Heterogeneous hydrogenation reactions are of great importance for chemical upgrading and synthesis, but still face the challenges of controlling selectivity and long‐term stability. To improve the ...catalytic performance, many hydrogenation reactions utilize special yolk/core–shell nanoreactors (YCSNs) with unique architectures and advantageous properties. This work presents the developmental and technological challenges in the preparation of YCSNs that are potentially useful for hydrogenation reactions, and provides a summary of the properties of these materials. The work also addresses the scientific challenges in applications of these YCSNs in various gas and liquid‐phase hydrogenation reactions. The catalyst structures, catalytic performance, structure–performance relationships, reaction mechanisms, and unsolved problems are discussed too. Also, a brief outlook and opportunities for future research in this field are presented. This work on the advancements in YCSNs might inspire the creation of new materials with desired structures for achieving maximal hydrogenation performances.
This work presents recent progress and challenges in the development of yolk/core–shell nanoreactors (YCSNs) for gas‐phase hydrogenation of CO/CO2 and liquid‐phase hydrogenation of alkenes, alkynes, aromatics, and biomass for the production of liquid fuels and renewable chemicals.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Inspired by natural mobile microorganisms, researchers have developed micro/nanomotors (MNMs) that can autonomously move by transducing different kinds of energies into kinetic energy. The rapid ...development of MNMs has created tremendous opportunities for biomedical fields including diagnostics, therapeutics, and theranostics. Although the great progress has been made in MNM research, at a fundamental level, the accepted propulsion mechanisms are still a controversial matter. In practical applications such as precision nanomedicine, the precise control of the motion, including the speed and directionality, of MNMs is also important, which makes advanced motion manipulation desirable. Very recently, diverse MNMs with different propulsion strategies, morphologies, sizes, porosities and chemical structures have been fabricated and applied for various uses. Herein, we thoroughly summarize the physical principles behind propulsion strategies, as well as the recent advances in motion manipulation methods and relevant biomedical applications of these MNMs. The current challenges in MNM research are also discussed. We hope this review can provide a bird's eye overview of the MNM research and inspire researchers to create novel and more powerful MNMs.
Micro/nanomotors with advanced motion manipulation show great promise in biomedical fields. This review article critically summarizes the working principles, manipulation strategies, biomedical applications, and future prospects of micro/nanomotors.
Photocatalysis offers a sustainable strategy for hydrogen peroxide (H2O2) production, which is an essential oxidant and emerging energy carrier in modern chemical industry. The development of ...polymer‐based photocatalysts to produce H2O2 has great potential but is limited by lower efficiency due to the limitation of light utilization and the low charge separation efficiency. Herein, a series of monodispersed mesoporous resorcinol‐formaldehyde resin spheres (MRFS) are reported with a rational designed spatial charge distribution, exhibiting wide light absorption with a solar‐to‐chemical conversion (SCC) efficiency of 1.1%. Surface photovoltage microscopy (SPVM) measurements unraveled the charge separation in nanospace with uneven distribution of donor (D) and acceptor (A) sites. A density functional theory (DFT) calculation elucidated the origin of photogenerated electrons and holes. Moreover, MRFS demonstrates photocatalytic water oxidation ability. The findings in this work open a new avenue for the development of porous polymeric photocatalysts toward highly efficient solar energy conversion.
A series of phenolic resin spheres with different meso‐structures have been developed as state‐of‐art porous polymeric photocatalysts with a solar‐to‐chemical conversion (SCC) efficiency of 1.1% for H2O2 production. These phenolic resin spheres have an uneven distribution of donor (D) and acceptor (A) sites, providing new insights into the nanospatial charge modulation.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
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•The design strategies of NPCSPs were systematically summarized.•The representative progresses for the synthesis of NPCSPs were presented.•A series of typical applications in ...bio-adsorption and bio-catalysis were highlighted.•The current challenges and perspectives on the future research directions were proposed.
Core@shell particles with controlled structure and morphology are gradually attracting attention due to their unique properties and potential applications related to electronics, catalysis, sustainability and biomedicine. In particular, the design of nanoporous core@shell particles has emerged as a key focus in recent years because of their ultra-high surface area, tunable porous structure and orientation, which play vital roles in bioadsorption and biocatalysis. In this review, we start with a brief introduction of the structures and properties of nanoporous core@shell particles, followed by a summary of their application in bioadsorption and biocatalysis. Then, we surveyed the design and preparation of these core@shell particles, including the structure and surface chemistry that will affect the particles function in bioadsorption and biocatalysis which is then correlated with the synthesis methods. Finally, we highlight the bioadsorption and biocatalysis application of nanoporous core@shell particles, how they benefit from their physical characteristics (i.e. porosity and size) before concluding with perspectives on the future directions for this topic. There is great potential for nanoporous core@shell particles to reach high biomolecular loading capacities for bioadsorption applications as well as improved catalytic efficiencies as biocatalytic materials due to their unique nanostructure, composition and biocompatibility. This review aims to guide researchers towards understanding the latest research progress in these fields, with the ultimate goal being to influence future developments in these areas.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Hollow nanostructures with fascinating properties have inspired numerous interests in broad research fields. Cell‐mimicking complex hollow architectures with precise active components distributions ...are particularly important, while their synthesis remains highly challenging. Herein, a “top‐down” chemical surgery strategy is introduced to engrave the 3‐aminophenol formaldehyde resin (APF) spheres at nanoscale. Undergoing the cleavage of (Ar)CN bonds with ethanol as chemical scissors and subsequent repolymerization process, the Solid APF transform to multilevel hollow architecture with precise nanospatial distribution of organic functional groups (e.g., hydroxymethyl and amine). The transformation is tracked by electron microscopy and solid‐state nuclear magnetic resonance techniques, the category and dosage of alcohol are pivotal for constructing multilevel hollow structures. Moreover, it is demonstrated the evolution of nanostructures accompanied with unique organic microenvironments is able to accurately confine multiple gold (Au) nanoparticles, leading to the formation of pomegranate‐like particles. Through selectively depositing palladium (Pd) nanoparticles onto the outer shell, bimetallic Au@APF@Pd catalysts are formed, which exhibit excellent hydrogenation performance with turnover frequency (TOF) value up to 11257 h–1. This work provides an effective method for precisely manipulating the nanostructure and composition of polymers at nanoscale and sheds light on the design of catalysts with precise spatial active components.
A nanoscale chemical surgery is reported on phenolic resins based on a dissolution and repolymerization procedure, to construct multilevel hollow structures with well‐defined functional groups. Those special architectures are useful in the fabrication of novel nanomaterials, Au@APF composites, with Au nanoparticles fully embedded within the spheres, which are well suited to architect the bimetallic catalyst with remarkable hydrogenation activity.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
High cholesterol levels greatly increase the risk of cardiovascular disease. About 50 per cent of cholesterol is eliminated from the body by its conversion into bile acids. However, bile acids ...released from the bile duct are constantly recycled, being reabsorbed in the intestine by the apical sodium-dependent bile acid transporter (ASBT, also known as SLC10A2). It has been shown in animal models that plasma cholesterol levels are considerably lowered by specific inhibitors of ASBT, and ASBT is thus a target for hypercholesterolaemia drugs. Here we report the crystal structure of a bacterial homologue of ASBT from Neisseria meningitidis (ASBT(NM)) at 2.2 Å. ASBT(NM) contains two inverted structural repeats of five transmembrane helices. A core domain of six helices harbours two sodium ions, and the remaining four helices pack in a row to form a flat, 'panel'-like domain. Overall, the architecture of the protein is remarkably similar to the sodium/proton antiporter NhaA, despite having no detectable sequence homology. The ASBT(NM) structure was captured with the substrate taurocholate present, bound between the core and panel domains in a large, inward-facing, hydrophobic cavity. Residues near this cavity have been shown to affect the binding of specific inhibitors of human ASBT. The position of the taurocholate molecule, together with the molecular architecture, suggests the rudiments of a possible transport mechanism.
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DOBA, IJS, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Chemotherapy is a primary cancer treatment strategy, the monitoring of which is critical to enhancing the survival rate and quality of life of cancer patients. However, current chemotherapy ...monitoring mainly relies on imaging tools with inefficient sensitivity and radiation invasiveness. Herein, we develop the bowl-shaped submicroreactor chip of Au-loaded 3-aminophenol formaldehyde resin (denoted as APF-bowl&Au) with a specifically designed structure and Au loading content. The obtained APF-bowl&Au, used as the matrix of laser desorption/ionization mass spectrometry (LDI MS), possesses an enhanced localized electromagnetic field for strengthened small metabolite detection. The APF-bowl&Au enables the extraction of serum metabolic fingerprints (SMFs), and machine learning of the SMFs achieves chemotherapy monitoring of ovarian cancer with area-under-the-curve (AUC) of 0.81–0.98. Furthermore, a serum metabolic biomarker panel is preliminarily identified, exhibiting gradual changes as the chemotherapy cycles proceed. This work provides insights into the development of nanochips and contributes to a universal detection platform for chemotherapy monitoring.
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IJS, KILJ, NUK, PNG, UL, UM
Background
The diagnosis of periprosthetic joint infection (PJI) remains a serious clinical challenge. There is a pressing need for improved diagnostic testing methods; biomarkers offer one ...potentially promising approach.
Questions/purposes
We evaluated the diagnostic characteristics of 16 promising synovial fluid biomarkers for the diagnosis of PJI.
Methods
Synovial fluid was collected from 95 patients meeting the inclusion criteria of this prospective diagnostic study. All patients were being evaluated for a revision hip or knee arthroplasty, including patients with systemic inflammatory disease and those already receiving antibiotic treatment. The Musculoskeletal Infection Society (MSIS) definition was used to classify 29 PJIs and 66 aseptic joints. Synovial fluid samples were tested by immunoassay for 16 biomarkers optimized for use in synovial fluid. Sensitivity, specificity, and receiver operating characteristic curve analysis were performed to assess for diagnostic performance.
Results
Five biomarkers, including human α-defensin 1-3, neutrophil elastase 2, bactericidal/permeability-increasing protein, neutrophil gelatinase-associated lipocalin, and lactoferrin, correctly predicted the MSIS classification of all patients in this study, with 100% sensitivity and specificity for the diagnosis of PJI. An additional eight biomarkers demonstrated excellent diagnostic strength, with an area under the curve of greater than 0.9.
Conclusions
Synovial fluid biomarkers exhibit a high accuracy in diagnosing PJI, even when including patients with systemic inflammatory disease and those receiving antibiotic treatment. Considering that these biomarkers match the results of the more complex MSIS definition of PJI, we believe that synovial fluid biomarkers can be a valuable addition to the methods utilized for the diagnosis of infection.
Level of Evidence
Level II, diagnostic study. See Instructions for Authors for a complete description of levels of evidence.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NUK, OBVAL, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
5‐hydroxymethylfurfural represents a key chemical in the drive towards a sustainable circular economy within the chemical industry. The final step in 5‐hydroxymethylfurfural production is the acid ...catalysed dehydration of fructose, for which supported organoacids are excellent potential catalyst candidates. Here we report a range of solid acid catalysis based on sulphonic acid grafted onto different porous silica nanosphere architectures, as confirmed by TEM, N2 porosimetry, XPS and ATR‐IR. All four catalysts display enhanced active site normalised activity and productivity, relative to alternative silica supported equivalent systems in the literature, with in‐pore diffusion of both substrate and product key to both performance and humin formation pathway. An increase in‐pore diffusion coefficient of 5‐hydroxymethylfurfural within wormlike and stellate structures results in optimal productivity. In contrast, poor diffusion within a raspberry‐like morphology decreases rates of 5‐hydroxymethylfurfural production and increases its consumption within humin formation.
Sulphonic acid (RSO3H) functionalized porous silica nanospheres show high catalytic activity towards selective dehydration of fructose to 5‐hydroxymethylfurfural with pore architecture dictating performance and susceptibility to deactivation via humin by‐product formation. Catalyst performance is governed by in‐pore diffusion of substrate and product, which are assessed by diffusion NMR.
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FZAB, GIS, IJS, IZUM, KILJ, NLZOH, NUK, OILJ, PILJ, PNG, SAZU, SBCE, SBMB, UL, UM, UPUK
10.
Overcoming the challenges of membrane protein crystallography Carpenter, Elisabeth P; Beis, Konstantinos; Cameron, Alexander D ...
Current opinion in structural biology,
October 2008, 2008-Oct, 2008-10-00, 20081001, Volume:
18, Issue:
5
Journal Article
Peer reviewed
Open access
Membrane protein structural biology is still a largely unconquered area, given that approximately 25% of all proteins are membrane proteins and yet less than 150 unique structures are available. ...Membrane proteins have proven to be difficult to study owing to their partially hydrophobic surfaces, flexibility and lack of stability. The field is now taking advantage of the high-throughput revolution in structural biology and methods are emerging for effective expression, solubilisation, purification and crystallisation of membrane proteins. These technical advances will lead to a rapid increase in the rate at which membrane protein structures are solved in the near future.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
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