, are reviewed.
Abstract: An attractive “unconventional” lithographic technique to pattern periodic, sub-100 nm features uses self-assembled block copolymer thin films as etch masks. Unfortunately, as-cast films lack the orientational and positional order of the microphase-separated domains that are necessary for many desired applications. Reviewed herein are techniques developed to guide the self-assembly process in thin films, which permit varying degrees of control over the patterns formed by the microdomains. Techniques that can control the out-of-plane order of the microdomains are first summarized. Then, techniques that control the lateral ordering are reviewed, beginning with those that generate large defect-free grains, then those that impart orientational order to the microdomains, and finally those that can control both the orientation and position of individual microdomains. Each technique is summarized with experimental examples and discussions regarding the mechanism of the guided self-assembly process.
135 citations
TL;DR: This review will discuss the developments in the field of transcutaneous immunization in the past decade with special emphasis on disease targets and vaccine delivery technologies and the challenges that need to be overcome.
Abstract: Skin is an immunologically active tissue composed of specialized cells and agents that capture and process antigens to confer immune protection. Transcutaneous immunization takes advantage of the skin immune network by inducing a protective immune response against topically applied antigens. This mode of vaccination presents a novel and attractive approach for needle-free immunization that is safe, noninvasive, and overcomes many of the limitations associated with needle-based administrations. In this review we will discuss the developments in the field of transcutaneous immunization in the past decade with special emphasis on disease targets and vaccine delivery technologies. We will also briefly discuss the challenges that need to be overcome to translate early laboratory successes in transcutaneous immunization into the development of effective clinical prophylactics.
77 citations
TL;DR: This review highlights experiments that have contributed to the elucidation of structure-function relationships in organic electronics and also point to areas in which knowledge of such relationships is still lacking.
Abstract: The field of organic electronics has progressed rapidly in recent years. However, understanding the direct structure-function relationships between the morphology in electrically active layers and the performance of devices composed of these materials has proven difficult. The morphology of active layers in organic electronics is inherently complex, with heterogeneities existing across multiple length scales, from subnanometer to micron and millimeter range. A major challenge still facing the organic electronics community is understanding how the morphology across all of the length scales in active layers collectively determines the device performance of organic electronics. In this review we highlight experiments that have contributed to the elucidation of structure-function relationships in organic electronics and also point to areas in which knowledge of such relationships is still lacking. Such knowledge will lead to the ability to select active materials on the basis of their inherent properties for the fabrication of devices with prespecified characteristics.
76 citations
TL;DR: The biological production of fuels from renewable sources has been regarded as a feasible solution to the energy and environmental problems in the foreseeable future, and the biofuel product spectrum has expanded from ethanol and fatty acid methyl esters to other molecules, such as higher alcohols and alkanes, with more desirable fuel properties.
Abstract: The biological production of fuels from renewable sources has been regarded as a feasible solution to the energy and environmental problems in the foreseeable future. Recently, the biofuel product spectrum has expanded from ethanol and fatty acid methyl esters (biodiesel) to other molecules, such as higher alcohols and alkanes, with more desirable fuel properties. In general, biosynthesis of these fuel molecules can be divided into two phases: carbon chain elongation and functional modification. In addition to natural fatty acid and isoprenoid chain elongation pathways, keto acid-based chain elongation followed by decarboxylation and reduction has been explored for higher alcohol production. Other issues such as metabolic balance, strain robustness, and industrial production process efficiency have also been addressed. These successes may provide both scientific insights into and practical applications toward the ultimate goal of sustainable fuel production.
TL;DR: Volume-related parameters that can be used to compare the proton conductivity of different polymer electrolytes are established and the impact of these phenomena on designing next-generation sulfonated polymers for polymer electrolyte membrane fuel cells is discussed.
Abstract: The proton conductivity of polymer electrolytes is critical for fuel cells and has therefore been studied in significant detail. The conductivity of sulfonated polymers has been linked to material characteristics to elucidate trends. Mass-based measurements based on water uptake and ion exchange capacity are two of the most common material characteristics used to make comparisons between polymer electrolytes, but they have significant limitations when correlated to proton conductivity. These limitations arise in part because different polymers can have significantly different densities and because conduction occurs over length scales more appropriately represented by volume measurements rather than mass. Herein we establish and review volume-related parameters that can be used to compare the proton conductivity of different polymer electrolytes. Morphological effects on proton conductivity are also considered. Finally, the impact of these phenomena on designing next-generation sulfonated polymers for polymer electrolyte membrane fuel cells is discussed.
TL;DR: Biomass to liquid fuel conversion processes that treat biomass primarily as a carbon source and boost liquid fuel production substantially by using supplementary energy that is recovered from solar energy at much higher efficiencies than the biomass itself are reviewed.
Abstract: In a solar economy, sustainably available biomass holds the potential to be an excellent nonfossil source of high energy density transportation fuel. However, if sustainably available biomass cannot supply the liquid fuel need for the entire transport sector, alternatives must be sought. This article reviews biomass to liquid fuel conversion processes that treat biomass primarily as a carbon source and boost liquid fuel production substantially by using supplementary energy that is recovered from solar energy at much higher efficiencies than the biomass itself. The need to develop technologies for an energy-efficient future sustainable transport sector infrastructure that will use different forms of energy, such as electricity, H(2), and heat, in a synergistic interaction with each other is emphasized. An enabling template for such a future transport infrastructure is presented. An advantage of the use of such a template is that it reduces the land area needed to propel an entire transport sector. Also, some solutions for the transition period that synergistically combine biomass with fossil fuels are briefly discussed.
TL;DR: The signaling, patterning, and biomechanical transformations that occur in two well-studied model systems of epithelial folding are reviewed to illustrate both the complexity and modularity of tissue development.
Abstract: The development of multicellular organisms relies on a small set of construction techniques-assembly, sculpting, and folding-that are spatially and temporally regulated in a combinatorial manner to produce the diversity of tissues within the body. These basic processes are well conserved across tissue types and species at the level of both genes and mechanisms. Here we review the signaling, patterning, and biomechanical transformations that occur in two well-studied model systems of epithelial folding to illustrate both the complexity and modularity of tissue development. In particular, we discuss the possibility of a spatial code specifying morphogenesis. To decipher this code, engineers and scientists need to establish quantitative experimental systems and to develop models that address mechanisms at multiple levels of organization, from gene sequence to tissue biomechanics. In turn, quantitative models of embryogenesis can inspire novel methods for creating synthetic organs and treating degenerative tissue diseases.
TL;DR: In this article, a review highlights theoretical and experimental methods that identified force-dependent molecular properties that are central to the biological activity of adhesion proteins, including surface force apparatus, atomic force microscopy, and vesicle-based probes.
Abstract: Cell adhesion to matrix, other cells, or pathogens plays a pivotal role in many processes in biomolecular engineering. Early macroscopic methods of quantifying adhesion led to the development of quantitative models of cell adhesion and migration. The more recent use of sensitive probes to quantify the forces that alter or manipulate adhesion proteins has revealed much greater functional diversity than was apparent from population average measurements of cell adhesion. This review highlights theoretical and experimental methods that identified force-dependent molecular properties that are central to the biological activity of adhesion proteins. Experimental and theoretical methods emphasized in this review include the surface force apparatus, atomic force microscopy, and vesicle-based probes. Specific examples given illustrate how these tools have revealed unique properties of adhesion proteins and their structural origins.
TL;DR: How the immune system recognizes antigens by searching the large space of receptor molecules is described, as well as how the complementary evolution of pathogens that occurs in response to immune system pressure is reviewed.
Abstract: The immune system recognizes a myriad of invading pathogens and their toxic products. It does so with a finite repertoire of antibodies and T cell receptors. We here describe theories that quantify the dynamics of the immune system. We describe how the immune system recognizes antigens by searching the large space of receptor molecules. We consider in some detail the theories that quantify the immune response to influenza and dengue fever. We review theoretical descriptions of the complementary evolution of pathogens that occurs in response to immune system pressure. Methods including bioinformatics, molecular simulation, random energy models, and quantum field theory contribute to a theoretical understanding of aspects of immunity.
TL;DR: To discuss various facets of chemical engineering education, the author proceeding step by step through his own education and career touches on various points concerning the operation of the educational system.
Abstract: To discuss various facets of chemical engineering education, I proceed step by step through my own education and career. In this way, I touch on various points concerning the operation of the educational system that may be of interest to others.