Atomically dispersed metal catalysts (ADCs), as an emerging class of heterogeneous catalysts, have been widely investigated during the past two decades. The atomic dispersion nature of the catalytic ...metal centers makes them an ideal system for bridging homogeneous and heterogeneous metal catalysts. The recent rapid development of new synthetic strategies has led to the explosive growth of ADCs with a wide spectrum of metal atoms dispersed on supports of different chemical compositions and natures. The availability of diverse ADCs creates a powerful materials platform for investigating mechanisms of complicated heterogeneous catalysis at the atomic levels. Considering most dispersed metal atoms on ADCs are coordinated by the donors from supports, this review will demonstrate how the surface coordination chemistry plays an important role in determining the catalytic performance of ADCs. This review will start from the link between coordination chemistry and heterogeneous catalysis. After the brief description on the advantages and limitations of common structure characterization methods in determining the coordination structure of ADCs, the surface coordination chemistry of ADCs on different types of supports will be discussed. We will mainly illustrate how the local and vicinal coordination species on different support systems act together with the dispersed catalytic metal center to determine the catalytic activity, selectivity, and stability of ADCs. The dynamic coordination structure change of ADCs in catalysis will be highlighted. At the end of the review, personal perspectives on the further development of the field of ADCs will be provided.
Some infectious or malignant diseases such as cancers are seriously threatening the health of human beings all over the world. The commonly used antibiotic therapy cannot effectively treat these ...diseases within a short time, and also bring about adverse effects such as drug resistance and immune system damage during long-term systemic treatment. Phototherapy is an emerging antibiotic-free strategy to treat these diseases. Upon light irradiation, phototherapeutic agents can generate cytotoxic reactive oxygen species (ROS) or induce a temperature increase, which leads to the death of targeted cells. These two kinds of killing strategies are referred to as photodynamic therapy (PDT) and photothermal therapy (PTT), respectively. So far, many photo-responsive agents have been developed. Among them, the metal-organic framework (MOF) is becoming one of the most promising photo-responsive materials because its structure and chemical compositions can be easily modulated to achieve specific functions. MOFs can have intrinsic photodynamic or photothermal ability under the rational design of MOF construction, or serve as the carrier of therapeutic agents, owing to its tunable porosity. MOFs also provide feasibility for various combined therapies and targeting methods, which improves the efficiency of phototherapy. In this review, we firstly investigated the principles of phototherapy, and comprehensively summarized recent advances of MOF in PDT, PTT and synergistic therapy, from construction to modification. We expect that our demonstration will shed light on the future development of this field, and bring it one step closer to clinical trials.
Some infectious or malignant diseases such as cancers are seriously threatening the health of human beings all over the world.
Originally published, uncorrected article. https://doi.org/10.1371/journal.pone.0099918.s001 (PDF) File S2. Mayzel B, Aizenberg J, Ilan M (2014) The Elemental Composition of Demospongiae from the Red ...Sea, Gulf of Aqaba.
Against the backdrop of increased public health awareness, inorganic nanomaterials have been widely explored as promising nanoagents for various kinds of biomedical applications. Layered double ...hydroxides (LDHs), with versatile physicochemical advantages including excellent biocompatibility, pH-sensitive biodegradability, highly tunable chemical composition and structure, and ease of composite formation with other materials, have shown great promise in biomedical applications. In this review, we comprehensively summarize the recent advances in LDH-based nanomaterials for biomedical applications. Firstly, the material categories and advantages of LDH-based nanomaterials are discussed. The preparation and surface modification of LDH-based nanomaterials, including pristine LDHs, LDH-based nanocomposites and LDH-derived nanomaterials, are then described. Thereafter, we systematically describe the great potential of LDHs in biomedical applications including drug/gene delivery, bioimaging diagnosis, cancer therapy, biosensing, tissue engineering, and anti-bacteria. Finally, on the basis of the current state of the art, we conclude with insights on the remaining challenges and future prospects in this rapidly emerging field.
This review summarizes the recent advances in layered double hydroxide (LDH)-based nanomaterials for biomedical applications including drug/gene delivery, bioimaging diagnosis, cancer therapy, biosensing, tissue engineering, and anti-bacteria.
In Earth and planetary sciences, the chemical composition of chondritic meteorites provides an essential reference to constrain the composition and differentiation history of planetary reservoirs. ...Yet, for many trace elements, and in particular for volatile trace elements the composition of chondrites is not well constrained. Here we present new compositional data for carbonaceous chondrites with an emphasis on the origin of the volatile element depletion pattern. Our database includes 25 carbonaceous chondrites from 6 different groups (CI, CM, CR, CV, CO, CK), two ungrouped carbonaceous chondrites and Murchison powder samples heated up to 1000 °C in O2 or Ar gas streams, respectively. A total of 51 major and trace elements were analyzed by sector field inductively coupled plasma mass spectrometry (SF-ICP-MS), using chondrite-matched calibration solutions. Our results confirm that parent body alteration and terrestrial weathering only have minor effects on the bulk chondrite compositions. Thermal metamorphism can lead to the loss of some volatile elements, as best observed in the heating experiments and two thermally overprinted chondrites Y-980115 (CI) and EET 96026 (CV4/5 or CK4/5). The effects of aqueous alteration and terrestrial weathering on the Antarctic samples are difficult to discriminate. Both processes may redistribute fluid mobile elements such as K, Na, Rb, U and the light rare earth elements (LREE) within the meteorite. In hot desert finds, the typical weathering effects are enrichments of Sr, Ba and U and a depletion of S.
In general, moderately volatile elements with 50% condensation temperatures (TC) ranging from 1250 K to 800 K show an increasing depletion, whereas 11 moderately volatile elements with 50% TC between 800 K and 500 K are unfractionated from each other in most samples. Their extent of depletion is characteristic for the different chondrite groups. Because of this well-defined “hockey stick” pattern, we propose to divide the moderately volatile elements into two subgroups, the ‘slope volatile elements’ and the unfractionated ‘plateau volatile elements’ with lower TC. Notably, the abundances of plateau volatile elements exhibit a co-variation with the matrix abundances of the respective host meteorites. Carbonaceous chondrite matrices are likely mixes of: (i) CI-like material and (ii) chondrule-related matrix. Chondrule-related matrix is expected to be depleted in volatile elements relative to CI and likely formed contemporaneously with chondrules, leading to chondrule-matrix complementarity. The addition of CI-like material only changed the absolute elemental concentrations of bulk matrix and bulk chondrite, while refractory and main component element ratios such as Mg/Si remain unaffected. Such a model can also account for the co-existence of low temperature CI-like material and high temperature chondrule and chondrule-related matrix. However, elevated volatile element abundances observed in chondrules still provide a challenge for the model as proposed here.
A defining characteristic of nearly all catalytically functional MOFs is uniform, molecular-scale porosity. MOF pores, linkers and nodes that define them, help regulate reactant and product ...transport, catalyst siting, catalyst accessibility, catalyst stability, catalyst activity, co-catalyst proximity, composition of the chemical environment at and beyond the catalytic active site, chemical intermediate and transition-state conformations, thermodynamic affinity of molecular guests for MOF interior sites, framework charge and density of charge-compensating ions, pore hydrophobicity/hydrophilicity, pore and channel rigidity
flexibility, and other features and properties. Collectively and individually, these properties help define overall catalyst functional behaviour. This review focuses on how porous, catalyst-containing MOFs capitalize on molecular-scale confinement, containment, isolation, environment modulation, energy delivery, and mobility to accomplish desired chemical transformations with potentially superior selectivity or other efficacy, especially in comparison to catalysts in homogeneous solution environments.
Lupins are an excellent source of protein which can be used to obtain protein isolates with potential use in the food industry. Some studies use supercritical CO2 (SC-CO2) to defat legume flours, but ...no study analyzes the effect of applying this technology directly to the protein isolate. This article has proposed the use of SC-CO2 to improve lupin protein isolate (LPI) quality. SC-CO2 increased the LPI purity while reducing oil and other antitechnological factors (saponins and polyphenols). The treatment significantly improved the LPI color due to the elimination of the lipid fraction and lipophilic pigments (carotenoids). No changes in amino acid contents or chemical score were observed due to the SC-CO2. Finally, the treatment improved or did not affect the main LPI technofunctional properties. Therefore, SC-CO2 is a promising technique to enhance the quality of protein isolates, without affecting or improving their functional properties.
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•The SC-CO2 treatment increases the purity of lupin protein isolate (LPI)•The SC-CO2 treatment did not modify the LPI amino acids profile & nutritional quality•The SC-CO2 improves LPI color by dramatic reduction of a* and b* parameters•The SC-CO2 improve or did not affect the technofunctional properties of LPI•Lupin protein isolate is a valuable resource for functional food ingredients
Heteroatom-doped porous carbon materials (HPCMs) have found extensive applications in adsorption/separation, organic catalysis, sensing, and energy conversion/storage. The judicious choice of carbon ...precursors is crucial for the manufacture of HPCMs with specific usages and maximization of their functions. In this regard, polymers as precursors have demonstrated great promise because of their versatile molecular and nanoscale structures, modulatable chemical composition, and rich processing techniques to generate textures that, in combination with proper solid-state chemistry, can be maintained throughout carbonization. This Review comprehensively surveys the progress in polymer-derived functional HPCMs in terms of how to produce and control their porosities, heteroatom doping effects, and morphologies and their related use. First, we summarize and discuss synthetic approaches, including hard and soft templating methods as well as direct synthesis strategies employing polymers to control the pores and/or heteroatoms in HPCMs. Second, we summarize the heteroatom doping effects on the thermal stability, electronic and optical properties, and surface chemistry of HPCMs. Specifically, the heteroatom doping effect, which involves both single-type heteroatom doping and codoping of two or more types of heteroatoms into the carbon network, is discussed. Considering the significance of the morphologies of HPCMs in their application spectrum, potential choices of suitable polymeric precursors and strategies to precisely regulate the morphologies of HPCMs are presented. Finally, we provide our perspective on how to predefine the structures of HPCMs by using polymers to realize their potential applications in the current fields of energy generation/conversion and environmental remediation. We believe that these analyses and deductions are valuable for a systematic understanding of polymer-derived carbon materials and will serve as a source of inspiration for the design of future HPCMs.
Wuhan was the first city to adopt the lockdown measures to prevent COVID-19 spreading, which improved the air quality accordingly. This study investigated the variations in chemical compositions, ...source contributions, and regional transport of fine particles (PM2.5) during January 23–February 22 of 2020, compared with the same period in 2019. The average mass concentration of PM2.5 decreased from 72.9 μg m−3 (2019) to 45.9 μg m−3 (2020), by 27.0 μg m−3. It was predominantly contributed by the emission reduction (92.0%), retrieved from a random forest tree approach. The main chemical species of PM2.5 all decreased with the reductions ranging from 0.85 μg m−3 (chloride) to 9.86 μg m−3 (nitrate) (p < 0.01). Positive matrix factorization model indicated that the mass contributions of seven PM2.5 sources all decreased. However, their contribution percentages varied from −11.0% (industrial processes) to 8.70% (secondary inorganic aerosol). Source contributions of PM2.5 transported from potential geographical regions showed reductions with mean values ranging from 0.22 to 4.36 μg m−3. However, increased contributions of firework burning, secondary inorganic aerosol, road dust, and vehicle emissions from transboundary transport were observed. This study highlighted the complex and nonlinear response of chemical compositions and sources of PM2.5 to air pollution control measures, suggesting the importance of regional-joint control.
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•Differences in PM2.5 chemical species and sources since lockdown were reported.•Primary emission reduced while secondary formation enhanced since lockdown.•Emission reduction dominated the improvement of air quality in Wuhan during lockdown.
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