Topics in Current Chemistry最新文献

Nowadays, attention to single-atoms and also porous structures like metal–organic frameworks (MOFs) and covalent-organic frameworks (COFs) for the preparation of high-performance material is expanding rapidly. These dazzling materials with unprecedented properties have lots of applications, especially as promising catalysts for organic pollutants abatement, hydrogen evolution, reduction of CO₂, etc. To provide an in-depth understanding, in this mini-review, we begin with a brief description and a general background about single-atoms, COFs, as well as MOFs. After considering some fundamentals, the synergism effects, advantages, and their applications are discussed.

Near-infrared (NIR) refers to the section of the spectrum from 650 to 2500 nm. NIR luminescent materials are widely employed in organic light-emitting diodes (OLEDs), fiber optic communication, sensing, biological detection, and medical imaging. This paper reviews organic NIR electroluminescent materials, including organic NIR electrofluorescent materials and organic NIR electrophosphorescent materials that have been investigated in the past 6 years. Small-molecule, polymer NIR fluorescent materials and platinum(II) and iridium(III) complex NIR phosphorescent materials are described, and the limitations of the development of NIR luminescent materials and future prospects are discussed.

Photocatalytic chemical transformations in the presence of irradiated TiO₂ are generally considered in terms of interfacial electron transfer. However, more elusive energy-transfer-driven reactions have been also hypothesized to occur, mainly on the basis of the indirect evidence of detected reaction products whose existence could not be justified simply by electron transfer. Unlike in homogeneous and colloidal systems, where energy transfer mechanisms have been investigated deeply for several organic syntheses, understanding of similar processes in heterogeneous systems is at only a nascent level. However, this gap of knowledge can be filled by considering the important achievements of synthetic heterogeneous photocatalysis, which bring the field closer to industrial exploitation. The present manuscript summarizes the main findings of previous literature reports and, also on the basis of some novel experimental evidences, tentatively proposes that the energy transfer in TiO₂ photocatalysis could possess a Förster-like nature.

This review article focuses on the α-functionalization of acetophenones involving Kornblum oxidation and C–H functionalizations. Although various other strategies, such as classical approaches, enamine approaches and umpolung strategy are also known for this functionalization, here we discuss mainly the Kornblum oxidation approach and C–H functionalization strategy as they have advantages over the others. In Kornblum oxidation, the reaction uses iodine and dimethylsulfoxide and proceeds through the formation of arylglyoxal as the key intermediate. In C–H functionalization, the reaction requires metal, or metal-free catalyst, and generates radical intermediate in most cases. α-Functionalization of acetophenones is very important because of their huge applications in the synthesis of various natural products and pharmaceuticals and, therefore, a number of research articles have been published in this area. However, no review articles are available so far. In this article, we present a succinct discussion of various important and novel reactions, along with their mechanisms, published since 2012 to date. We believe that this first review article in this field will give readers one-stop information on this topic and encourage further intriguing work in this area.

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A series of methods (SDSCI, SDSPT2, iCI, iCIPT2, iCISCF(2), iVI, and iCAS) is introduced to accurately describe strongly correlated systems of electrons. Born from the (restricted) static–dynamic–static (SDS) framework for designing many-electron wave functions, SDSCI is a minimal multireference (MR) configuration interaction (CI) approach that constructs and diagonalizes a (3N_{text {P}}times 3N_{text {P}}) matrix for (N_{text {P}}) states, regardless of the numbers of orbitals and electrons to be correlated. If the full molecular Hamiltonian H in the QHQ block (which describes couplings between functions of the first-order interaction space Q) of the SDSCI CI matrix is replaced with a zeroth-order Hamiltonian (H_0) before the diagonalization is taken, we obtain SDSPT2, a CI-like second-order perturbation theory (PT2). Unlike most variants of MRPT2, SDSPT2 treats single and multiple states in the same way and is particularly advantageous in the presence of near degeneracy. On the other hand, if the SDSCI procedure is repeated until convergence, we will have iterative CI (iCI), which can converge quickly from the above to the exact solutions (full CI) even when starting with a poor guess. When further combined with the selection of important configurations followed by a PT2 treatment of dynamic correlation, iCI becomes iCIPT2, which is a near-exact theory for medium-sized systems. The microiterations of iCI for relaxing the coefficients of contracted many-electron functions can be generalized to an iterative vector interaction (iVI) approach for finding exterior or interior roots of a given matrix, in which the dimension of the search subspace is fixed by either the number of target roots or the user-specified energy window. Naturally, iCIPT2 can be employed as the active space solver of the complete active space (CAS) self-consistent field, leading to iCISCF(2), which can further be combined with iCAS for automated selection of active orbitals and assurance of the same CAS for all states and all geometries. The methods are calibrated by taking the Thiel set of benchmark systems as examples. Results for the corresponding cations, a new set of benchmark systems, are also reported.

Esters and their derivatives are distributed widely in natural products, pharmaceuticals, fine chemicals and other fields. Esters are important building blocks in pharmaceuticals such as clopidogrel, methylphenidate, fenofibrate, travoprost, prasugrel, oseltamivir, eszopiclone and fluticasone. Therefore, esterification reaction becomes more and more popular in the photochemical field. In this review, we highlight three types of reactions to synthesize esters using photochemical strategies. The reaction mechanisms involve mainly single electron transfer, energy transfer or other radical procedures.

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Sustainable scientific software needs a strong collaboration framework to ensure continuity by passing on the tools, skills and knowledge needed to the next generation. The COVID-19 pandemic triggered the unexpected effect of accelerating the development of remote platforms and tools to open up collaborations to a wider global community. In this article we outline the elements needed for such a framework, such as education, tools and community building, and discuss the current advances in technology with a nod to the future.

Bioorthogonal reactions are rapid, specific and high yield reactions that can be performed in in vivo microenvironments or simulated microenvironments. At present, the main biorthogonal reactions include Staudinger ligation, copper-catalyzed azide alkyne cycloaddition, strain-promoted [3 + 2] reaction, tetrazine ligation, metal-catalyzed coupling reaction and photo-induced biorthogonal reactions. To date, many reviews have reported that bioorthogonal reactions have been used widely as a powerful tool in the field of life sciences, such as in target recognition, drug discovery, drug activation, omics research, visualization of life processes or exogenous bacterial infection processes, signal transduction pathway research, chemical reaction dynamics analysis, disease diagnosis and treatment. In contrast, to date, few studies have investigated the application of bioorthogonal reactions in the analysis of biomacromolecules in vivo. Therefore, the application of bioorthogonal reactions in the analysis of proteins, nucleic acids, metabolites, enzyme activities and other endogenous molecules, and the determination of disease-related targets is reviewed. In addition, this review discusses the future development opportunities and challenges of biorthogonal reactions.

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This review presents an overview of recent advances for application in biomolecular analysis and disease diagnosis, with a focus on proteins, metabolites and RNA detection.

Pyrone moieties are present in natural products and can be synthesized by a diverse range of synthetic methods, resulting in the formation of various derivatives through chemical modifications. Many pyrone-based derivatives are commercially available and are biocompatible. They are building blocks of various intermediates in organic synthesis. They possess remarkable biological properties including antimicrobial, antiviral, cytotoxic, and antitumor activity. These characteristics have made them valuable for the development of drugs. We have summarized recent developments in the synthesis of 2-pyrone and its derivatives and their potential applications. With regard to synthetic approaches, the focus has been on metal-free and transition metal-catalyzed reactions.

Traditional drug discovery effectively contributes to the treatment of many diseases but is limited by high costs and long cycles. Quantitative structure–activity relationship (QSAR) methods were introduced to evaluate the activity of compounds virtually, which saves the significant cost of determining the activities of the compounds experimentally. Over the past two decades, many web tools for QSAR modeling with various features have been developed to facilitate the usage of QSAR methods. These web tools significantly reduce the difficulty of using QSAR and indirectly promote drug discovery. However, there are few comprehensive summaries of these QSAR tools, and researchers may have difficulty determining which tool to use. Hence, we systematically surveyed the mainstream web tools for QSAR modeling. This work may guide researchers in choosing appropriate web tools for developing QSAR models, and may also help develop more bioinformatics tools based on these existing resources. For nonprofessionals, we also hope to make more people aware of QSAR methods and expand their use.

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