Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition be...Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.展开更多
Due to the complicated film formation kinetics, morphology control remains a major challenge for the development of efficient and stable all-polymer solar cells(all-PSCs). To overcome this obstacle, the sequential dep...Due to the complicated film formation kinetics, morphology control remains a major challenge for the development of efficient and stable all-polymer solar cells(all-PSCs). To overcome this obstacle, the sequential deposition method is used to fabricate the photoactive layers of all-PSCs comprising a polymer donor PTzBI-oF and a polymer acceptor PS1. The film morphology can be manipulated by incorporating amounts of a dibenzyl ether additive into the PS1 layer. Detailed morphology investigations by grazing incidence wide-angle X-ray scattering and a transmission electron microscope reveal that the combination merits of sequential deposition and DBE additive can render favorable crystalline properties as well as phase separation for PTzBI-oF:PS1 blends. Consequently, the optimized all-PSCs delivered an enhanced power conversion efficiency(PCE) of 15.21%along with improved carrier extraction and suppressed charge recombination. More importantly, the optimized all-PSCs remain over 90% of their initial PCEs under continuous thermal stress at 65 °C for over 500 h. This work validates that control over microstructure morphology via a sequential deposition process is a promising strategy for fabricating highly efficient and stable all-PSCs.展开更多
Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)...Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.展开更多
Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structur...Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structural and dynamic details.Herein,we commence with a brief introduction to recent research on lithium-ion battery oxide materials studied using ^(17)O solid-state NMR spectroscopy.Then we delve into a review of ^(17)O isotopic labeling methods for tagging oxygen sites in both the bulk and surfaces of metal oxides.At last,the unresolved problems and the future research directions for advancing the ^(17)O labeling technique are discussed.展开更多
The objective of this study was to improve the dissolution and bioavailability of silymarin(SM).Solid dispersions(SDs)were prepared using solution-enhanced dispersion by supercritical fluids(SEDS)and evaluated in vitr...The objective of this study was to improve the dissolution and bioavailability of silymarin(SM).Solid dispersions(SDs)were prepared using solution-enhanced dispersion by supercritical fluids(SEDS)and evaluated in vitro and in vivo,compared with pure SM powder.The particle sizes,stability,and contents of residual solvent of the prepared SM-SDs with SEDS and solvent evaporation(SE)were investigated.Four polymer matrix materials were evaluated for the preparation of SM-SD-SEDS,and the hydrophilic polymer,polyvinyl pyrrolidone K17,was selected with a ratio of 1:5 between SM and the polymer.Physicochemical analyses using X-ray diffraction and differential scanning calorimetry indicated that SM was dispersed in SD in an amorphous state.The optimized SM-SD-SEDS showed no loss of SM after storage for 6 months and negligible residual solvent(ethanol)was detected using gas chromatography.In vitro drug release was increased from the SM-SDSEDS,as compared with pure SM powder or SM-SD-SE.In vivo,the area under the rat plasma SM concentration-time curve and the maximum plasma SM concentration were 2.4-fold and 1.9-fold higher,respectively,after oral administration of SM-SD-SEDS as compared with an aqueous SM suspension.These results illustrated the potential of using SEDS to prepare SM-SD,further improving the biopharmaceutical properties of this compound.展开更多
The activation of iron oxide Fischer–Tropsch Synthesis(FTS) catalysts was investigated during pretreatment: reduction in hydrogen followed by carburization in either CO or syngas mixture, or simultaneously reduction ...The activation of iron oxide Fischer–Tropsch Synthesis(FTS) catalysts was investigated during pretreatment: reduction in hydrogen followed by carburization in either CO or syngas mixture, or simultaneously reduction and carburization in syngas. A combination of different complementary in situ techniques was used to gain insight into the behavior of Fe-based FTS catalysts during activation. In situ XRD was used to identify the crystalline structures present during both reduction in hydrogen and carburization. An increase in reduction rate was established when increasing the temperature. A complete reduction was demonstrated in the ETEM and a grain size dependency was proven, i.e. bigger grains need higher temperature in order to reduce. XPS and XAS both indicate the formation of a small amount of carbonaceous species at the surface of the bulk metallic iron during carburization.展开更多
Morphology control of perovskite films is of critical importance for high-performance photovoltaic devices. Although solvent vapor annealing(SVA) treatment has been widely used to improve the film quality efficiently,...Morphology control of perovskite films is of critical importance for high-performance photovoltaic devices. Although solvent vapor annealing(SVA) treatment has been widely used to improve the film quality efficiently, the detailed mechanism of film growth is still under construction, and there is still no consensus on the selection of solvents and volume for further optimization. Here, a series of solvents(DMF, DMSO, mixed DMF/DMSO) were opted for exploring their impact on fundamental structural and physical properties of perovskite films and the performance of corresponding devices. Mixed solvent SVA treatment resulted in unique benefits that integrated the advantages of each solvent, generating a champion device efficiency of 19.76% with improved humidity and thermal stability. The crystallization mechanism was constructed by conducting grazing-incidence wide-angle x-ray diffraction(GIWAXS) characterizations, showing that dissolution and recrystallization dominated the film formation. A proper choice of solvent and its volume balancing the two processes thus afforded the desired perovskite film. This study reveals the underlying process of film formation, paving the way to producing energy-harvesting materials in a controlled manner towards energy-efficient and stable perovskite-based devices.展开更多
The recent discovery of room temperature superconductivity(283 K)in carbonaceous sulfur hydride(C-S-H)has attracted much interest in ternary hydrogen rich materials.In this report,ternary hydride P-S-H was synthesized...The recent discovery of room temperature superconductivity(283 K)in carbonaceous sulfur hydride(C-S-H)has attracted much interest in ternary hydrogen rich materials.In this report,ternary hydride P-S-H was synthesized through a photothermal-chemical reaction from elemental sulfur(S),phosphorus(P)and molecular hydrogen(H_(2))at high pressures and room temperature.Raman spectroscopy under pressure shows that H_(2)S and PH_(3) compounds are synthesized after laser heating at 0.9 GPa,and a ternary van der Waals compound P-S-H is synthesized with further compression to 4.6 GPa.The P-S-H compound is probably a mixed alloy of PH_(3) and(H_(2)S)_(2)H_(2) with a guest-host structure similar to the C-S-H system.The ternary hydride can persist up to 35.6 GPa at least and shows two phase transitions at approximately 23.6 GPa and 32.8 GPa,respectively.展开更多
Physical and chemical properties of wool surface significantly affect the absorbency,rate of dye bath exhaustion and fixation of the industrial dyes.Hence,surface modification is a necessary operation prior to colorat...Physical and chemical properties of wool surface significantly affect the absorbency,rate of dye bath exhaustion and fixation of the industrial dyes.Hence,surface modification is a necessary operation prior to coloration process in wool wet processing industries.Plasma treatment is an effective alternative for physiochemical modification of wool surface.However,optimum processing parameters to get the expected modification are still under investigation,hence this technology is still under development in the wool wet processing industries.Therefore,in this paper,treatment parameters with the help of simple dielectric barrier discharge plasma reactor and air as a plasma gas,which could be a promising combination for treatment of wool substrate at industrial scale were schematically studied,and their influence on the water absorbency,mechanical,and dyeing properties of twill woven wool fabric samples are reported.It is expected that the results will assist to the wool coloration industries to improve the dyeing processes.展开更多
A series of 1,2,4-triazole derivatives were synthesized, and their abilities to inhibit the in vitro replication of Coxsackie B3/B6 were evaluated. Among the 1,2,4-triazole derivatives, compound 3 g displayed potent a...A series of 1,2,4-triazole derivatives were synthesized, and their abilities to inhibit the in vitro replication of Coxsackie B3/B6 were evaluated. Among the 1,2,4-triazole derivatives, compound 3 g displayed potent activity, with a high antiviral potency (IC50 = 1.71 μM (against CVB3), 1.43 μM (against CVB6)). The structures of all the new synthesized compounds were confirmed by 1H-NMR spectra, mass spectra and elemental analyses.展开更多
Aqueous zinc-ion battery(ZIB)featuring with high safety,low cost,environmentally friendly,and high energy density is one of the most promising systems for large-scale energy storage application.Despite extensive resea...Aqueous zinc-ion battery(ZIB)featuring with high safety,low cost,environmentally friendly,and high energy density is one of the most promising systems for large-scale energy storage application.Despite extensive research progress made in developing high-performance cathodes,the Zn anode issues,such as Zn dendrites,corrosion,and hydrogen evolution,have been observed to shorten ZIB’s lifespan seriously,thus restricting their practical application.Engineering advanced Zn anodes based on two-dimensional(2D)materials are widely investigated to address these issues.With atomic thickness,2D materials possess ultrahigh specific surface area,much exposed active sites,superior mechanical strength and flexibility,and unique electrical properties,which confirm to be a promising alternative anode material for ZIBs.This review aims to boost rational design strategies of 2D materials for practical application of ZIB by combining the fundamental principle and research progress.Firstly,the fundamental principles of 2D materials against the drawbacks of Zn anode are introduced.Then,the designed strategies of several typical 2D materials for stable Zn anodes are comprehensively summarized.Finally,perspectives on the future development of advanced Zn anodes by taking advantage of these unique properties of 2D materials are proposed.展开更多
The charge carrier concentration profile is a critical factor that determines semiconducting material properties and device performance.Dielectric force microscopy(DFM)has been previously developed to map charge carri...The charge carrier concentration profile is a critical factor that determines semiconducting material properties and device performance.Dielectric force microscopy(DFM)has been previously developed to map charge carrier concentrations with nanometer-scale spatial resolution.However,it is challenging to quantitatively obtain the charge carrier concentration,since the dielectric force is also affected by the mobility.Here,we quantitative measured the charge carrier concentration at the saturation mobility regime via the rectification effect-dependent gating ratio of DFM.By measuring a series of n-type GaAs and GaN thin films with mobility in the saturation regime,we confirmed the decreased DFM-measured gating ratio with increasing electron concentration.Combined with numerical simulation to calibrate the tip–sample geometry-induced systematic error,the quantitative correlation between the DFM-measured gating ratio and the electron concentration has been established,where the extracted electron concentration presents high accuracy in the range of 4×10^(16)–1×10^(18)cm^(-3).We expect the quantitative DFM to find broad applications in characterizing the charge carrier transport properties of various semiconducting materials and devices.展开更多
The ionic transport in sub-nanochannels plays a key role in energy storage,yet suffers from a high energy barrier.Wetting sub-nanochannels is crucial to accelerate ionic transport,but the introduction of water is chal...The ionic transport in sub-nanochannels plays a key role in energy storage,yet suffers from a high energy barrier.Wetting sub-nanochannels is crucial to accelerate ionic transport,but the introduction of water is challenging because of the hydrophobic extreme confinement.We propose wetting the channels by the exothermic hydration process of pre-intercalated ions,the effect of which varies distinctly with different ionic hydration structures and energies.Compared to the failed pre-intercalation of SO_(4)^(2-),HSO_(4)^(-) with weak hydration energy results in a marginal effect on the HOMO(Highest Occupied Molecular Orbital)level of water to avoid water splitting during the electrochemical intercalation.Meanwhile,the ability of water introduction is reserved by the initial incomplete dissociation state of HSO_(4)^(-),so the consequent exothermic reionization and hydration processes of the intercalated HSO_(4)^(-) promote the water introduction into sub-nanochannels,finally forming the stable confined water through hydrogen bonding with functional groups.The wetted channels exhibit a significantly enhanced ionic diffusion coef-ficient by~9.4 times.展开更多
Aiming at accessing polyethylene-bearing in-chain degradable functionality,copolymerization of carbon dioxide(CO_(2))with ethylene has long been recognized as a significant but highly challenging transformation.Nevert...Aiming at accessing polyethylene-bearing in-chain degradable functionality,copolymerization of carbon dioxide(CO_(2))with ethylene has long been recognized as a significant but highly challenging transformation.Nevertheless,most trials have resulted in ethylene homopolymerization because of the endothermic property and high energy barriers of CO_(2)insertion during polymer chain propagation.Here we report an unprecedented tandem reaction protocol for the synthesis of polyethylenes with in-chain carbonyls from CO_(2)and ethylene by the combination of photocatalytic CO_(2)reduction and palladium-catalyzed coordination/insertion polymerization.This protocol provides an easy way to adjust the carbonyl content(from 0.13 to 12 mol%)and insertion selectivity(up to 99%isolated carbonyls)of the polyethylene copolymers,which enables the polymers tomaintain the main properties of highdensity polyethylene and simultaneously endows them with good photodegradability.In addition,besides apolar polyethylene copolymers,polar-functionalized polyethylenes with in-chain isolated carbonyls can also be synthesized from CO_(2),ethylene and a polar monomer using the same protocol.We believe our present work sheds new light on the synthesis of degradable polyethylenes by employing CO_(2)as a green carbonyl source.展开更多
Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge proce...Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge process to prepare a noblemetal-free MC-60 catalyst containing MoO_(3),Mo_(2)C,and a Mo_(2)C–MoO_(3)interface.In the GOR,MC-60 shows activity as high as 745μA/(mmol/L cm^(2)),considerably higher than those of the Pt/CNT(270μA/(mmol/L cm^(2)))and Au/CNT catalysts(110μA/(mmol/L cm^(2))).In the GOR,the response minimum on MC-60 is as low as 8μmol/L,with a steady-state response time of only 3 s.Moreover,MC-60 has superior stability and anti-interference ability to impurities in the GOR.The better performance of MC-60 in the GOR is attributed to the abundant Mo sites bonding to C and O atoms at the MoO_(3)–Mo_(2)C interface.These Mo sites create active sites for promoting glucose adsorption and oxidation,enhancing MC-60 performance in the GOR.Thus,these results help to fabricate more effi cient noble-metal-free catalysts for the fabrication of glucose-based biofuel cells.展开更多
The spatial arrangement of activating ligands is known to have great influence on T cell activation.However,independently studying each ligand’s spatial organization parameter that affects T cell activation remains a...The spatial arrangement of activating ligands is known to have great influence on T cell activation.However,independently studying each ligand’s spatial organization parameter that affects T cell activation remains a great challenge.Here,with DNA origami,we precisely organized the CD3ɛantibodies simulating T cell receptor(TCR)ligands and CD28 antibodies simulating co-stimulatory ligands to interrogate the independent role of TCR-ligand spacing and local copy numbers as well as the spacing between TCR ligands and co-stimulatory ligands on T cell activation.We found that T cell activation benefited fromlocally concentrated TCR ligands with a shorter spacing and was maximized by an∼38 nm spacing between TCR ligands and co-stimulatory ligands.The T cell expander constructed based on our findings could efficiently expand CD8+T cells for tumor immunotherapy.Thus,the DNA nanostructurebased ligands’precise arrangement can be a unique tool in studying immune cell activations and cellbased immunotherapies.展开更多
Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been e...Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been established as one of the most efficient methods, the substrates are largely limited to terminal olefins with electron-withdrawing group(s). Herein, we report a synergistic silver-mediated and palladium-catalyzed non-directed C-H olefination of arenes with vinyl(pseudo)halides, which offers a complementary strategy to the typical Fujiwara-Moritani reaction. The reactions proceeded well for a variety of halogenated arenes, heteroarenes, and olefin substrates, providing an efficient access to various multi-substituted aryl olefins, including trisubstituted/tetrasubstituted olefins and several complex olefins derived from medicines or natural products. Mechanistic studies indicated a bimetallic Pd/Ag cooperation is operative in the catalysis, i.e., the reaction is initiated by aryl C-H bond cleavage via ligation with phosphine/Ag species, followed by transferring of the aryl moiety to a vinyl palladium intermediate,which is in turn formed by oxidative addition of vinyl(pseudo)halide to a Pd complex. This method enables the synthesis of a wide range of challenging multi-substituted vinyl products from simple arenes(directing-group free) in a streamlined and controllable fashion.展开更多
Background:Ginkgo biloba L.preparations(GBLPs)are a class of Chinese herbal medicine used in the adjuvant treatment of ischemic stroke(IS).Recently,several systematic reviews(SRs)and meta-analyses(MAs)of GBLPs for IS ...Background:Ginkgo biloba L.preparations(GBLPs)are a class of Chinese herbal medicine used in the adjuvant treatment of ischemic stroke(IS).Recently,several systematic reviews(SRs)and meta-analyses(MAs)of GBLPs for IS have been published.Objective:This overview aims to assess the quality of related SRs and MAs.Search strategy:Pub Med,Embase,Cochrane Library,Web of Science,Chinese Biological Medicine,China National Knowledge Infrastructure,Wanfang,and Chinese Science and Technology Journals databases were searched from their inception to December 31,2022.Inclusion criteria:SRs and MAs of randomized controlled trials(RCTs)that explored the efficacy of GBLPs for patients with IS were included.Data extraction and analysis:Two independent reviewers extracted data and assessed the methodological quality,risk of bias(ROB),reporting quality,and credibility of evidence of the included SRs and MAs using A Measurement Tool to Assess Systematic Reviews 2(AMSTAR 2),Risk of Bias in Systematic Reviews(ROBIS),the Preferred Reporting Items for Systematic Reviews and Meta-analyses(PRISMA),and the Grading of Recommendations Assessment,Development and Evaluation(GRADE),respectively.Additionally,descriptive analysis and data synthesis were conducted.Results:Twenty-nine SRs/MAs involving 119 outcomes were included in this review.The overall methodological quality of all SRs/MAs was critically low based on AMSTAR 2,and 28 had a high ROB based on the ROBIS.According to the PRISMA statement,the reporting items of the included SRs/MAs are relatively complete.The results based on GRADE showed that of the 119 outcomes,8 were rated as moderate quality,24 as low quality,and 87 as very low quality.Based on the data synthesis,GBLPs used in conjunction with conventional treatment were superior to conventional treatment alone for decreasing neurological function scores.Conclusion:GBLPs can be considered a beneficial supplemental therapy for IS.However,because of the low quality of the existing evidence,high-quality RCTs and SRs/MAs are warranted to further evaluate the benefits of GBLPs for treating IS.展开更多
The central dogma of modern biology underscores the pivotal roles proteins play in diverse biological processes,the study of which necessitates advanced methods to produce proteins with precision and versatility.Chemi...The central dogma of modern biology underscores the pivotal roles proteins play in diverse biological processes,the study of which necessitates advanced methods to produce proteins with precision and versatility.Chemical protein synthesis,a powerful approach utilizing chemical reactions for the de novo construction of structurally accurate proteins,has emerged as a transformative tool for studying proteins and generating protein derivatives/mimics inaccessible by natural biological machinery,including post-translationally modified proteins,proteins comprised of unnatural amino acids,as well as mirror-image proteins.This review summarizes recent strides in synthetic method developments for chemical protein synthesis,including innovative techniques in solid-phase peptide synthesis,the challenges presented by difficult sequences in either synthesis or folding and the exploration of novel ligation reactions using both chemical and enzymatic methods.Furthermore,the review also delves into newly developed protocols for site-selective protein modifications and the generation of stapled or macrocyclized peptides/miniproteins,highlighting the power of chemical methods to make structurally diverse proteins.Recent applications of synthetic proteins in investigating post-translational modifications(phosphorylation,lipidation,glycosylation,ubiquitination,etc.),mirror-image biological processes and drug development are further discussed.Together,these topics provide a comprehensive overview of the current landscape of chemical protein synthesis.展开更多
Lutein was nano-encapsuled with hydroxypropylmethyl cellulose phthalate(HPMCP)to maintain its bioactivity and to avoid thermal/light degradation.Supercritical antisolvent precipitation was applied to prepare lutein/HP...Lutein was nano-encapsuled with hydroxypropylmethyl cellulose phthalate(HPMCP)to maintain its bioactivity and to avoid thermal/light degradation.Supercritical antisolvent precipitation was applied to prepare lutein/HPMCP nano-capsule.The effects of several operating parameters on the yield,lutein loading,encapsulation efficiency,particle size and particle size distribution of the nanocapsule were investigated.The mean diameter of nanocapsules ranged from 163nm to 219nm under appropriate experimental conditions.The result of scanning electron microscope showed that the nanocapsules were nearly spherical.The highest yield reached 95.35% when the initial concentration of lutein was saturated.The highest lutein loading of 15.80% and encapsulation efficiency of 88.41% were obtained under the conditions of 11MPa,40℃ and CHPMCP︰Clutein=5︰l.The results may promote the application of lutein in food industry.展开更多
基金supported by the National Natural Science Foundation of China (52302292, 52302058, 52302085)the China Postdoctoral Science Foundation (2021M702225)+1 种基金the Anhui Province University Natural Science Research Project (2023AH030093, 2023AH040301)the Startup Research Fund of Chaohu University (KYQD-2023005, KYQD-2023051)。
文摘Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.
基金financially supported by Guangdong Major Project of Basic and Applied Basic Research (No.2019B030302007)National Key Research and Development Program of China (No. 2019YFA0705900) funded by MOSTthe financial support by State Key Lab of Luminescent Materials and Devices,South China University of Technology (Skllmd-2022-03)。
文摘Due to the complicated film formation kinetics, morphology control remains a major challenge for the development of efficient and stable all-polymer solar cells(all-PSCs). To overcome this obstacle, the sequential deposition method is used to fabricate the photoactive layers of all-PSCs comprising a polymer donor PTzBI-oF and a polymer acceptor PS1. The film morphology can be manipulated by incorporating amounts of a dibenzyl ether additive into the PS1 layer. Detailed morphology investigations by grazing incidence wide-angle X-ray scattering and a transmission electron microscope reveal that the combination merits of sequential deposition and DBE additive can render favorable crystalline properties as well as phase separation for PTzBI-oF:PS1 blends. Consequently, the optimized all-PSCs delivered an enhanced power conversion efficiency(PCE) of 15.21%along with improved carrier extraction and suppressed charge recombination. More importantly, the optimized all-PSCs remain over 90% of their initial PCEs under continuous thermal stress at 65 °C for over 500 h. This work validates that control over microstructure morphology via a sequential deposition process is a promising strategy for fabricating highly efficient and stable all-PSCs.
基金supported by the National Natural Science Foundation of China(21571038,22035004)the Education Department of Guizhou Province(2021312)+2 种基金the Foundation of Guizhou Province(2019-5666)the National Key R&D Program of China(2017YFA0700101)the State Key Laboratory of Physical Chemistry of Solid Surfaces(Xiamen University,202009)。
文摘Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.
基金supported by National Key R&D Program of China(2021YFA1502803)the National Natural Science Foundation of China(NSFC)(21972066,91745202)+3 种基金NSFC-Royal Society Joint Program(21661130149)L.P.thanks the Royal Society and Newton Fund for a Royal Society-Newton Advanced Fellowshipsupported by the Research Funds for the Frontiers Science Centre for Critical Earth Material Cycling,Nanjing Universitya Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Recent advances in utilizing ^(17)O isotopic labeling methods for solid-state nuclear magnetic resonance(NMR)investigations of metal oxides for lithium-ion batteries have yielded extensive insights into their structural and dynamic details.Herein,we commence with a brief introduction to recent research on lithium-ion battery oxide materials studied using ^(17)O solid-state NMR spectroscopy.Then we delve into a review of ^(17)O isotopic labeling methods for tagging oxygen sites in both the bulk and surfaces of metal oxides.At last,the unresolved problems and the future research directions for advancing the ^(17)O labeling technique are discussed.
基金supported financially by the Subject Chief Scientist Program(10XD14303900)from Science and Technology Commission of Shanghai Municipalitythe Specialized Research Fund for the Doctoral Program of Higher Education of China(20123107110005).
文摘The objective of this study was to improve the dissolution and bioavailability of silymarin(SM).Solid dispersions(SDs)were prepared using solution-enhanced dispersion by supercritical fluids(SEDS)and evaluated in vitro and in vivo,compared with pure SM powder.The particle sizes,stability,and contents of residual solvent of the prepared SM-SDs with SEDS and solvent evaporation(SE)were investigated.Four polymer matrix materials were evaluated for the preparation of SM-SD-SEDS,and the hydrophilic polymer,polyvinyl pyrrolidone K17,was selected with a ratio of 1:5 between SM and the polymer.Physicochemical analyses using X-ray diffraction and differential scanning calorimetry indicated that SM was dispersed in SD in an amorphous state.The optimized SM-SD-SEDS showed no loss of SM after storage for 6 months and negligible residual solvent(ethanol)was detected using gas chromatography.In vitro drug release was increased from the SM-SDSEDS,as compared with pure SM powder or SM-SD-SE.In vivo,the area under the rat plasma SM concentration-time curve and the maximum plasma SM concentration were 2.4-fold and 1.9-fold higher,respectively,after oral administration of SM-SD-SEDS as compared with an aqueous SM suspension.These results illustrated the potential of using SEDS to prepare SM-SD,further improving the biopharmaceutical properties of this compound.
基金supported by the “Villum Center for the Science of Sustainable Fuels and Chemicals” (V-Sustain, grant number 9455) research initiative funded by the VILLUM FONDEN。
文摘The activation of iron oxide Fischer–Tropsch Synthesis(FTS) catalysts was investigated during pretreatment: reduction in hydrogen followed by carburization in either CO or syngas mixture, or simultaneously reduction and carburization in syngas. A combination of different complementary in situ techniques was used to gain insight into the behavior of Fe-based FTS catalysts during activation. In situ XRD was used to identify the crystalline structures present during both reduction in hydrogen and carburization. An increase in reduction rate was established when increasing the temperature. A complete reduction was demonstrated in the ETEM and a grain size dependency was proven, i.e. bigger grains need higher temperature in order to reduce. XPS and XAS both indicate the formation of a small amount of carbonaceous species at the surface of the bulk metallic iron during carburization.
基金supported by the National Natural Science Foundation of China (Grant Nos. 21734009, 51473009, 21225209, 91427303, and 61805138)Portions of this research were carried out at beamline 7.3.3 at the Advanced Light Source,Molecular Foundry,Lawrence Berkeley National Laboratory,which was supported by the DOE,Office of Science,and Office of Basic Energy Sciences。
文摘Morphology control of perovskite films is of critical importance for high-performance photovoltaic devices. Although solvent vapor annealing(SVA) treatment has been widely used to improve the film quality efficiently, the detailed mechanism of film growth is still under construction, and there is still no consensus on the selection of solvents and volume for further optimization. Here, a series of solvents(DMF, DMSO, mixed DMF/DMSO) were opted for exploring their impact on fundamental structural and physical properties of perovskite films and the performance of corresponding devices. Mixed solvent SVA treatment resulted in unique benefits that integrated the advantages of each solvent, generating a champion device efficiency of 19.76% with improved humidity and thermal stability. The crystallization mechanism was constructed by conducting grazing-incidence wide-angle x-ray diffraction(GIWAXS) characterizations, showing that dissolution and recrystallization dominated the film formation. A proper choice of solvent and its volume balancing the two processes thus afforded the desired perovskite film. This study reveals the underlying process of film formation, paving the way to producing energy-harvesting materials in a controlled manner towards energy-efficient and stable perovskite-based devices.
基金supported by the National Natural Science Foundation of China(Grant Nos.52002372,51672279,51727806,11874361,and 11774354)Science Challenge Project(Grant No.TZ2016001)Chinese Academy of Sciences Innovation Grant(Grant No.CXJJ-19-B08)。
文摘The recent discovery of room temperature superconductivity(283 K)in carbonaceous sulfur hydride(C-S-H)has attracted much interest in ternary hydrogen rich materials.In this report,ternary hydride P-S-H was synthesized through a photothermal-chemical reaction from elemental sulfur(S),phosphorus(P)and molecular hydrogen(H_(2))at high pressures and room temperature.Raman spectroscopy under pressure shows that H_(2)S and PH_(3) compounds are synthesized after laser heating at 0.9 GPa,and a ternary van der Waals compound P-S-H is synthesized with further compression to 4.6 GPa.The P-S-H compound is probably a mixed alloy of PH_(3) and(H_(2)S)_(2)H_(2) with a guest-host structure similar to the C-S-H system.The ternary hydride can persist up to 35.6 GPa at least and shows two phase transitions at approximately 23.6 GPa and 32.8 GPa,respectively.
基金financially supported by the China National Textile & Apparel Council (2013‘Textile Vision’ Applied Basic Research,2013-153)the Collaborative Innovation Plan of Hubei Province for Key Technology of Eco-Ramie Industry (2014–8)
文摘Physical and chemical properties of wool surface significantly affect the absorbency,rate of dye bath exhaustion and fixation of the industrial dyes.Hence,surface modification is a necessary operation prior to coloration process in wool wet processing industries.Plasma treatment is an effective alternative for physiochemical modification of wool surface.However,optimum processing parameters to get the expected modification are still under investigation,hence this technology is still under development in the wool wet processing industries.Therefore,in this paper,treatment parameters with the help of simple dielectric barrier discharge plasma reactor and air as a plasma gas,which could be a promising combination for treatment of wool substrate at industrial scale were schematically studied,and their influence on the water absorbency,mechanical,and dyeing properties of twill woven wool fabric samples are reported.It is expected that the results will assist to the wool coloration industries to improve the dyeing processes.
文摘A series of 1,2,4-triazole derivatives were synthesized, and their abilities to inhibit the in vitro replication of Coxsackie B3/B6 were evaluated. Among the 1,2,4-triazole derivatives, compound 3 g displayed potent activity, with a high antiviral potency (IC50 = 1.71 μM (against CVB3), 1.43 μM (against CVB6)). The structures of all the new synthesized compounds were confirmed by 1H-NMR spectra, mass spectra and elemental analyses.
基金supported by the National Natural Science Foundation of China(Grant Nos.22225801 and 21905206)the Open Project of the State Key Laboratory of Functional Materials for Informatics(SKL202107)supported by the Fundamental Research Funds for the Central Universities,conducted at Tongji University.
文摘Aqueous zinc-ion battery(ZIB)featuring with high safety,low cost,environmentally friendly,and high energy density is one of the most promising systems for large-scale energy storage application.Despite extensive research progress made in developing high-performance cathodes,the Zn anode issues,such as Zn dendrites,corrosion,and hydrogen evolution,have been observed to shorten ZIB’s lifespan seriously,thus restricting their practical application.Engineering advanced Zn anodes based on two-dimensional(2D)materials are widely investigated to address these issues.With atomic thickness,2D materials possess ultrahigh specific surface area,much exposed active sites,superior mechanical strength and flexibility,and unique electrical properties,which confirm to be a promising alternative anode material for ZIBs.This review aims to boost rational design strategies of 2D materials for practical application of ZIB by combining the fundamental principle and research progress.Firstly,the fundamental principles of 2D materials against the drawbacks of Zn anode are introduced.Then,the designed strategies of several typical 2D materials for stable Zn anodes are comprehensively summarized.Finally,perspectives on the future development of advanced Zn anodes by taking advantage of these unique properties of 2D materials are proposed.
基金Project supported by the National Key R&D Program of China (Grant No. 2021YFA1202802)the National Natural Science Foundation of China (Grant Nos. 21875280,21991150, 21991153, and 22022205)+1 种基金the CAS Project for Young Scientists in Basic Research (Grant No. YSBR-054)the Special Foundation for Carbon Peak Neutralization Technology Innovation Program of Jiangsu Province,China(Grant No. BE2022026)
文摘The charge carrier concentration profile is a critical factor that determines semiconducting material properties and device performance.Dielectric force microscopy(DFM)has been previously developed to map charge carrier concentrations with nanometer-scale spatial resolution.However,it is challenging to quantitatively obtain the charge carrier concentration,since the dielectric force is also affected by the mobility.Here,we quantitative measured the charge carrier concentration at the saturation mobility regime via the rectification effect-dependent gating ratio of DFM.By measuring a series of n-type GaAs and GaN thin films with mobility in the saturation regime,we confirmed the decreased DFM-measured gating ratio with increasing electron concentration.Combined with numerical simulation to calibrate the tip–sample geometry-induced systematic error,the quantitative correlation between the DFM-measured gating ratio and the electron concentration has been established,where the extracted electron concentration presents high accuracy in the range of 4×10^(16)–1×10^(18)cm^(-3).We expect the quantitative DFM to find broad applications in characterizing the charge carrier transport properties of various semiconducting materials and devices.
基金supported by the National Key Research and Development Program of China(2021YFA1101300)the National Natural Science Foundation of China(Grant No.22225801,21776197,22078214,and 21905206)Special Fund for Science and Technology Innovation Team of Shanxi Province(No.202204051001009).
文摘The ionic transport in sub-nanochannels plays a key role in energy storage,yet suffers from a high energy barrier.Wetting sub-nanochannels is crucial to accelerate ionic transport,but the introduction of water is challenging because of the hydrophobic extreme confinement.We propose wetting the channels by the exothermic hydration process of pre-intercalated ions,the effect of which varies distinctly with different ionic hydration structures and energies.Compared to the failed pre-intercalation of SO_(4)^(2-),HSO_(4)^(-) with weak hydration energy results in a marginal effect on the HOMO(Highest Occupied Molecular Orbital)level of water to avoid water splitting during the electrochemical intercalation.Meanwhile,the ability of water introduction is reserved by the initial incomplete dissociation state of HSO_(4)^(-),so the consequent exothermic reionization and hydration processes of the intercalated HSO_(4)^(-) promote the water introduction into sub-nanochannels,finally forming the stable confined water through hydrogen bonding with functional groups.The wetted channels exhibit a significantly enhanced ionic diffusion coef-ficient by~9.4 times.
基金supported by the National Natural Science Foundation of China(grant nos.21890730,21890733,and 22231007)the Program for Basic Research of Shanghai Science and Technology Commission(grant no.19JC1410400)+2 种基金the Fundamental Research Funds for the Central Universities(grant no.23X010301599)the Shanghai Pujiang Program(grant no.21PJ1406500)the China Postdoctoral Science Foundation(grant no.2022M722073).
文摘Aiming at accessing polyethylene-bearing in-chain degradable functionality,copolymerization of carbon dioxide(CO_(2))with ethylene has long been recognized as a significant but highly challenging transformation.Nevertheless,most trials have resulted in ethylene homopolymerization because of the endothermic property and high energy barriers of CO_(2)insertion during polymer chain propagation.Here we report an unprecedented tandem reaction protocol for the synthesis of polyethylenes with in-chain carbonyls from CO_(2)and ethylene by the combination of photocatalytic CO_(2)reduction and palladium-catalyzed coordination/insertion polymerization.This protocol provides an easy way to adjust the carbonyl content(from 0.13 to 12 mol%)and insertion selectivity(up to 99%isolated carbonyls)of the polyethylene copolymers,which enables the polymers tomaintain the main properties of highdensity polyethylene and simultaneously endows them with good photodegradability.In addition,besides apolar polyethylene copolymers,polar-functionalized polyethylenes with in-chain isolated carbonyls can also be synthesized from CO_(2),ethylene and a polar monomer using the same protocol.We believe our present work sheds new light on the synthesis of degradable polyethylenes by employing CO_(2)as a green carbonyl source.
基金supported by the National Natural Science Foundation of China(Nos.82170426 and 22078193)Double Thousand Plan of Jiangxi Province(Nos.461654,jxsq2019102052).
文摘Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge process to prepare a noblemetal-free MC-60 catalyst containing MoO_(3),Mo_(2)C,and a Mo_(2)C–MoO_(3)interface.In the GOR,MC-60 shows activity as high as 745μA/(mmol/L cm^(2)),considerably higher than those of the Pt/CNT(270μA/(mmol/L cm^(2)))and Au/CNT catalysts(110μA/(mmol/L cm^(2))).In the GOR,the response minimum on MC-60 is as low as 8μmol/L,with a steady-state response time of only 3 s.Moreover,MC-60 has superior stability and anti-interference ability to impurities in the GOR.The better performance of MC-60 in the GOR is attributed to the abundant Mo sites bonding to C and O atoms at the MoO_(3)–Mo_(2)C interface.These Mo sites create active sites for promoting glucose adsorption and oxidation,enhancing MC-60 performance in the GOR.Thus,these results help to fabricate more effi cient noble-metal-free catalysts for the fabrication of glucose-based biofuel cells.
基金supported by the National Research Programs from the Ministry of Science and Technology of China(grant no.2021YFF0701800)the National Natural Science Foundation of China(grant nos.52032008 and 22277071)+1 种基金the Collaborative Innovation Center of Suzhou Nano Science and Technologythe“111”program from the Ministry of Education of China.
文摘The spatial arrangement of activating ligands is known to have great influence on T cell activation.However,independently studying each ligand’s spatial organization parameter that affects T cell activation remains a great challenge.Here,with DNA origami,we precisely organized the CD3ɛantibodies simulating T cell receptor(TCR)ligands and CD28 antibodies simulating co-stimulatory ligands to interrogate the independent role of TCR-ligand spacing and local copy numbers as well as the spacing between TCR ligands and co-stimulatory ligands on T cell activation.We found that T cell activation benefited fromlocally concentrated TCR ligands with a shorter spacing and was maximized by an∼38 nm spacing between TCR ligands and co-stimulatory ligands.The T cell expander constructed based on our findings could efficiently expand CD8+T cells for tumor immunotherapy.Thus,the DNA nanostructurebased ligands’precise arrangement can be a unique tool in studying immune cell activations and cellbased immunotherapies.
基金supported by the National Key R&D Program of China(2021YFA1500100)the National Natural Science Foundation of China(21821002,92256303,22171278)+1 种基金Shanghai Science and Technology Committee(23ZR1482400)the Natural Science Foundation of Ningbo(2023J034)。
文摘Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been established as one of the most efficient methods, the substrates are largely limited to terminal olefins with electron-withdrawing group(s). Herein, we report a synergistic silver-mediated and palladium-catalyzed non-directed C-H olefination of arenes with vinyl(pseudo)halides, which offers a complementary strategy to the typical Fujiwara-Moritani reaction. The reactions proceeded well for a variety of halogenated arenes, heteroarenes, and olefin substrates, providing an efficient access to various multi-substituted aryl olefins, including trisubstituted/tetrasubstituted olefins and several complex olefins derived from medicines or natural products. Mechanistic studies indicated a bimetallic Pd/Ag cooperation is operative in the catalysis, i.e., the reaction is initiated by aryl C-H bond cleavage via ligation with phosphine/Ag species, followed by transferring of the aryl moiety to a vinyl palladium intermediate,which is in turn formed by oxidative addition of vinyl(pseudo)halide to a Pd complex. This method enables the synthesis of a wide range of challenging multi-substituted vinyl products from simple arenes(directing-group free) in a streamlined and controllable fashion.
基金supported by the Traditional Chinese Medicine Ancient Book Documents and Characteristic Technology Inheritance Project of the National Administration of Traditional Chinese Medicine(No.GZY-KJS-2020-079)the Research and Transformation Application of Clinical Characteristic Diagnosis and Treatment Techniques in the Capital(No.Z221100007422081)the National Famous Old TCM Experts Baoliang Wang Inheritance Studio Construction Program,State TCM Office Human Education Letter(No.[2022]75)。
文摘Background:Ginkgo biloba L.preparations(GBLPs)are a class of Chinese herbal medicine used in the adjuvant treatment of ischemic stroke(IS).Recently,several systematic reviews(SRs)and meta-analyses(MAs)of GBLPs for IS have been published.Objective:This overview aims to assess the quality of related SRs and MAs.Search strategy:Pub Med,Embase,Cochrane Library,Web of Science,Chinese Biological Medicine,China National Knowledge Infrastructure,Wanfang,and Chinese Science and Technology Journals databases were searched from their inception to December 31,2022.Inclusion criteria:SRs and MAs of randomized controlled trials(RCTs)that explored the efficacy of GBLPs for patients with IS were included.Data extraction and analysis:Two independent reviewers extracted data and assessed the methodological quality,risk of bias(ROB),reporting quality,and credibility of evidence of the included SRs and MAs using A Measurement Tool to Assess Systematic Reviews 2(AMSTAR 2),Risk of Bias in Systematic Reviews(ROBIS),the Preferred Reporting Items for Systematic Reviews and Meta-analyses(PRISMA),and the Grading of Recommendations Assessment,Development and Evaluation(GRADE),respectively.Additionally,descriptive analysis and data synthesis were conducted.Results:Twenty-nine SRs/MAs involving 119 outcomes were included in this review.The overall methodological quality of all SRs/MAs was critically low based on AMSTAR 2,and 28 had a high ROB based on the ROBIS.According to the PRISMA statement,the reporting items of the included SRs/MAs are relatively complete.The results based on GRADE showed that of the 119 outcomes,8 were rated as moderate quality,24 as low quality,and 87 as very low quality.Based on the data synthesis,GBLPs used in conjunction with conventional treatment were superior to conventional treatment alone for decreasing neurological function scores.Conclusion:GBLPs can be considered a beneficial supplemental therapy for IS.However,because of the low quality of the existing evidence,high-quality RCTs and SRs/MAs are warranted to further evaluate the benefits of GBLPs for treating IS.
基金supported by the National Key R&D Program of China(2022YFC3401500)the National Natural Science Foundation of China(22137005,92253302,22227810 to Lei Liu,22177004,92153301,22321005 to Suwei Dong,22277020 to Yiming Li,22022703,22177108,22377118 to Ji-Shen Zheng,92353302,22177059 to Yongxiang Chen,22177035 to Jun Guo,22277029,22077036 to Chunmao He,22077078 to Honggang Hu92353302,92053108 to Yanmei Li,22277015 to Junfeng Zhao)。
文摘The central dogma of modern biology underscores the pivotal roles proteins play in diverse biological processes,the study of which necessitates advanced methods to produce proteins with precision and versatility.Chemical protein synthesis,a powerful approach utilizing chemical reactions for the de novo construction of structurally accurate proteins,has emerged as a transformative tool for studying proteins and generating protein derivatives/mimics inaccessible by natural biological machinery,including post-translationally modified proteins,proteins comprised of unnatural amino acids,as well as mirror-image proteins.This review summarizes recent strides in synthetic method developments for chemical protein synthesis,including innovative techniques in solid-phase peptide synthesis,the challenges presented by difficult sequences in either synthesis or folding and the exploration of novel ligation reactions using both chemical and enzymatic methods.Furthermore,the review also delves into newly developed protocols for site-selective protein modifications and the generation of stapled or macrocyclized peptides/miniproteins,highlighting the power of chemical methods to make structurally diverse proteins.Recent applications of synthetic proteins in investigating post-translational modifications(phosphorylation,lipidation,glycosylation,ubiquitination,etc.),mirror-image biological processes and drug development are further discussed.Together,these topics provide a comprehensive overview of the current landscape of chemical protein synthesis.
基金Supported by the National High Technology Research and Development Program of China(2007AA10Z350)
文摘Lutein was nano-encapsuled with hydroxypropylmethyl cellulose phthalate(HPMCP)to maintain its bioactivity and to avoid thermal/light degradation.Supercritical antisolvent precipitation was applied to prepare lutein/HPMCP nano-capsule.The effects of several operating parameters on the yield,lutein loading,encapsulation efficiency,particle size and particle size distribution of the nanocapsule were investigated.The mean diameter of nanocapsules ranged from 163nm to 219nm under appropriate experimental conditions.The result of scanning electron microscope showed that the nanocapsules were nearly spherical.The highest yield reached 95.35% when the initial concentration of lutein was saturated.The highest lutein loading of 15.80% and encapsulation efficiency of 88.41% were obtained under the conditions of 11MPa,40℃ and CHPMCP︰Clutein=5︰l.The results may promote the application of lutein in food industry.