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Annual Review of Analytical Chemistry

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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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)...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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...
June 12, 2016: Annual Review of Analytical Chemistry
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