Topics in Current Chemistry最新文献

Cellular functions rely on a series of organized and regulated multienzyme cascade reactions. The catalytic efficiencies of these cascades depend on the precise spatial organization of the constituent enzymes, which is optimized to facilitate substrate transport and regulate activities. Mimicry of this organization in a non-living, artificial system would be very useful in a broad range of applications—with impacts on both the scientific community and society at large. Self-assembled DNA nanostructures are promising applications to organize biomolecular components into prescribed, multidimensional patterns. In this review, we focus on recent progress in the field of DNA-scaffolded assembly and confinement of multienzyme reactions. DNA self-assembly is exploited to build spatially organized multienzyme cascades with control over their relative distance, substrate diffusion paths, compartmentalization and activity actuation. The combination of addressable DNA assembly and multienzyme cascades can deliver breakthroughs toward the engineering of novel synthetic and biomimetic reactors.

Self-assembly, which is ubiquitous in living systems, also stimulates countless synthetic molecular self-assembling systems. Most synthetic self-assemblies are realized by passive processes, going from high-energy states to thermodynamic equilibrium. Conversely, living systems work out of equilibrium, meaning they are energy-consuming, dissipative and active. In recently years, chemists have made extensive efforts to design artificial active self-assembly systems, which will be pivotal to emulating and understanding life. Among various strategies, emerging approaches based on DNA nanotechnology have attracted a lot of attention. Structural- as well as dynamic-DNA-nanotechnology offer diverse tools with which to design building blocks and to shape their assembly behaviors. To achieve active self-assembly, a synergy of diverse DNA techniques is essential, including structural design, controllable assembly–disassembly, autonomous assembly, molecular circuits, biochemical oscillators, and so on. In this review, we introduce progress towards, or related to, active assembly via DNA nanotechnology. Dynamic DNA assembly systems ranging from passive assembly–disassembly systems, to autonomous assembly systems to sophisticated artificial metabolism and time-clocking oscillation systems will be discussed. We catalogue these systems from the perspective of free energy change with the reaction process. We end the review with a brief outlook and discussion.

The efficacy of photocatalysis strongly depends on the activity of the catalysts and the operational factors, especially factors associated with mass transfer and the possibility of catalyst deactivation. The use of ultrasound has great potential to enhance catalyst activity, during both the synthesis and actual oxidation processes due to the cavitational effects of turbulence and liquid streaming. This article presents an overview of the application aspects of ultrasound, both in the synthesis of the photocatalyst and applications for wastewater treatment. A review of the literature revealed that the use of ultrasound in the synthesis processes can result in a catalyst with a lower mean size and higher surface area as well as uniform size distribution. The application of ultrasound in the actual photocatalytic oxidation facilitates enhancement of the oxidation capacity, leading to higher degradation rates, sometimes synergistic results and definitely?lower treatment times. This article also presents guidelines for the selection of the best operating conditions for the use of ultrasound in photocatalytic systems and includes a discussion on the possible reactor configurations suitable for large-scale operations. Overall, a combination of ultrasound with photocatalytic oxidation or the optimized application of ultrasound in catalyst synthesis can yield significant benefits.

DNA nanostructures hold great promise for various applications due to their remarkable properties, including programmable assembly, nanometric positional precision, and dynamic structural control. The past few decades have seen the development of various kinds of DNA nanostructures that can be employed as useful tools in fields such as chemistry, materials, biology, and medicine. Aptamers are short single-stranded nucleic acids that bind to specific targets with excellent selectivity and high affinity and play critical roles in molecular recognition. Recently, many attempts have been made to integrate aptamers with DNA nanostructures for a range of biological applications. This review starts with an introduction to the features of aptamer-functionalized DNA nanostructures. The discussion then focuses on recent progress (particularly during the last five?years) in the applications of these nanostructures in areas such as biosensing, bioimaging, cancer therapy, and biophysics. Finally, challenges involved in the practical application of aptamer-functionalized DNA nanostructures are discussed, and perspectives on future directions for research into and applications of aptamer-functionalized DNA nanostructures are provided.

DNA molecules with superior flexibility, affinity and programmability have garnered considerable attention for the controllable assembly of nanoparticles (NPs). By controlling the density, length and sequences of DNA on NPs, the configuration of NP assemblies can be rationally designed. The specific recognition of DNA enables changes to be made to the spatial structures of NP assemblies, resulting in differences in tailorable optical signals. Comprehensive information on the fabrication of DNA-driven NP assemblies would be beneficial for their application in biosensing and bioimaging. This review analyzes the progress of DNA-driven NP assemblies, and discusses the tunable configurations determined by the structural parameters of DNA skeletons. The collective optical properties, such as chirality, fluorescence and surface enhanced Raman resonance (SERS), etc., of DNA-driven NP assemblies are explored, and engineered tailorable optical properties of these spatial structures are achieved. We discuss the development of DNA-directed NP assemblies for the quantification of DNA, toxins, and heavy metal ions, and demonstrate their potential application in the biosensing and bioimaging of tumor markers, RNA, living metal ions and phototherapeutics. We hihghlight possible challenges in the development of DNA-driven NP assemblies, and further direct potential prospects in the practical applications of macroscopical materials and photonic devices.

Petroleum is an essential source of energy for our daily life. However, crude oil contains various kinds of sulfur-containing compounds that will form sulfur oxides upon combustion and cause severe environmental problems. To reduce the environmental impact of petroleum energy, the desulfurization of fuels is necessary. Metal–organic frameworks (MOFs), an emerging class of porous materials, have shown great potential in a variety of applications. In this review, we summarize the use of MOFs in the desulfurization of fuels. The scope of this review includes MOFs and MOF-derived materials that have been applied in oxidative desulfurization and adsorptive desulfurization processes. We aim to provide an overview of the progress of MOFs in fuel desulfurization as well as shed light on the development of superior MOF-based materials in the field of desulfurization.

Nowadays, biomaterials have become a crucial element in numerous biomedical, preclinical, and clinical applications. The use of nanoparticles entails a great potential in these fields mainly because of the high ratio of surface atoms that modify the physicochemical properties and increases the chemical reactivity. Among them, carbon nanotubes (CNTs) have emerged as a powerful tool to improve biomedical approaches in the management of numerous diseases. CNTs have an excellent ability to penetrate cell membranes, and the sp² hybridization of all carbons enables their functionalization with almost every biomolecule or compound, allowing them to target cells and deliver drugs under the appropriate environmental stimuli. Besides, in the new promising field of artificial biomaterial generation, nanotubes are studied as the load in nanocomposite materials, improving their mechanical and electrical properties, or even for direct use as scaffolds in body tissue manufacturing. Nevertheless, despite their beneficial contributions, some major concerns need to be solved to boost the clinical development of CNTs, including poor solubility in water, low biodegradability and dispersivity, and toxicity problems associated with CNTs’ interaction with biomolecules in tissues and organs, including the possible effects in the proteome and genome. This review performs a wide literature analysis to present the main and latest advances in the optimal design and characterization of carbon nanotubes with biomedical applications, and their capacities in different areas of preclinical research.

Classical molecular simulations can provide significant insights into the gas adsorption mechanisms and binding sites in various metal–organic frameworks (MOFs). These simulations involve assessing the interactions between the MOF and an adsorbate molecule by calculating the potential energy of the MOF–adsorbate system using a functional form that generally includes nonbonded interaction terms, such as the repulsion/dispersion and permanent electrostatic energies. Grand canonical Monte Carlo (GCMC) is the most widely used classical method that is carried out to simulate gas adsorption and separation in MOFs and identify the favorable adsorbate binding sites. In this review, we provide an overview of the GCMC methods that are normally utilized to perform these simulations. We also describe how a typical force field is developed for the MOF, which is required to compute the classical potential energy of the system. Furthermore, we highlight some of the common analysis techniques that have been used to determine the locations of the preferential binding sites in these materials. We also review some of the early classical molecular simulation studies that have contributed to our working understanding of the gas adsorption mechanisms in MOFs. Finally, we show that the implementation of classical polarization for simulations in MOFs can be necessary for the accurate modeling of an adsorbate in these materials, particularly those that contain open-metal sites. In general, molecular simulations can provide a great complement to experimental studies by helping to rationalize the favorable MOF–adsorbate interactions and the mechanism of gas adsorption.