Annual review of chemical and biomolecular engineering最新文献

The prediction of the crystal structures that a given organic molecule is likely to form is an important theoretical problem of significant interest for the pharmaceutical and agrochemical industries, among others. As evidenced by a series of six blind tests organized over the past 2 decades, methodologies for crystal structure prediction (CSP) have witnessed substantial progress and have now reached a stage of development where they can begin to be applied to systems of practical significance. This article reviews the state of the art in general-purpose methodologies for CSP, placing them within a common framework that highlights both their similarities and their differences. The review discusses specific areas that constitute the main focus of current research efforts toward improving the reliability and widening applicability of these methodologies, and offers some perspectives for the evolution of this technology over the next decade.

There is considerable interest in the development of hybrid organic-inorganic materials because of the potential for harvesting the unique capabilities that each system has to offer. Proteins are an especially attractive organic component owing to the high amount of chemical information encoded in their amino acid sequence, their amenability to molecular and computational (re)design, and the many structures and functions they specify. Genetic installation of solid-binding peptides (SBPs) within protein frameworks affords control over the position and orientation of adhesive and morphogenetic segments, and a path toward predictive synthesis and assembly of functional materials and devices, all while harnessing the built-in properties of the host scaffold. Here, we review the current understanding of the mechanisms through which SBPs bind to technologically relevant interfaces, with an emphasis on the variables that influence the process, and highlight the last decade of progress in the use of solid-binding proteins for hybrid and hierarchical materials synthesis.

I review my career from its academic beginning to my recent retirement. I grew up and studied chemical engineering in New York City. My initial failure to understand thermodynamics the way it had been taught, evidenced by the difficulty I had when starting graduate school, led me years later to write a textbook on the subject that is now in a fifth edition, in addition to other books I have written. My research areas have included molecular simulation, statistical- and quantum mechanical-based methods, and a variety of experimental thermodynamic measurements. In addition, I have been a consultant in traditional chemical engineering areas, as well in nontraditional areas, such as assisting in the design of a heat shield for interplanetary exploration, the destruction of armed chemical weapons, and the cleanup of nuclear weapons production facilities.

Since its first appearance in the 1960s, solid support-free liquid-liquid chromatography has played an ever-growing role in the field of natural products research. The use of the two phases of a liquid biphasic system, the mobile and stationary phases, renders the technique highly versatile and adaptable to a wide spectrum of target molecules, from hydrophobic to highly polar small molecules to proteins. Generally considered a niche technique used only for small-scale preparative separations, liquid-liquid chromatography currently lags far behind conventional liquid-solid chromatography and liquid-liquid extraction in process modeling and industrial acceptance. This review aims to expose a broader audience to this high-potential separation technique by presenting the wide variety of available operating modes and solvent systems as well as structured, model-based design approaches. Topics currently offering opportunities for further investigation are also addressed.

CO₂ storage in saline aquifers offers a realistic means of achieving globally significant reductions in greenhouse gas emissions at the scale of billions of tonnes per year. We review insights into the processes involved using well-documented industrial-scale projects, supported by a range of laboratory analyses, field studies, and flow simulations. The main topics we address are (a) the significant physicochemical processes, (b) the factors limiting CO₂ storage capacity, and (c) the requirements for global scale-up.Although CO₂ capture and storage (CCS) technology can be considered mature and proven, it requires significant and rapid scale-up to meet the objectives of the Paris Climate Agreement. The projected growth in the number of CO₂ injection wells required is significantly lower than the historic petroleum industry drill rates, indicating that decarbonization via CCS is a highly credible and affordable ambition for modern human society. Several technology developments are needed to reduce deployment costs and to stimulate widespread adoption of this technology, and these should focus on demonstration of long-term retention and safety of CO₂ storage and development of smart ways of handling injection wells and pressure, cost-effective monitoring solutions, and deployment of CCS hubs with associated infrastructure.

Magnetic nanoparticles are of interest for biomedical applications because of their biocompatibility, tunable surface chemistry, and actuation using applied magnetic fields. Magnetic nanoparticles respond to time-varying magnetic fields via physical particle rotation or internal dipole reorientation, which can result in signal generation or conversion of magnetic energy to heat. This dynamic magnetization response enables their use as tracers in magnetic particle imaging (MPI), an emerging biomedical imaging modality in which signal is quantitative of tracer mass and there is no tissue background signal or signal attenuation. Conversion of magnetic energy to heat motivates use in nanoscale thermal cancer therapy, magnetic actuation of drug release, and rapid rewarming of cryopreserved organs. This review introduces basic concepts of magnetic nanoparticle response to time-varying magnetic fields and presents recent advances in the field, with an emphasis on MPI and conversion of magnetic energy to heat.

Detailed analysis of textural properties, e.g., pore size and connectivity, of nanoporous materials is essential to identify correlations of these properties with the performance of gas storage, separation, and catalysis processes. The advances in developing nanoporous materials with uniform, tailor-made pore structures, including the introduction of hierarchical pore systems, offer huge potential for these applications. Within this context, major progress has been made in understanding the adsorption and phase behavior of confined fluids and consequently in physisorption characterization. This enables reliable pore size, volume, and network connectivity analysis using advanced, high-resolution experimental protocols coupled with advanced methods based on statistical mechanics, such as methods based on density functional theory and molecular simulation. If macro-pores are present, a combination of adsorption and mercury porosimetry can be useful. Hence, some important recent advances in understanding the mercury intrusion/extrusion mechanism are discussed. Additionally, some promising complementary techniques for characterization of porous materials immersed in a liquid phase are introduced.

Improving the yield and selectivity of chemical reactions is one of the challenging tasks in paving the way for a more sustainable and climate-friendly economy. For the industrially highly relevant gas-liquid reactions, this can be achieved by tailoring the timescales of mixing to the requirements of the reaction. Although this has long been known for idealized reactors and time- and space-averaged processes, considerable progress has been made recently on the influence of local mixing processes. This progress has become possible through joint research between chemists, mathematicians, and engineers. We present the reaction systems with adjustable kinetics that have been developed, which are easy to handle and analyze. We show examples of how the selectivity of competitive-consecutive reactions can be controlled via local bubble wake structures. This is demonstrated for Taylor bubbles and bubbly flows under technical conditions. Highly resolvednumerical simulations confirm the importance of the bubble wake structure for the performance of a particular chemical reaction and indicate tremendous potential for future process improvements.

High-performance wearable and implantable devices capable of recording physiological signals and delivering appropriate therapeutics in real time are playing a pivotal role in revolutionizing personalized healthcare. However, the mechanical and biochemical mismatches between rigid, inorganic devices and soft, organic human tissues cause significant trouble, including skin irritation, tissue damage, compromised signal-to-noise ratios, and limited service time. As a result, profuse research efforts have been devoted to overcoming these issues by using flexible and stretchable device designs and soft materials. Here, we summarize recent representative research and technological advances for soft bioelectronics, including conformable and stretchable device designs, various types of soft electronic materials, and surface coating and treatment methods. We also highlight applications of these strategies to emerging soft wearable and implantable devices. We conclude with some current limitations and offer future prospects of this booming field.