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Chemical Reviews

Chaoliang Tan, Xiehong Cao, Xue-Jun Wu, Qiyuan He, Jian Yang, Xiao Zhang, Junze Chen, Wei Zhao, Shikui Han, Gwang-Hyeon Nam, Melinda Sindoro, Hua Zhang
Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances...
March 17, 2017: Chemical Reviews
Tao Chen, Bin Dong, Kuangcai Chen, Fei Zhao, Xiaodong Cheng, Changbei Ma, Seungah Lee, Peng Zhang, Seong Ho Kang, Ji Won Ha, Weilin Xu, Ning Fang
Optical super-resolution imaging has gained momentum in investigations of heterogeneous and homogeneous chemical reactions at the single-molecule level. Thanks to its exceptional spatial resolution and ability to monitor dynamic systems, much detailed information on single-molecule reaction/adsorption processes and single-particle catalytic processes has been revealed, including chemical kinetics and reaction dynamics; active-site distributions on single-particle surfaces; and size-, shape-, and facet-dependent catalytic activities of individual nanocatalysts...
March 17, 2017: Chemical Reviews
Giuseppe Lubes, Mohammad Goodarzi
Smelling is one of the five senses, which plays an important role in our everyday lives. Volatile compounds are, for example, characteristics of food where some of them can be perceivable by humans because of their aroma. They have a great influence on the decision making of consumers when they choose to use a product or not. In the case where a product has an offensive and strong aroma, many consumers might not appreciate it. On the contrary, soft and fresh natural aromas definitely increase the acceptance of a given product...
March 17, 2017: Chemical Reviews
Klaus Kuhnke, Christoph Große, Pablo Merino, Klaus Kern
The conversion of electric power to light is an important scientific and technological challenge. Advanced experimental methods have provided access to explore the relevant microscopic processes at the nanometer scale. Here, we review state-of-the-art studies of electroluminescence induced on the molecular scale by scanning tunneling microscopy. We discuss the generation of excited electronic states and electron-hole pairs (excitons) at molecular interfaces and address interactions between electronic states, local electromagnetic fields (tip-induced plasmons), and molecular vibrations...
March 15, 2017: Chemical Reviews
Zachary G Brill, Matthew L Condakes, Chi P Ting, Thomas J Maimone
The pool of abundant chiral terpene building blocks (i.e., "chiral pool terpenes") has long served as a starting point for the chemical synthesis of complex natural products, including many terpenes themselves. As inexpensive and versatile starting materials, such compounds continue to influence modern synthetic chemistry. This review highlights 21st century terpene total syntheses which themselves use small, terpene-derived materials as building blocks. An outlook to the future of research in this area is highlighted as well...
March 15, 2017: Chemical Reviews
Markus Sauer, Mike Heilemann
Super-resolution fluorescence imaging by photoactivation or photoswitching of single fluorophores and position determination (single-molecule localization microscopy, SMLM) provides microscopic images with subdiffraction spatial resolution. This technology has enabled new insights into how proteins are organized in a cellular context, with a spatial resolution approaching virtually the molecular level. A unique strength of SMLM is that it delivers molecule-resolved information, along with super-resolved images of cellular structures...
March 13, 2017: Chemical Reviews
Xiao-Song Xue, Pengju Ji, Biying Zhou, Jin-Pei Cheng
The most fundamental concepts in chemistry are structure, energetics, reactivity and their inter-relationships, which are indispensable for promoting chemistry into a rational science. In this regard, bond energy, the intrinsic determinant directly related to structure and reactivity, should be most essential in serving as a quantitative basis for the design and understanding of organic transformations. Although C-H activation/functionalization have drawn tremendous research attention and flourished during the past decades, understanding the governing rules of bond energetics in these processes is still fragmentary and seems applicable only to limited cases, such as metal-oxo-mediated hydrogen atom abstraction...
March 10, 2017: Chemical Reviews
Hanna Jędrzejewska, Agnieszka Szumna
This review discusses chiral self-sorting-the process of choosing an interaction partner with a given chirality from a complex mixture of many possible racemic partners. Chiral self-sorting (also known as chiral self-recognition or chiral self-discrimination) is fundamental for creating functional structures in nature and in the world of chemistry because interactions between molecules of the same or the opposite chirality are characterized by different interaction energies and intrinsically different resulting structures...
March 9, 2017: Chemical Reviews
Dawei Zhang, Alexandre Martinez, Jean-Pierre Dutasta
In the wide area of host-guest chemistry, hemicryptophanes, combining a cyclotribenzylene (or cyclotriveratrylene CTV) unit with another different C3-symmetrical moiety, appears as a recent family of molecular cages. The synthesis and recognition properties of the first hemicryptophane were reported in 1982 by Collet and Lehn, but the very little attention received by this class of host compounds in the 20 years following this first promising result can account for their apparent novelty. Indeed, in the last 10 years hemicryptophanes have aroused growing interest, and new aspects have been developed...
March 9, 2017: Chemical Reviews
Jan Hermann, Robert A DiStasio, Alexandre Tkatchenko
Noncovalent van der Waals (vdW) or dispersion forces are ubiquitous in nature and influence the structure, stability, dynamics, and function of molecules and materials throughout chemistry, biology, physics, and materials science. These forces are quantum mechanical in origin and arise from electrostatic interactions between fluctuations in the electronic charge density. Here, we explore the conceptual and mathematical ingredients required for an exact treatment of vdW interactions, and present a systematic and unified framework for classifying the current first-principles vdW methods based on the adiabatic-connection fluctuation-dissipation (ACFD) theorem (namely the Rutgers-Chalmers vdW-DF, Vydrov-Van Voorhis (VV), exchange-hole dipole moment (XDM), Tkatchenko-Scheffler (TS), many-body dispersion (MBD), and random-phase approximation (RPA) approaches)...
March 8, 2017: Chemical Reviews
Jian-Feng Li, Yue-Jiao Zhang, Song-Yuan Ding, Rajapandiyan Panneerselvam, Zhong-Qun Tian
Core-shell nanoparticles are at the leading edge of the hot research topics and offer a wide range of applications in optics, biomedicine, environmental science, materials, catalysis, energy, and so forth, due to their excellent properties such as versatility, tunability, and stability. They have attracted enormous interest attributed to their dramatically tunable physicochemical features. Plasmonic core-shell nanomaterials are extensively used in surface-enhanced vibrational spectroscopies, in particular, surface-enhanced Raman spectroscopy (SERS), due to the unique localized surface plasmon resonance (LSPR) property...
March 8, 2017: Chemical Reviews
Ye Wei, Peng Hu, Min Zhang, Weiping Su
C-H bond activation and decarboxylation are two significant processes in organic synthesis. The combination of these processes provides a novel synthetic strategy, that is, decarboxylative C-H bond functionalization. Considerable attention has been focused on such an active research field. This review offers an overview of the utility of decarboxylative C-H bond functionalization in the synthesis of various organic compounds, such as styrenes, chalcones, biaryls, and heterocycles, covering most of the recent advances of the decarboxylative functionalization of Csp-H, Csp(2)-H, and Csp(3)-H bonds, as well as their scopes, limitations, practical applications, and synthetic potentials...
March 7, 2017: Chemical Reviews
Hans Blom, Jerker Widengren
Despite its short history, diffraction-unlimited fluorescence microscopy techniques have already made a substantial imprint in the biological sciences. In this review, we describe how stimulated emission depletion (STED) imaging originally evolved, how it compares to other optical super-resolution imaging techniques, and what advantages it provides compared to previous golden-standards for biological microscopy, such as diffraction-limited optical microscopy and electron microscopy. We outline the prerequisites for successful STED imaging experiments, emphasizing the equally critical roles of instrumentation, sample preparation, and photophysics, and describe major evolving strategies for how to push the borders of STED imaging even further in life science...
March 6, 2017: Chemical Reviews
Dong Won Shin, Michael D Guiver, Young Moo Lee
A fundamental understanding of polymer microstructure is important in order to design novel polymer electrolyte membranes (PEMs) with excellent electrochemical performance and stabilities. Hydrocarbon-based polymers have distinct microstructure according to their chemical structure. The ionic clusters and/or channels play a critical role in PEMs, affecting ion conductivity and water transport, especially at medium temperature and low relative humidity (RH). In addition, physical properties such as water uptake and dimensional swelling behavior depend strongly on polymer morphology...
March 3, 2017: Chemical Reviews
Brandon J Burkhart, Christopher J Schwalen, Greg Mann, James H Naismith, Douglas A Mitchell
With advances in sequencing technology, uncharacterized proteins and domains of unknown function (DUFs) are rapidly accumulating in sequence databases and offer an opportunity to discover new protein chemistry and reaction mechanisms. The focus of this review, the formerly enigmatic YcaO superfamily (DUF181), has been found to catalyze a unique phosphorylation of a ribosomal peptide backbone amide upon attack by different nucleophiles. Established nucleophiles are the side chains of Cys, Ser, and Thr which gives rise to azoline/azole biosynthesis in ribosomally synthesized and posttranslationally modified peptide (RiPP) natural products...
March 3, 2017: Chemical Reviews
Alideertu Dong, Yan-Jie Wang, Yangyang Gao, Tianyi Gao, Ge Gao
Microbial contamination arising from pathogens poses serious threats to human health and in recent decades has presented an unprecedented challenge to antibacterial research. Of the various antibacterial agents that effectively kill pathogens, halogen-based antibacterial compounds have been successful in eliminating harmful pathogen-associated diseases and are becoming the most popular disinfectants. As a significant subcategory of halogen antibacterial agents, N-halamines have drawn increasing research interest into their chemistry and practical applications...
March 2, 2017: Chemical Reviews
Damien Laage, Thomas Elsaesser, James T Hynes
The structure and function of biomolecules are strongly influenced by their hydration shells. Structural fluctuations and molecular excitations of hydrating water molecules cover a broad range in space and time, from individual water molecules to larger pools and from femtosecond to microsecond time scales. Recent progress in theory and molecular dynamics simulations as well as in ultrafast vibrational spectroscopy has led to new and detailed insight into fluctuations of water structure, elementary water motions, electric fields at hydrated biointerfaces, and processes of vibrational relaxation and energy dissipation...
March 1, 2017: Chemical Reviews
Xian Qin, Xiaowang Liu, Wei Huang, Marco Bettinelli, Xiaogang Liu
The synthesis of lanthanide-activated phosphors is pertinent to many emerging applications, ranging from high-resolution luminescence imaging to next-generation volumetric full-color display. In particular, the optical processes governed by the 4f-5d transitions of divalent and trivalent lanthanides have been the key to enabling precisely tuned color emission. The fundamental importance of lanthanide-activated phosphors for the physical and biomedical sciences has led to rapid development of novel synthetic methodologies and relevant tools that allow for probing the dynamics of energy transfer processes...
February 27, 2017: Chemical Reviews
Binshen Wang, Li Qin, Tiancheng Mu, Zhimin Xue, Guohua Gao
Ionic liquids have attracted a great deal of interest in recent years, illustrated by their applications in a variety of areas involved with chemistry, physics, biology, and engineering. Usually, the stabilities of ionic liquids are highlighted as one of their outstanding advantages. However, are ionic liquids really stable in all cases? This review covers the chemical stabilities of ionic liquids. It focuses on the reactivity of the most popular imidazolium ionic liquids at structural positions, including C2 position, N1 and N3 positions, and C4 and C5 positions, and decomposition on the imidazolium ring...
February 27, 2017: Chemical Reviews
Curt Wentrup
Flash vacuum pyrolysis (FVP) of azides is an extremely valuable method of generating nitrenes and studying their thermal rearrangements. The nitrenes can in many cases be isolated in low-temperature matrices and observed spectroscopically. NH and methyl, alkyl, aralkyl, vinyl, cyano, aryl and N-heteroaryl, acyl, carbamoyl, alkoxycarbonyl, imidoyl, boryl, silyl, phosphonyl, and sulfonyl nitrenes are included. FVP of triazoloazines generates diazomethylazines and azinylcarbenes, which often rearrange to the energetically more stable arylnitrenes...
February 24, 2017: Chemical Reviews
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