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  • Chemical and Biological Dynamics Using Droplet-Based Microfluidics
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Oliver J. Dressler, Xavier Casadevall i Solvas, Andrew J. deMello

    Recent years have witnessed an increased use of droplet-based microfluidic techniques in a wide variety of chemical and biological assays. Nevertheless, obtaining dynamic data from these platforms has remained challenging, as this often requires reading the same droplets (possibly thousands of them) multiple times over a wide range of intervals (from milliseconds to hours). In this review, we introduce the elemental techniques for the formation and manipulation of microfluidic droplets, together with the most recent developments in these areas. We then discuss a wide range of analytical methods that have been successfully adapted for analyte detection in droplets. Finally, we highlight a diversity of studies where droplet-based microfluidic strategies have enabled the characterization of dynamic systems that would otherwise have remained unexplorable.

    更新日期:2017-06-21
  • Sizing Up Protein–Ligand Complexes: The Rise of Structural Mass Spectrometry Approaches in the Pharmaceutical Sciences
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Joseph D. Eschweiler, Richard Kerr, Jessica Rabuck-Gibbons, Brandon T. Ruotolo

    Capturing the dynamic interplay between proteins and their myriad interaction partners is critically important for advancing our understanding of almost every biochemical process and human disease. The importance of this general area has spawned many measurement methods capable of assaying such protein complexes, and the mass spectrometry–based structural biology methods described in this review form an important part of that analytical arsenal. Here, we survey the basic principles of such measurements, cover recent applications of the technology that have focused on protein–small-molecule complexes, and discuss the bright future awaiting this group of technologies.

    更新日期:2017-06-21
  • Applications of the New Family of Coherent Multidimensional Spectroscopies for Analytical Chemistry
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    John C. Wright

    A new family of vibrational and electronic spectroscopies has emerged, comprising the coherent analogs of traditional analytical methods. These methods are also analogs of coherent multidimensional nuclear magnetic resonance (NMR) spectroscopy. This new family is based on creating the same quantum mechanical superposition states called multiple quantum coherences (MQCs). NMR MQCs are mixtures of nuclear spin states that retain their quantum mechanical phase information for milliseconds. The MQCs in this new family are mixtures of vibrational and electronic states that retain their phases for picoseconds or shorter times. Ultrafast, high-intensity coherent beams rapidly excite multiple states. The excited MQCs then emit bright beams while they retain their phases. Time-domain methods measure the frequencies of the MQCs by resolving their phase oscillations, whereas frequency-domain methods measure the resonance enhancements of the output beam while scanning the excitation frequencies. The resulting spectra provide multidimensional spectral signatures that increase the spectroscopic selectivity required for analyzing complex samples.

    更新日期:2017-06-21
  • Coupling Front-End Separations, Ion Mobility Spectrometry, and Mass Spectrometry For Enhanced Multidimensional Biological and Environmental Analyses
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Xueyun Zheng, Roza Wojcik, Xing Zhang, Yehia M. Ibrahim, Kristin E. Burnum-Johnson, Daniel J. Orton, Matthew E. Monroe, Ronald J. Moore, Richard D. Smith, Erin S. Baker

    Ion mobility spectrometry (IMS) is a widely used analytical technique for rapid molecular separations in the gas phase. Though IMS alone is useful, its coupling with mass spectrometry (MS) and front-end separations is extremely beneficial for increasing measurement sensitivity, peak capacity of complex mixtures, and the scope of molecular information available from biological and environmental sample analyses. In fact, multiple disease screening and environmental evaluations have illustrated that the IMS-based multidimensional separations extract information that cannot be acquired with each technique individually. This review highlights three-dimensional separations using IMS-MS in conjunction with a range of front-endtechniques, such as gas chromatography, supercritical fluid chromatography, liquid chromatography, solid-phase extractions, capillary electrophoresis, field asymmetric ion mobility spectrometry, and microfluidic devices. The origination, current state, various applications, and future capabilities of these multidimensional approaches are described in detail to provide insight into their uses and benefits.

    更新日期:2017-06-21
  • Multianalyte Physiological Microanalytical Devices
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Anna Nix Davis, Adam R. Travis, Dusty R. Miller, David E. Cliffel

    Advances in scientific instrumentation have allowed experimentalists to evaluate well-known systems in new ways and to gain insight into previously unexplored or poorly understood phenomena. Within the growing field of multianalyte physiometry (MAP), microphysiometers are being developed that are capable of electrochemically measuring changes in the concentration of various metabolites in real time. By simultaneously quantifying multiple analytes, these devices have begun to unravel the complex pathways that govern biological responses to ischemia and oxidative stress while contributing to basic scientific discoveries in bioenergetics and neurology. Patients and clinicians have also benefited from the highly translational nature of MAP, and the continued expansion of the repertoire of analytes that can be measured with multianalyte microphysiometers will undoubtedly play a role in the automation and personalization of medicine. This is perhaps most evident with the recent advent of fully integrated noninvasive sensor arrays that can continuously monitor changes in analytes linked to specific disease states and deliver a therapeutic agent as required without the need for patient action.

    更新日期:2017-06-21
  • Nanosensor Technology Applied to Living Plant Systems
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Seon-Yeong Kwak, Min Hao Wong, Tedrick Thomas Salim Lew, Gili Bisker, Michael A. Lee, Amir Kaplan, Juyao Dong, Albert Tianxiang Liu, Volodymyr B. Koman, Rosalie Sinclair, Catherine Hamann, Michael S. Strano

    An understanding of plant biology is essential to solving many long-standing global challenges, including sustainable and secure food production and the generation of renewable fuel sources. Nanosensor platforms, sensors with a characteristic dimension that is nanometer in scale, have emerged as important tools for monitoring plant signaling pathways and metabolism that are nondestructive, minimally invasive, and capable of real-time analysis. This review outlines the recent advances in nanotechnology that enable these platforms, including the measurement of chemical fluxes even at the single-molecule level. Applications of nanosensors to plant biology are discussed in the context of nutrient management, disease assessment, food production, detection of DNA proteins, and the regulation of plant hormones. Current trends and future needs are discussed with respect to the emerging trends of precision agriculture, urban farming, and plant nanobionics.

    更新日期:2017-06-21
  • Coded Apertures in Mass Spectrometry
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Jason J. Amsden, Michael E. Gehm, Zachary E. Russell, Evan X. Chen, Shane T. Di Dona, Scott D. Wolter, Ryan M. Danell, Gottfried Kibelka, Charles B. Parker, Brian R. Stoner, David J. Brady, Jeffrey T. Glass

    The use of coded apertures in mass spectrometry can break the trade-off between throughput and resolution that has historically plagued conventional instruments. Despite their very early stage of development, coded apertures have been shown to increase throughput by more than one order of magnitude, with no loss in resolution in a simple 90-degree magnetic sector. This enhanced throughput can increase the signal level with respect to the underlying noise, thereby significantly improving sensitivity to low concentrations of analyte. Simultaneous resolution can be maintained, preventing any decrease in selectivity. Both one- and two-dimensional (2D) codes have been demonstrated. A 2D code can provide increased measurement diversity and therefore improved numerical conditioning of the mass spectrum that is reconstructed from the coded signal. This review discusses the state of development, the applications where coding is expected to provide added value, and the various instrument modifications necessary to implement coded apertures in mass spectrometers.

    更新日期:2017-06-21
  • Magnetic Resonance Spectroscopy as a Tool for Assessing Macromolecular Structure and Function in Living Cells
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Conggang Li, Jiajing Zhao, Kai Cheng, Yuwei Ge, Qiong Wu, Yansheng Ye, Guohua Xu, Zeting Zhang, Wenwen Zheng, Xu Zhang, Xin Zhou, Gary Pielak, Maili Liu

    Investigating the structure, modification, interaction, and function of biomolecules in their native cellular environment leads to physiologically relevant knowledge about their mechanisms, which will benefit drug discovery and design. In recent years, nuclear and electron magnetic resonance (NMR) spectroscopy has emerged as a useful tool for elucidating the structure and function of biomacromolecules, including proteins, nucleic acids, and carbohydrates in living cells at atomic resolution. In this review, we summarize the progress and future of in-cell NMR as it is applied to proteins, nucleic acids, and carbohydrates.

    更新日期:2017-06-21
  • Plasmonic Imaging of Electrochemical Impedance
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Liang Yuan, Nongjian Tao, Wei Wang

    Electrochemical impedance spectroscopy (EIS) measures the frequency spectrum of an electrochemical interface to resist an alternating current. This method allows label-free and noninvasive studies on interfacial adsorption and molecular interactions and has applications in biosensing and drug screening. Although powerful, traditional EIS lacks spatial resolution or imaging capability, hindering the study of heterogeneous electrochemical processes on electrodes. We have recently developed a plasmonics-based electrochemical impedance technique to image local electrochemical impedance with a submicron spatial resolution and a submillisecond temporal resolution. In this review, we provide a systematic description of the theory, instrumentation, and data analysis of this technique. To illustrate its present and future applications, we further describe several selected samples analyzed with this method, including protein microarrays, two-dimensional materials, and single cells. We conclude by summarizing the technique's unique features and discussing the remaining challenges and new directions of its application.

    更新日期:2017-06-21
  • Tailored Surfaces/Assemblies for Molecular Plasmonics and Plasmonic Molecular Electronics
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Jean-Christophe Lacroix, Pascal Martin, Pierre-Camille Lacaze

    Molecular plasmonics uses and explores molecule–plasmon interactions on metal nanostructures for spectroscopic, nanophotonic, and nanoelectronic devices. This review focuses on tailored surfaces/assemblies for molecular plasmonics and describes active molecular plasmonic devices in which functional molecules and polymers change their structural, electrical, and/or optical properties in response to external stimuli and that can dynamically tune the plasmonic properties. We also explore an emerging research field combining molecular plasmonics and molecular electronics.

    更新日期:2017-06-21
  • Light-Addressable Potentiometric Sensors for Quantitative Spatial Imaging of Chemical Species
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Tatsuo Yoshinobu, Ko-ichiro Miyamoto, Carl Frederik Werner, Arshak Poghossian, Torsten Wagner, Michael J. Schöning

    A light-addressable potentiometric sensor (LAPS) is a semiconductor-based chemical sensor, in which a measurement site on the sensing surface is defined by illumination. This light addressability can be applied to visualize the spatial distribution of pH or the concentration of a specific chemical species, with potential applications in the fields of chemistry, materials science, biology, and medicine. In this review, the features of this chemical imaging sensor technology are compared with those of other technologies. Instrumentation, principles of operation, and various measurement modes of chemical imaging sensor systems are described. The review discusses and summarizes state-of-the-art technologies, especially with regard to the spatial resolution and measurement speed; for example, a high spatial resolution in a submicron range and a readout speed in the range of several tens of thousands of pixels per second have been achieved with the LAPS. The possibility of combining this technology with microfluidic devices and other potential future developments are discussed.

    更新日期:2017-06-21
  • Analyzing the Heterogeneous Hierarchy of Cultural Heritage Materials: Analytical Imaging
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Karen Trentelman

    Objects of cultural heritage significance are created using a wide variety of materials, or mixtures of materials, and often exhibit heterogeneity on multiple length scales. The effective study of these complex constructions thus requires the use of a suite of complementary analytical technologies. Moreover, because of the importance and irreplaceability of most cultural heritage objects, researchers favor analytical techniques that can be employed noninvasively, i.e., without having to remove any material for analysis. As such, analytical imaging has emerged as an important approach for the study of cultural heritage. Imaging technologies commonly employed, from the macroscale through the micro- to nanoscale, are discussed with respect to how the information obtained helps us understand artists’ materials and methods, the cultures in which the objects were created, how the objects may have changed over time, and importantly, how we may develop strategies for their preservation.

    更新日期:2017-06-21
  • Raman Imaging in Cell Membranes, Lipid-Rich Organelles, and Lipid Bilayers
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Aleem Syed, Emily A. Smith

    Raman-based optical imaging is a promising analytical tool for noninvasive, label-free chemical imaging of lipid bilayers and cellular membranes. Imaging using spontaneous Raman scattering suffers from a low intensity that hinders its use in some cellular applications. However, developments in coherent Raman imaging, surface-enhanced Raman imaging, and tip-enhanced Raman imaging have enabled video-rate imaging, excellent detection limits, and nanometer spatial resolution, respectively. After a brief introduction to these commonly used Raman imaging techniques for cell membrane studies, this review discusses selected applications of these modalities for chemical imaging of membrane proteins and lipids. Finally, recent developments in chemical tags for Raman imaging and their applications in the analysis of selected cell membrane components are summarized. Ongoing developments toward improving the temporal and spatial resolution of Raman imaging and small-molecule tags with strong Raman scattering cross sections continue to expand the utility of Raman imaging for diverse cell membrane studies.

    更新日期:2017-06-21
  • Beyond Antibodies as Binding Partners: The Role of Antibody Mimetics in Bioanalysis
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Xiaowen Yu, Yu-Ping Yang, Emre Dikici, Sapna K. Deo, Sylvia Daunert

    The emergence of novel binding proteins or antibody mimetics capable of binding to ligand analytes in a manner analogous to that of the antigen–antibody interaction has spurred increased interest in the biotechnology and bioanalytical communities. The goal is to produce antibody mimetics designed to outperform antibodies with regard to binding affinities, cellular and tumor penetration, large-scale production, and temperature and pH stability. The generation of antibody mimetics with tailored characteristics involves the identification of a naturally occurring protein scaffold as a template that binds to a desired ligand. This scaffold is then engineered to create a superior binder by first creating a library that is then subjected to a series of selection steps. Antibody mimetics have been successfully used in the development of binding assays for the detection of analytes in biological samples, as well as in separation methods, cancer therapy, targeted drug delivery, and in vivo imaging. This review describes recent advances in the field of antibody mimetics and their applications in bioanalytical chemistry, specifically in diagnostics and other analytical methods.

    更新日期:2017-06-21
  • Identification and Quantitation of Circulating Tumor Cells
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Siddarth Rawal, Yu-Ping Yang, Richard Cote, Ashutosh Agarwal

    Circulating tumor cells (CTCs) are shed from the primary tumor into the circulatory system and act as seeds that initiate cancer metastasis to distant sites. CTC enumeration has been shown to have a significant prognostic value as a surrogate marker in various cancers. The widespread clinical utility of CTC tests, however, is still limited due to the inherent rarity and heterogeneity of CTCs, which necessitate robust techniques for their efficient enrichment and detection. Significant recent advances have resulted in technologies with the ability to improve yield and purity of CTC enrichment as well as detection sensitivity. Current efforts are largely focused on the translation and standardization of assays to fully realize the clinical utility of CTCs. In this review, we aim to provide a comprehensive overview of CTC enrichment and detection techniques with an emphasis on novel approaches for rapid quantification of CTCs.

    更新日期:2017-06-21
  • Single-Molecule Arrays for Protein and Nucleic Acid Analysis
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Limor Cohen, David R. Walt

    The last few years have seen breakthroughs that will transform our ability to measure important analytes. Miniaturization of reaction volumes and confinement of analytes of interest into ultrasmall containers have greatly enhanced the sensitivity and throughput of many detection methods. Fabrication of microwell arrays and implementation of bead-based assays have been instrumental in the development of methods for measuring relevant biomolecules, with applications to both diagnostics and fundamental biological studies. In this review, we describe how microwell arrays are fabricated and utilized for measuring analytes of interest. We then discuss the fundamental concepts of digital enzyme-linked immunosorbent assay (ELISA) using single-molecule arrays and applications of microwell arrays to ultrasensitive protein measurements. We also explore the utility of microwell arrays for nucleic acid detection and applications for single-cell studies.

    更新日期:2017-06-21
  • The Solution Assembly of Biological Molecules Using Ion Mobility Methods: From Amino Acids to Amyloid β-Protein
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Christian Bleiholder, Michael T. Bowers

    Ion mobility spectrometry-mass spectrometry (IMS-MS) methods are increasingly used to study noncovalent assemblies of peptides and proteins. This review focuses on the noncovalent self-assembly of amino acids and peptides, systems at the heart of the amyloid process that play a central role in a number of devastating diseases. Three different systems are discussed in detail: the 42-residue peptide amyloid-β42 implicated in the etiology of Alzheimer's disease, several amyloid-forming peptides with 6–11 residues, and the assembly of individual amino acids. We also discuss from a more fundamental perspective the processes that determine how quickly proteins and their assemblies denature when the analyte ion has been stripped of its solvent in an IMS-MS measurement and how to soften the measurement so that biologically meaningful data can be recorded.

    更新日期:2017-06-21
  • Applications of Surface Second Harmonic Generation in Biological Sensing
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Renee J. Tran, Krystal L. Sly, John C. Conboy

    Surface second harmonic generation (SHG) is a coherent, nonlinear optical technique that is well suited for investigations of biomolecular interactions at interfaces. SHG is surface specific due to the intrinsic symmetry constraints on the nonlinear process, providing a distinct analytical advantage over linear spectroscopic methods, such as fluorescence and UV-Visible absorbance spectroscopies. SHG has the ability to detect low concentrations of analytes, such as proteins, peptides, and small molecules, due to its high sensitivity, and the second harmonic response can be enhanced through the use of target molecules that are resonant with the incident (ω) and/or second harmonic (2ω) frequencies. This review describes the theoretical background of SHG, and then it discusses its sensitivity, limit of detection, and the implementation of the method. It also encompasses the applications of surface SHG directed at the study of protein-surface, small-molecule–surface, and nanoparticle-membrane interactions, as well as molecular chirality, imaging, and immunoassays. The versatility, high sensitivity, and surface specificity of SHG show great potential for developments in biosensors and bioassays.

    更新日期:2017-06-21
  • Bioanalytical Measurements Enabled by Surface-Enhanced Raman Scattering (SERS) Probes
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Lauren E. Jamieson, Steven M. Asiala, Kirsten Gracie, Karen Faulds, Duncan Graham

    Since its discovery in 1974, surface-enhanced Raman scattering (SERS) has gained momentum as an important tool in analytical chemistry. SERS is used widely for analysis of biological samples, ranging from in vitro cell culture models, to ex vivo tissue and blood samples, and direct in vivo application. New insights have been gained into biochemistry, with an emphasis on biomolecule detection, from small molecules such as glucose and amino acids to larger biomolecules such as DNA, proteins, and lipids. These measurements have increased our understanding of biological systems, and significantly, they have improved diagnostic capabilities. SERS probes display unique advantages in their detection sensitivity and multiplexing capability. We highlight key considerations that are required when performing bioanalytical SERS measurements, including sample preparation, probe selection, instrumental configuration, and data analysis. Some of the key bioanalytical measurements enabled by SERS probes with application to in vitro, ex vivo, and in vivo biological environments are discussed.

    更新日期:2017-06-21
  • Single-Cell Transcriptional Analysis
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2017-06-12
    Angela R. Wu, Jianbin Wang, Aaron M. Streets, Yanyi Huang

    Despite being a relatively recent technological development, single-cell transcriptional analysis through high-throughput sequencing has already been used in hundreds of fruitful studies to make exciting new biological discoveries that would otherwise be challenging or even impossible. Consequently, this has fueled a virtuous cycle of even greater interest in the field and compelled development of further improved technical methodologies and approaches. Thanks to the combined efforts of the research community, including the fields of biochemistry and molecular biology, technology and instrumentation, data science, computational biology, and bioinformatics, the single-cell RNA-sequencing field is advancing at a pace that is both astounding and unprecedented. In this review, we provide a broad introduction to this revolutionary technology by presenting the state-of-the-art in sample preparation methodologies, technology platforms, and computational analysis methods, while highlighting the key considerations for designing, executing, and interpreting a study using single-cell RNA sequencing.

    更新日期:2017-06-21
  • Applications of Optical Microcavity Resonators in Analytical Chemistry
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    James H. Wade, Ryan C. Bailey

    Optical resonator sensors are an emerging class of analytical technologies that use recirculating light confined within a microcavity to sensitively measure the surrounding environment. Bolstered by advances in microfabrication, these devices can be configured for a wide variety of chemical or biomolecular sensing applications. We begin with a brief description of optical resonator sensor operation, followed by discussions regarding sensor design, including different geometries, choices of material systems, methods of sensor interrogation, and new approaches to sensor operation. Throughout, key developments are highlighted, including advancements in biosensing and other applications of optical sensors. We discuss the potential of alternative sensing mechanisms and hybrid sensing devices for more sensitive and rapid analyses. We conclude with our perspective on the future of optical microcavity sensors and their promise as versatile detection elements within analytical chemistry.

    更新日期:2017-06-12
  • Molecular Plasmonics
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Andrew J. Wilson, Katherine A. Willets

    In this review, we survey recent advances in the field of molecular plasmonics beyond the traditional sensing modality. Molecular plasmonics is explored in the context of the complex interaction between plasmon resonances and molecules and the ability of molecules to support plasmons self-consistently. First, spectroscopic changes induced by the interaction between molecular and plasmonic resonances are discussed, followed by examples of how tuning molecular properties leads to active molecular plasmonic systems. Next, the role of the position and polarizability of a molecular adsorbate on surface-enhanced Raman scattering signals is examined experimentally and theoretically. Finally, we introduce recent research focused on using molecules as plasmonic materials. Each of these examples is intended to highlight the role of molecules as integral components in coupled molecule-plasmon systems, as well as to show the diversity of applications in molecular plasmonics.

    更新日期:2017-06-12
  • Advances in Mid-Infrared Spectroscopy for Chemical Analysis
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Julian Haas, Boris Mizaikoff

    Infrared spectroscopy in the 3–20 μm spectral window has evolved from a routine laboratory technique into a state-of-the-art spectroscopy and sensing tool by benefitting from recent progress in increasingly sophisticated spectra acquisition techniques and advanced materials for generating, guiding, and detecting mid-infrared (MIR) radiation. Today, MIR spectroscopy provides molecular information with trace to ultratrace sensitivity, fast data acquisition rates, and high spectral resolution catering to demanding applications in bioanalytics, for example, and to improved routine analysis. In addition to advances in miniaturized device technology without sacrificing analytical performance, selected innovative applications for MIR spectroscopy ranging from process analysis to biotechnology and medical diagnostics are highlighted in this review.

    更新日期:2017-06-12
  • In Situ and In Vivo Molecular Analysis by Coherent Raman Scattering Microscopy
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Chien-Sheng Liao, Ji-Xin Cheng

    Coherent Raman scattering (CRS) microscopy is a high-speed vibrational imaging platform with the ability to visualize the chemical content of a living specimen by using molecular vibrational fingerprints. We review technical advances and biological applications of CRS microscopy. The basic theory of CRS and the state-of-the-art instrumentation of a CRS microscope are presented. We further summarize and compare the algorithms that are used to separate the Raman signal from the nonresonant background, to denoise a CRS image, and to decompose a hyperspectral CRS image into concentration maps of principal components. Important applications of single-frequency and hyperspectral CRS microscopy are highlighted. Potential directions of CRS microscopy are discussed.

    更新日期:2017-06-12
  • Advances in Magnetic Resonance Imaging Contrast Agents for Biomarker Detection
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Sanhita Sinharay, Mark D. Pagel

    Recent advances in magnetic resonance imaging (MRI) contrast agents have provided new capabilities for biomarker detection through molecular imaging. MRI contrast agents based on the T2 exchange mechanism have more recently expanded the armamentarium of agents for molecular imaging. Compared with T1 and T2* agents, T2 exchange agents have a slower chemical exchange rate, which improves the ability to design these MRI contrast agents with greater specificity for detecting the intended biomarker. MRI contrast agents that are detected through chemical exchange saturation transfer (CEST) have even slower chemical exchange rates. Another emerging class of MRI contrast agents uses hyperpolarized 13C to detect the agent with outstanding sensitivity. These hyperpolarized 13C agents can be used to track metabolism and monitor characteristics of the tissue microenvironment. Together, these various MRI contrast agents provide excellent opportunities to develop molecular imaging for biomarker detection.

    更新日期:2017-06-12
  • Progress in the Analysis of Complex Atmospheric Particles
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Alexander Laskin, Mary K. Gilles, Daniel A. Knopf, Bingbing Wang, Swarup China

    This article presents an overview of recent advances in field and laboratory studies of atmospheric particles formed in processes of environmental air-surface interactions. The overarching goal of these studies is to advance predictive understanding of atmospheric particle composition, particle chemistry during aging, and their environmental impacts. The diversity between chemical constituents and lateral heterogeneity within individual particles adds to the chemical complexity of particles and their surfaces. Once emitted, particles undergo transformation via atmospheric aging processes that further modify their complex composition. We highlight a range of modern analytical approaches that enable multimodal chemical characterization of particles with both molecular and lateral specificity. When combined, these approaches provide a comprehensive arsenal of tools for understanding the nature of particles at air-surface interactions and their reactivity and transformations with atmospheric aging. We discuss applications of these novel approaches in recent studies and highlight additional research areas to explore the environmental effects of air-surface interactions.

    更新日期:2017-06-12
  • Electroanalytical Ventures at Nanoscale Interfaces Between Immiscible Liquids
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Damien W.M. Arrigan, Yang Liu

    Ion transfer at the interface between immiscible electrolyte solutions offers many benefits to analytical chemistry, including the ability to detect nonredox active ionized analytes, to detect ions whose redox electrochemistry is accompanied by complications, and to separate ions based on electrocontrolled partition. Nanoscale miniaturization of such interfaces brings the benefits of enhanced mass transport, which in turn leads to improved analytical performance in areas such as sensitivity and limits of detection. This review discusses the development of such nanoscale interfaces between immiscible liquids and examines the analytical advances that have been made to date, including prospects for trace detection of ion concentrations.

    更新日期:2017-06-12
  • Reagentless, Structure-Switching, Electrochemical Aptamer-Based Sensors
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Lauren R. Schoukroun-Barnes, Florika C. Macazo, Brenda Gutierrez, Justine Lottermoser, Juan Liu, Ryan J. White

    The development of structure-switching, electrochemical, aptamer-based sensors over the past ∼10 years has led to a variety of reagentless sensors capable of analytical detection in a range of sample matrices. The crux of this methodology is the coupling of target-induced conformation changes of a redox-labeled aptamer with electrochemical detection of the resulting altered charge transfer rate between the redox molecule and electrode surface. Using aptamer recognition expands the highly sensitive detection ability of electrochemistry to a range of previously inaccessible analytes. In this review, we focus on the methods of sensor fabrication and how sensor signaling is affected by fabrication parameters. We then discuss recent studies addressing the fundamentals of sensor signaling as well as quantitative characterization of the analytical performance of electrochemical aptamer-based sensors. Although the limits of detection of reported electrochemical aptamer-based sensors do not often reach that of gold-standard methods such as enzyme-linked immunosorbent assays, the operational convenience of the sensor platform enables exciting analytical applications that we address. Using illustrative examples, we highlight recent advances in the field that impact important areas of analytical chemistry. Finally, we discuss the challenges and prospects for this class of sensors.

    更新日期:2017-06-12
  • New Functionalities for Paper-Based Sensors Lead to Simplified User Operation, Lower Limits of Detection, and New Applications
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Josephine C. Cunningham, Paul R. DeGregory, Richard M. Crooks

    In the last decade, paper analytical devices (PADs) have evolved into sophisticated yet simple sensors with biological and environmental applications in the developed and developing world. The focus of this review is the technological improvements that have over the past five years increased the applicability of PADs to real-world problems. Specifically, this review reports on advances in sample processing, fluid flow control, signal amplification, and component integration. Throughout, we have sought to emphasize advances that retain the main virtues of PADs: low cost, portability, and simplicity.

    更新日期:2017-06-12
  • Fabrication and Operation of Paper-Based Analytical Devices
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Xiao Jiang, Z. Hugh Fan

    This review focuses on the fabrication techniques and operational components of microfluidic paper-based analytical devices (μPADs). Being low-cost, user-friendly, fast, and simple, μPADs have seen explosive growth in the literature in the last decade. Many different materials and technologies have been employed to fabricate μPADs for various applications, including those that employ patterning, the creation of physical boundaries, and three-dimensional structures. In addition to fabrication techniques, flow control and other operational components in μPADs are of great interest. These components enable μPADs to control flow rates, direct flow paths via valves, sequentially deliver reagents automatically, and display test results, all of which will make μPADs more suitable for point-of-care applications.

    更新日期:2017-06-12
  • Glycan Arrays: From Basic Biochemical Research to Bioanalytical and Biomedical Applications
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Andreas Geissner, Peter H. Seeberger

    A major branch of glycobiology and glycan-focused biomedicine studies the interaction between carbohydrates and other biopolymers, most importantly, glycan-binding proteins. Today, this research into glycan-biopolymer interaction is unthinkable without glycan arrays, tools that enable high-throughput analysis of carbohydrate interaction partners. Glycan arrays offer many applications in basic biochemical research, for example, defining the specificity of glycosyltransferases and lectins such as immune receptors. Biomedical applications include the characterization and surveillance of influenza strains, identification of biomarkers for cancer and infection, and profiling of immune responses to vaccines. Here, we review major applications of glycan arrays both in basic and applied research. Given the dynamic nature of this rapidly developing field, we focus on recent findings.

    更新日期:2017-06-12
  • Microfluidic Devices for the Measurement of Cellular Secretion
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Adrian M. Schrell, Nikita Mukhitov, Lian Yi, Xue Wang, Michael G. Roper

    The release of chemical information from cells and tissues holds the key to understanding cellular behavior and dysfunction. The development of methodologies that can measure cellular secretion in a time-dependent fashion is therefore essential. Often these measurements are made difficult by the high-salt conditions of the cellular environment, the presence of numerous other secreted factors, and the small mass samples that are produced when frequent sampling is used to resolve secretory dynamics. In this review, the methods that we have developed for measuring hormone release from islets of Langerhans are dissected to illustrate the practical difficulties of studying cellular secretions. Other methods from the literature are presented that provide alternative approaches to particularly challenging areas of monitoring cellular secretion. The examples presented in this review serve as case studies and should be adaptable to other cell types and systems for unique applications.

    更新日期:2017-06-12
  • Plant Molecular Farming: Much More than Medicines
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Marc Tschofen, Dietmar Knopp, Elizabeth Hood, Eva Stöger

    Plants have emerged as commercially relevant production systems for pharmaceutical and nonpharmaceutical products. Currently, the commercially available nonpharmaceutical products outnumber the medical products of plant molecular farming, reflecting the shorter development times and lower regulatory burden of the former. Nonpharmaceutical products benefit more from the low costs and greater scalability of plant production systems without incurring the high costs associated with downstream processing and purification of pharmaceuticals. In this review, we explore the areas where plant-based manufacturing can make the greatest impact, focusing on commercialized products such as antibodies, enzymes, and growth factors that are used as research-grade or diagnostic reagents, cosmetic ingredients, and biosensors or biocatalysts. An outlook is provided on high-volume, low-margin proteins such as industrial enzymes that can be applied as crude extracts or unprocessed plant tissues in the feed, biofuel, and papermaking industries.

    更新日期:2017-06-12
  • Methods for the Analysis of Protein Phosphorylation–Mediated Cellular Signaling Networks
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Forest M. White, Alejandro Wolf-Yadlin

    Protein phosphorylation–mediated cellular signaling networks regulate almost all aspects of cell biology, including the responses to cellular stimulation and environmental alterations. These networks are highly complex and comprise hundreds of proteins and potentially thousands of phosphorylation sites. Multiple analytical methods have been developed over the past several decades to identify proteins and protein phosphorylation sites regulating cellular signaling, and to quantify the dynamic response of these sites to different cellular stimulation. Here we provide an overview of these methods, including the fundamental principles governing each method, their relative strengths and weaknesses, and some examples of how each method has been applied to the analysis of complex signaling networks. When applied correctly, each of these techniques can provide insight into the topology, dynamics, and regulation of protein phosphorylation signaling networks.

    更新日期:2017-06-12
  • Recent Progress in Monolithic Silica Columns for High-Speed and High-Selectivity Separations
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Tohru Ikegami, Nobuo Tanaka

    Monolithic silica columns have greater (through-pore size)/(skeleton size) ratios than particulate columns and fixed support structures in a column for chemical modification, resulting in high-efficiency columns and stationary phases. This review looks at how the size range of monolithic silica columns has been expanded, how high-efficiency monolithic silica columns have been realized, and how various methods of silica surface functionalization, leading to selective stationary phases, have been developed on monolithic silica supports, and provides information on the current status of these columns. Also discussed are the practical aspects of monolithic silica columns, including how their versatility can be improved by the preparation of small-sized structural features (sub-micron) and columns (1 mm ID or smaller) and by optimizing reaction conditions for in situ chemical modification with various restrictions, with an emphasis on recent research results for both topics.

    更新日期:2017-06-12
  • Mass-Selective Chiral Analysis
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Ulrich Boesl, Aras Kartouzian

    Three ways of realizing mass-selective chiral analysis are reviewed. The first is based on the formation of diastereomers that are of homo- and hetero- type with respect to the enantiomers of involved chiral molecules. This way is quite well-established with numerous applications. The other two ways are more recent developments, both based on circular dichroism (CD). In one, conventional or nonlinear electronic CD is linked to mass spectrometry (MS) by resonance-enhanced multiphoton ionization. The other is based on CD in the angular distribution of photoelectrons, which is measured in combination with MS via photoion photoelectron coincidence. Among the many important applications of mass-selective chiral analysis, this review focuses on its use as an analytical tool for the development of heterogeneous enantioselective chemical catalysis. There exist other approaches to combine chiral analysis and mass-selective detection, such as chiral chromatography MS, which are not discussed here.

    更新日期:2017-06-12
  • The Coupled Chemical and Physical Dynamics Model of MALDI
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Richard Knochenmuss

    The coupled physical and chemical dynamics model of ultraviolet matrix-assisted laser desorption/ionization (MALDI) has reproduced and explained a wide variety of MALDI phenomena. The rationale behind and elements of the model are reviewed, including the photophysics, kinetics, and thermodynamics of primary and secondary reaction steps. Experimental results are compared with model predictions to illustrate the foundations of the model, coupling of ablation and ionization, differences between and commonalities of matrices, secondary charge transfer reactions, ionization in both polarities, fluence and concentration dependencies, and suppression and enhancement effects.

    更新日期:2017-06-12
  • Advanced Multidimensional Separations in Mass Spectrometry: Navigating the Big Data Deluge
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Jody C. May, John A. McLean

    Hybrid analytical instrumentation constructed around mass spectrometry (MS) is becoming the preferred technique for addressing many grand challenges in science and medicine. From the omics sciences to drug discovery and synthetic biology, multidimensional separations based on MS provide the high peak capacity and high measurement throughput necessary to obtain large-scale measurements used to infer systems-level information. In this article, we describe multidimensional MS configurations as technologies that are big data drivers and review some new and emerging strategies for mining information from large-scale datasets. We discuss the information content that can be obtained from individual dimensions, as well as the unique information that can be derived by comparing different levels of data. Finally, we summarize some emerging data visualization strategies that seek to make highly dimensional datasets both accessible and comprehensible.

    更新日期:2017-06-12
  • Development and Applications of Liquid Sample Desorption Electrospray Ionization Mass Spectrometry
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Qiuling Zheng, Hao Chen

    Desorption electrospray ionization mass spectrometry (DESI-MS) is a recent advance in the field of analytical chemistry. This review surveys the development of liquid sample DESI-MS (LS-DESI-MS), a variant form of DESI-MS that focuses on fast analysis of liquid samples, and its novel analy-tical applications in bioanalysis, proteomics, and reaction kinetics. Due to the capability of directly ionizing liquid samples, liquid sample DESI (LS-DESI) has been successfully used to couple MS with various analytical techniques, such as microfluidics, microextraction, electrochemistry, and chromatography. This review also covers these hyphenated techniques. In addition, several closely related ionization methods, including transmission mode DESI, thermally assisted DESI, and continuous flow–extractive DESI, are briefly discussed. The capabilities of LS-DESI extend and/or complement the utilities of traditional DESI and electrospray ionization and will find extensive and valuable analytical application in the future.

    更新日期:2017-06-12
  • Mass Spectrometry Applied to Bottom-Up Proteomics: Entering the High-Throughput Era for Hypothesis Testing
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Ludovic C. Gillet, Alexander Leitner, Ruedi Aebersold

    Proteins constitute a key class of molecular components that perform essential biochemical reactions in living cells. Whether the aim is to extensively characterize a given protein or to perform high-throughput qualitative and quantitative analysis of the proteome content of a sample, liquid chromatography coupled to tandem mass spectrometry has become the technology of choice. In this review, we summarize the current state of mass spectrometry applied to bottom-up proteomics, the approach that focuses on analyzing peptides obtained from proteolytic digestion of proteins. With the recent advances in instrumentation and methodology, we show that the field is moving away from providing qualitative identification of long lists of proteins to delivering highly consistent and accurate quantification values for large numbers of proteins across large numbers of samples. We believe that this shift will have a profound impact for the field of proteomics and life science research in general.

    更新日期:2017-06-12
  • Mass Spectrometry as a Preparative Tool for the Surface Science of Large Molecules
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Stephan Rauschenbach, Markus Ternes, Ludger Harnau, Klaus Kern

    Measuring and understanding the complexity that arises when nanostructures interact with their environment are one of the major current challenges of nanoscale science and technology. High-resolution microscopy methods such as scanning probe microscopy have the capacity to investigate nanoscale systems with ultimate precision, for which, however, atomic scale precise preparation methods of surface science are a necessity. Preparative mass spectrometry (pMS), defined as the controlled deposition of m/z filtered ion beams, with soft ionization sources links the world of large, biological molecules and surface science, enabling atomic scale chemical control of molecular deposition in ultrahigh vacuum (UHV). Here we explore the application of high-resolution scanning probe microscopy and spectroscopy to the characterization of structure and properties of large molecules. We introduce the fundamental principles of the combined experiments electrospray ion beam deposition and scanning tunneling microscopy. Examples for the deposition and investigation of single particles, for layer and film growth, and for the investigation of electronic properties of individual nonvolatile molecules show that state-of-the-art pMS technology provides a platform analog to thermal evaporation in conventional molecular beam epitaxy. Additionally, it offers additional, unique features due to the use of charged polyatomic particles. This new field is an enormous sandbox for novel molecular materials research and demands the development of advanced molecular ion beam technology.

    更新日期:2017-06-12
  • Progress in Top-Down Proteomics and the Analysis of Proteoforms
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Timothy K. Toby, Luca Fornelli, Neil L. Kelleher

    From a molecular perspective, enactors of function in biology are intact proteins that can be variably modified at the genetic, transcriptional, or post-translational level. Over the past 30 years, mass spectrometry (MS) has become a powerful method for the analysis of proteomes. Prevailing bottom-up proteomics operates at the level of the peptide, leading to issues with protein inference, connectivity, and incomplete sequence/modification information. Top-down proteomics (TDP), alternatively, applies MS at the proteoform level to analyze intact proteins with diverse sources of intramolecular complexity preserved during analysis. Fortunately, advances in prefractionation workflows, MS instrumentation, and dissociation methods for whole-protein ions have helped TDP emerge as an accessible and potentially disruptive modality with increasingly translational value. In this review, we discuss technical and conceptual advances in TDP, along with the growing power of proteoform-resolved measurements in clinical and translational research.

    更新日期:2017-06-12
  • Proteogenomics: Integrating Next-Generation Sequencing and Mass Spectrometry to Characterize Human Proteomic Variation
    Annu. Rev. Anal. Chem. (IF 7.435) Pub Date : 2016-06-15
    Gloria M. Sheynkman, Michael R. Shortreed, Anthony J. Cesnik, Lloyd M. Smith

    Mass spectrometry–based proteomics has emerged as the leading method for detection, quantification, and characterization of proteins. Nearly all proteomic workflows rely on proteomic databases to identify peptides and proteins, but these databases typically contain a generic set of proteins that lack variations unique to a given sample, precluding their detection. Fortunately, proteogenomics enables the detection of such proteomic variations and can be defined, broadly, as the use of nucleotide sequences to generate candidate protein sequences for mass spectrometry database searching. Proteogenomics is experiencing heightened significance due to two developments: (a) advances in DNA sequencing technologies that have made complete sequencing of human genomes and transcriptomes routine, and (b) the unveiling of the tremendous complexity of the human proteome as expressed at the levels of genes, cells, tissues, individuals, and populations. We review here the field of human proteogenomics, with an emphasis on its history, current implementations, the types of proteomic variations it reveals, and several important applications.

    更新日期:2017-06-12
Some contents have been Reproduced with permission of the American Chemical Society.
Some contents have been Reproduced by permission of The Royal Society of Chemistry.
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