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Accounts of Chemical Research

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https://www.readbyqxmd.com/read/28094501/artificial-cells-synthetic-compartments-with-life-like-functionality-and-adaptivity
#1
Bastiaan C Buddingh', Jan C M van Hest
Cells are highly advanced microreactors that form the basis of all life. Their fascinating complexity has inspired scientists to create analogs from synthetic and natural components using a bottom-up approach. The ultimate goal here is to assemble a fully man-made cell that displays functionality and adaptivity as advanced as that found in nature, which will not only provide insight into the fundamental processes in natural cells but also pave the way for new applications of such artificial cells. In this Account, we highlight our recent work and that of others on the construction of artificial cells...
January 17, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28080028/a-grand-avenue-to-au-nanocluster-electrochemiluminescence
#2
Mahdi Hesari, Zhifeng Ding
In most cases of semiconductor quantum dot nanocrystals, the inherent optical and electrochemical properties of these interesting nanomaterials do not translate into expected efficient electrochemiluminescence or electrogenerated chemiluminescence (ECL) because of the surface-state induction effect. Thus, their low ECL efficiencies, while very interesting to explore, limit their applications. As their electrochemistry is not well-defined, insight into their ECL mechanistic details is also limited. Alternatively, gold nanoclusters possess monodispersed sizes with atomic precision, low and well defined HOMO-LUMO energy gaps, and stable optical and electrochemical properties that make them suitable for potential ECL applications...
January 12, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28075551/cucurbit-n-uril-based-microcapsules-self-assembled-within-microfluidic-droplets-a-versatile-approach-for-supramolecular-architectures-and-materials
#3
Ji Liu, Yang Lan, Ziyi Yu, Cindy S Y Tan, Richard M Parker, Chris Abell, Oren A Scherman
Microencapsulation is a fundamental concept behind a wide range of daily applications ranging from paints, adhesives, and pesticides to targeted drug delivery, transport of vaccines, and self-healing concretes. The beauty of microfluidics to generate microcapsules arises from the capability of fabricating monodisperse and micrometer-scale droplets, which can lead to microcapsules/particles with fine-tuned control over size, shape, and hierarchical structure, as well as high reproducibility, efficient material usage, and high-throughput manipulation...
January 11, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28071894/noninvasive-monitoring-of-blood-glucose-with-raman-spectroscopy
#4
Rishikesh Pandey, Santosh Kumar Paidi, Tulio A Valdez, Chi Zhang, Nicolas Spegazzini, Ramachandra Rao Dasari, Ishan Barman
The successful development of a noninvasive blood glucose sensor that can operate reliably over sustained periods of time has been a much sought after but elusive goal in diabetes management. Since diabetes has no well-established cure, control of elevated glucose levels is critical for avoiding severe secondary health complications in multiple organs including the retina, kidney and vasculature. While fingerstick testing continues to be the mainstay of blood glucose detection, advances in electrochemical sensing-based minimally invasive approaches have opened the door for alternate methods that would considerably improve the quality of life for people with diabetes...
January 10, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28068064/versatile-functionalization-of-polysaccharides-via-polymer-grafts-from-design-to-biomedical-applications
#5
Yang Hu, Yang Li, Fu-Jian Xu
Because of their biocompatibility, biodegradability, and unique bioactive properties, polysaccharides have been recognized and directly applied as excellent candidates for various biomedical applications. In order to introduce more functionalities onto polysaccharides, various modification methods were applied to improve the physical-chemical and biochemical properties. Grafting polysaccharides with functional polymers with limited reaction sites maximizes the structural integrity. To the best of our knowledge, great efforts have been made by scientists across the world, including our research group, to explore different strategies for the synthesis and design of controllable polymer-grafted polysaccharides...
January 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28068061/looking-at-photoinduced-charge-transfer-processes-in-the-ir-answers-to-several-long-standing-questions
#6
Bogdan Dereka, Marius Koch, Eric Vauthey
Because of its crucial role in many areas of science and technology, photoinduced electron transfer is the most investigated photochemical reaction. Despite this, several important questions remain open. We present recent efforts to answer some of them, which concern both inter- and intramolecular processes. The decisive factor that allowed these issues to be successfully addressed was the use of time-resolved infrared (TRIR) spectroscopy. Many different transient species, such as tight and loose ion pairs (TIPs and LIPs) and exciplexes, have been invoked to explain the dynamics of intermolecular photoinduced charge separation reactions (i...
January 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28068053/surface-modification-of-gold-nanoparticles-with-small-molecules-for-biochemical-analysis
#7
Yiping Chen, Yunlei Xianyu, Xingyu Jiang
As one of the major tools for and by chemical science, biochemical analysis is becoming increasingly important in fields like clinical diagnosis, food safety, environmental monitoring, and the development of chemistry and biochemistry. The advancement of nanotechnology boosts the development of analytical chemistry, particularly the nanoparticle (NP)-based approaches for biochemical assays. Functional NPs can greatly improve the performance of biochemical analysis because they can accelerate signal transduction, enhance the signal intensity, and enable convenient signal readout due to their unique physical and chemical properties...
January 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28067047/solvatochromic-and-fluorogenic-dyes-as-environment-sensitive-probes-design-and-biological-applications
#8
Andrey S Klymchenko
Fluorescent environment-sensitive probes are specially designed dyes that change their fluorescence intensity (fluorogenic dyes) or color (e.g., solvatochromic dyes) in response to change in their microenvironment polarity, viscosity, and molecular order. The studies of the past decade, including those of our group, have shown that these molecules become universal tools in fluorescence sensing and imaging. In fact, any biomolecular interaction or change in biomolecular organization results in modification of the local microenvironment, which can be directly monitored by these types of probes...
January 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28032510/ruthenium-catalyzed-ammonia-borane-dehydrogenation-mechanism-and-utility
#9
Xingyue Zhang, Lisa Kam, Ryan Trerise, Travis J Williams
One of the greatest challenges in using H2 as a fuel source is finding a safe, efficient, and inexpensive method for its storage. Ammonia borane (AB) is a solid hydrogen storage material that has garnered attention for its high hydrogen weight density (19.6 wt %) and ease of handling and transport. Hydrogen release from ammonia borane is mediated by either hydrolysis, thus giving borate products that are difficult to rereduce, or direct dehydrogenation. Catalytic AB dehydrogenation has thus been a popular topic in recent years, motivated both by applications in hydrogen storage and main group synthetic chemistry...
December 29, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28029779/hydrogel-droplet-microfluidics-for-high-throughput-single-molecule-cell-analysis
#10
Zhi Zhu, Chaoyong James Yang
Heterogeneity among individual molecules and cells has posed significant challenges to traditional bulk assays, due to the assumption of average behavior, which would lose important biological information in heterogeneity and result in a misleading interpretation. Single molecule/cell analysis has become an important and emerging field in biological and biomedical research for insights into heterogeneity between large populations at high resolution. Compared with the ensemble bulk method, single molecule/cell analysis explores the information on time trajectories, conformational states, and interactions of individual molecules/cells, all key factors in the study of chemical and biological reaction pathways...
December 28, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28009157/solar-water-splitting-and-nitrogen-fixation-with-layered-bismuth-oxyhalides
#11
Jie Li, Hao Li, Guangming Zhan, Lizhi Zhang
Hydrogen and ammonia are the chemical molecules that are vital to Earth's energy, environmental, and biological processes. Hydrogen with renewable, carbon-free, and high combustion-enthalpy hallmarks lays the foundation of next-generation energy source, while ammonia furnishes the building blocks of fertilizers and proteins to sustain the lives of plants and organisms. Such merits fascinate worldwide scientists in developing viable strategies to produce hydrogen and ammonia. Currently, at the forefronts of hydrogen and ammonia syntheses are solar water splitting and nitrogen fixation, because they go beyond the high temperature and pressure requirements of methane stream reforming and Haber-Bosch reaction, respectively, as the commercialized hydrogen and ammonia production routes, and inherit the natural photosynthesis virtues that are green and sustainable and operate at room temperature and atmospheric pressure...
December 23, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28004916/liquid-organic-hydrogen-carriers-lohcs-toward-a-hydrogen-free-hydrogen-economy
#12
Patrick Preuster, Christian Papp, Peter Wasserscheid
The need to drastically reduce CO2 emissions will lead to the transformation of our current, carbon-based energy system to a more sustainable, renewable-based one. In this process, hydrogen will gain increasing importance as secondary energy vector. Energy storage requirements on the TWh scale (to bridge extended times of low wind and sun harvest) and global logistics of renewable energy equivalents will create additional driving forces toward a future hydrogen economy. However, the nature of hydrogen requires dedicated infrastructures, and this has prevented so far the introduction of elemental hydrogen into the energy sector to a large extent...
December 22, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28001363/mass-spectrometry-imaging-of-complex-microbial-communities
#13
Sage J B Dunham, Joseph F Ellis, Bin Li, Jonathan V Sweedler
In the two decades since mass spectrometry imaging (MSI) was first applied to visualize the distribution of peptides across biological tissues and cells, the technique has become increasingly effective and reliable. MSI excels at providing complementary information to existing methods for molecular analysis-such as genomics, transcriptomics, and metabolomics-and stands apart from other chemical imaging modalities through its capability to generate information that is simultaneously multiplexed and chemically specific...
December 21, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28001359/multiconfiguration-pair-density-functional-theory-a-new-way-to-treat-strongly-correlated-systems
#14
Laura Gagliardi, Donald G Truhlar, Giovanni Li Manni, Rebecca K Carlson, Chad E Hoyer, Junwei Lucas Bao
The electronic energy of a system provides the Born-Oppenheimer potential energy for internuclear motion and thus determines molecular structure and spectra, bond energies, conformational energies, reaction barrier heights, and vibrational frequencies. The development of more efficient and more accurate ways to calculate the electronic energy of systems with inherently multiconfigurational electronic structure is essential for many applications, including transition metal and actinide chemistry, systems with partially broken bonds, many transition states, and most electronically excited states...
December 21, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28001034/the-o2-evolving-complex-of-photosystem-ii-recent-insights-from-quantum-mechanics-molecular-mechanics-qm-mm-extended-x-ray-absorption-fine-structure-exafs-and-femtosecond-x-ray-crystallography-data
#15
Mikhail Askerka, Gary W Brudvig, Victor S Batista
Efficient photoelectrochemical water oxidation may open a way to produce energy from renewable solar power. In biology, generation of fuel due to water oxidation happens efficiently on an immense scale during the light reactions of photosynthesis. To oxidize water, photosynthetic organisms have evolved a highly conserved protein complex, Photosystem II. Within that complex, water oxidation happens at the CaMn4O5 inorganic catalytic cluster, the so-called oxygen-evolving complex (OEC), which cycles through storage "S" states as it accumulates oxidizing equivalents and produces molecular oxygen...
December 21, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27997119/anisotropic-self-assembly-of-hairy-inorganic-nanoparticles
#16
Chenglin Yi, Shaoyi Zhang, Kyle Thomas Webb, Zhihong Nie
Current interest in functional assemblies of inorganic nanoparticles (NPs) stems from their collective properties and diverse applications ranging from nanomedicines to optically active metamaterials. Coating the surface of NPs with polymers allows for tailoring of the interactions between NPs to assemble them into hybrid nanocomposites with targeted architectures. This class of building blocks is termed "hairy" inorganic NPs (HINPs). Regiospecific attachment of polymers has been used to achieve directional interactions for HINP assembly...
December 20, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27992172/emissive-molecular-aggregates-and-energy-migration-in-luminescent-solar-concentrators
#17
James L Banal, Bolong Zhang, David J Jones, Kenneth P Ghiggino, Wallace W H Wong
Luminescent solar concentrators (LSCs) are light harvesting devices that are ideally suited to light collection in the urban environment where direct sunlight is often not available. LSCs consist of highly luminescent compounds embedded or coated on a transparent substrate that absorb diffuse or direct solar radiation over a large area. The resulting luminescence is trapped in the waveguide by total internal reflection to the thin edges of the substrate where the concentrated light can be used to improve the performance of photovoltaic devices...
December 19, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27991767/exploring-the-gas-phase-synthesis-of-the-elusive-class-of-boronyls-and-the-mechanism-of-boronyl-radical-reactions-under-single-collision-conditions
#18
Ralf I Kaiser, Nadia Balucani
Until recently, the chemistry of boronyl (BO), a diatomic radical isolectronic with the cyano (CN) species, has remained unknown. The boronyl group is characterized by a boron-oxygen multiple bond, and because of the inherent electron deficiency of the boron atom, boronyls (RBO) are highly reactive and typically only exist in their cyclotrimeric form (RBO)3. Due to their invaluable role as reactants, the isolation of the monomers in gas phase experiments has been extensively sought after by the organic synthesis and physical organic chemistry communities but never achieved...
December 19, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27983801/resonance-energy-transfer-in-upconversion-nanoplatforms-for-selective-biodetection
#19
Qianqian Su, Wei Feng, Dongpeng Yang, Fuyou Li
Resonance energy transfer (RET) describes the process that energy is transferred from an excited donor to an acceptor molecule, leading to a reduction in the fluorescence emission intensity of the donor and an increase in that of the acceptor. By this technique, measurements with the good sensitivity can be made about distance within 1 to 10 nm under physiological conditions. For this reason, the RET technique has been widely used in polymer science, biochemistry, and structural biology. Recently, a number of RET systems incorporated with nanoparticles, such as quantum dots, gold nanoparticles, and upconversion nanoparticles, have been developed...
December 16, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27977138/drugging-the-undruggable-therapeutic-potential-of-targeting-protein-tyrosine-phosphatases
#20
Zhong-Yin Zhang
Protein tyrosine phosphatases (PTPs) are essential signaling enzymes that, together with protein tyrosine kinases, regulate tyrosine phosphorylation inside the cell. Proper level of tyrosine phosphorylation is important for a diverse array of cellular processes, such as proliferation, metabolism, motility, and survival. Aberrant tyrosine phosphorylation, resulting from alteration of PTP expression, misregulation, and mutation, has been linked to the etiology of many human ailments including cancer, diabetes/obesity, autoimmune disorders, and infectious diseases...
December 15, 2016: Accounts of Chemical Research
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