Optimizing the microchannel design of the next generation of chips requires an understanding of the in situ property evolution of the chip-based materials under fast cooling.This work overcomes the conventional relian...Optimizing the microchannel design of the next generation of chips requires an understanding of the in situ property evolution of the chip-based materials under fast cooling.This work overcomes the conventional reliance on reheating data of melt-quenched glasses by demonstrating direct observations of glass transition on cooling curves utilizing the most advanced fast differential scanning calorimetry.By leveraging an MEMS chip sensor that allows for rapid heat extraction from microgram-sized samples to a purged gas coolant,the device is able to reach ultra-fast cooling rates of up to 40,000 K·s^(−1).Four thermal regions are identified by examining the cooling behaviors of two metallic glasses.This is because the actual rate of the specimen can differ from the programmed rate,especially at high set rate when the actual rate decreases before the glass transition is completed.We define the operational window for reliable cooling curve analysis,build models with empirical and theoretical analyses to determine the maximum feasible cooling rate,and demonstrate how optimizing sample mass and environment temperature broaden this window.The method avoids deceptive structural relaxation effects verified by fictivetemperature analysis and permits the capture of full glass transition during cooling.展开更多
Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-...Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.展开更多
High-pressure research has emerged as a pivotal approach for advancing our understanding and development of optoelectronic materials,which are vital for a wide range of applications,including photovoltaics,light-emitt...High-pressure research has emerged as a pivotal approach for advancing our understanding and development of optoelectronic materials,which are vital for a wide range of applications,including photovoltaics,light-emitting devices,and photodetectors.This review highlights various in situ characterization methods employed in high-pressure research to investigate the optical,electronic,and structural properties of optoelectronic materials.We explore the advances that have been made in techniques such as X-ray diffraction,absorption spectroscopy,nonlinear optics,photoluminescence spectroscopy,Raman spectroscopy,and photoresponse measurement,emphasizing how these methods have enhanced the elucidation of structural transitions,bandgap modulation,performance optimization,and carrier dynamics engineering.These insights underscore the pivotal role of high-pressure techniques in optimizing and tailoring optoelectronic materials for future applications.展开更多
Introduction Early cancer detection represents a critical evolution in healthcare,addressing a significant pain point in cancer treatment:the tendency for diagnoses to occur at advanced stages.Traditionally,many cance...Introduction Early cancer detection represents a critical evolution in healthcare,addressing a significant pain point in cancer treatment:the tendency for diagnoses to occur at advanced stages.Traditionally,many cancers are not identified until they have progressed to late stages,where treatment options become limited,less effective,and more costly.This late detection results in poorer prognoses,higher mortality rates,and increased healthcare costs.Without early detection tools like Fluorescence In Situ Hybridization(FISH),these challenges persist,leaving patients with fewer opportunities for successful outcomes.展开更多
Despite the ongoing increase in the efficiency of perovskite solar cells(PSCs),residual lead iodide(PbI2and moisture sensitivity issues continue to constrain their further commercialization.Herein,we propose a thermal...Despite the ongoing increase in the efficiency of perovskite solar cells(PSCs),residual lead iodide(PbI2and moisture sensitivity issues continue to constrain their further commercialization.Herein,we propose a thermally mediated in situ repair and encapsulation strategy to construct high-performance PSCs by incorporating piperazine thioctic acid salt(TAPPZ)as a dopant into the perovskite precursor Thermally dissociated piperazine(PPZ)from TAPPZ integrates microcrystals to form larger grain(>2000 nm),while the carboxylic acid in thioctic acid(TA)and the amine salt in TAPPZ synergistically passivate and transform PbI_(2),significantly reducing its residual amount.Additionally,TAPPZ undergoe thermal self-crosslinking during perovskite annealing,enabling melt-polymerization to form in situ encapsulation for enhanced water resistance.The TAPPZ-incorporated device achieves a remarkable efficiency of 25.65% and exhibits excellent operational stability,retaining over 90% of its initial efficiency after 2000 h under ambient conditions(20-30℃,20%-30% relative humidity).This study provide new insights into the construction of high-performance perovskite solar cells by designing and synthe sizing multifunctional single molecules for in situ repair and encapsulation of perovskites.展开更多
The pressure-preserving controller is the key component of deep in situ pressure-preserving coring(IPP-Coring).With increasing drilling depth,the environmental temperature and pressure increase accordingly.However,due...The pressure-preserving controller is the key component of deep in situ pressure-preserving coring(IPP-Coring).With increasing drilling depth,the environmental temperature and pressure increase accordingly.However,due to the strength and sealing problems of pressure-preserving controllers,the coring pressure is generally lower than 70 MPa.Establishing a high-temperature and ultrahigh-pressure test system is highly important for improving the strength and sealing performance of pressure-preserving controllers.This paper introduces a high-temperature and ultrahigh-pressure test system for deep IPP-Coring controller performance analysis.The device includes six parts:an auxiliary air source system,a pressurization system,a temperature control system,a hydraulic system,a data acquisition and electrical control system,and an ultrahigh-pressure vessel.The test system can reconstruct a 150℃ and 200 MPa in situ environment and simulate and test the movement state of the corer and the stability of the pressure-preserving action trigger of the pressure-preserving controller in the deep IPP-Coring process.To verify the performance of this test system,saddle-shaped pressure-preserving controllers made of four different materials were subjected to pressure tests under normal-temperature and high-temperature conditions.The results showed that the ultimate pressure-bearing capability of the pressure-preserving controller greatly varied between normal-temperature and high-temperature conditions.The pressure-preserving ability and sealing performance of the pressure-preserving controller decreased significantly at high temperature,and the pressure-preserving controller exhibited significantly different sealing failure characteristics due to material differences.This study is important for progressing the extraction and evaluation of deep reservoir resources.展开更多
In this work,silicon-carbon hybrid materials were adopted as an example to illustrate the novel strategy to in situ construct heterostructure with adjustable microstructure.Based on the temperature-dependent thermodyn...In this work,silicon-carbon hybrid materials were adopted as an example to illustrate the novel strategy to in situ construct heterostructure with adjustable microstructure.Based on the temperature-dependent thermodynamics and kinetics of reaction between Si and C,the processes for Si nanocrystals growth and C decoration were coupled at different zones of plasma flame according to its temperature and velocity fields by theoretical modeling,aiming to intentionally suppress the formation of undesirable carbide,and enable adjusting the microstructure of each counterpart separately in transient process.As a result,well-controlled Si/C nanocomposites,including nanospheres and nanowires with core-shell structures,were achieved,and this continuous and in-flight route is also potential for large-scale production.Further investigation on the electrochemical properties highlights the advantage of as proposed strategy to efficiently construct heterostructures with superior performance for various applications.展开更多
The clinical application of tumor vaccines is hindered by challenges such as timeconsuming and costly production processes.In this context,in situ cancer vaccines represent a promising strategy by leveraging endogenou...The clinical application of tumor vaccines is hindered by challenges such as timeconsuming and costly production processes.In this context,in situ cancer vaccines represent a promising strategy by leveraging endogenous tumor antigens to elicit robust antitumor T cell responses.Herein,a photoactivatable tumor-targeting in situ nanovaccine,Lipo-D8-6,was constructed using cRGD-functionalized liposomes that co-encapsulated the photosensitizer chlorin e6 and a cleavable immunoadjuvant conjugate D8,allowing light-triggered synchronous activation of three therapeutic modules.Upon near-infrared light irradiation,Lipo-D8-6 generates reactive oxygen species that exert direct cytotoxicity on tumor cells and induce immunogenic cell death,while concurrently cleaving the responsive linker within D8 to achieve the controlled release of R848.In vivo biodistribution analysis confirmed the superior intratumoral accumulation of Lipo-D8-6,facilitating precise treatment.In a large-volume tumor model,the nanovaccine exhibited pronounced antitumor efficacy,accompanied by enhanced tumor infiltration of CD8t T cells.Overall,this work provides a simplified and effective approach for developing in situ nanovaccines that enable synergistic photodynamic immunotherapy with precise spatiotemporal control over immune activation.展开更多
Electrocatalytic nitrate reduction reaction (NO_(3)-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues.We report a CuO nanoparticles in...Electrocatalytic nitrate reduction reaction (NO_(3)-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues.We report a CuO nanoparticles incorporated on nitrogen-doped porous carbon (CuO@NC) catalyst for NO_(3)-RR.Part of Cu(Ⅱ) is reduced to Cu(Ⅰ) during the NO_(3)-RR process to construct Cu(Ⅰ)-Cu(Ⅱ) pairs,confirmed by in situ X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy.Density functional theory (DFT) calculations indicated that the formation of Cu(Ⅰ) could provide a reaction path with smaller energy barrier for NO_(3)-RR,while Cu(Ⅱ) effectively suppressed the competition of hydrogen evolution reaction (HER).As a result,CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at -0.49 V versus reversible hydrogen electrode (RHE),and a NH_(3)yield rate of 17.2 mg h^(-1)mg^(-1)cat.at -0.79 V vs.RHE,higher than the HaberBosch process (<3.4 g h^(-1)g^(-1)cat.).This work may open a new avenue for effective NO_(3)-RR by modulating oxidation states.展开更多
The global demand for effective skin injury treatments has prompted the exploration of tissue engineering solutions.While three-dimensional(3D)bioprinting has shown promise,challenges persist with respect to achieving...The global demand for effective skin injury treatments has prompted the exploration of tissue engineering solutions.While three-dimensional(3D)bioprinting has shown promise,challenges persist with respect to achieving timely and compatible solutions to treat diverse skin injuries.In situ bioprinting has emerged as a key new technology,since it reduces risks during the implantation of printed scaffolds and demonstrates superior therapeutic effects.However,maintaining printing fidelity during in situ bioprinting remains a critical challenge,particularly with respect to model layering and path planning.This study proposes a novel optimization-based conformal path planning strategy for in situ bioprinting-based repair of complex skin injuries.This strategy employs constrained optimization to identify optimal waypoints on a point cloud-approximated curved surface,thereby ensuring a high degree of similarity between predesigned planar and surface-mapped 3D paths.Furthermore,this method is applicable for skin wound treatments,since it generates 3D-equidistant zigzag curves along surface tangents and enables multi-layer conformal path planning to facilitate the treatment of volumetric injuries.Furthermore,the proposed algorithm was found to be a feasible and effective treatment in a murine back injury model as well as in other complex models,thereby showcasing its potential to guide in situ bioprinting,enhance bioprinting fidelity,and facilitate improvement of clinical outcomes.展开更多
High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions wit...High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.展开更多
1.Introduction Various geological phenomena on the surface and in the interior of the Earth,as well as their associated physical and chemical pro-cesses,are closely correlated with the action of in situ rock stress[1-...1.Introduction Various geological phenomena on the surface and in the interior of the Earth,as well as their associated physical and chemical pro-cesses,are closely correlated with the action of in situ rock stress[1-5].Understanding the rock stress state at great depths is not only an indispensable foundation for solving scientific problems associated with geology,geophysics,and geodynamics-such as plate-driving mechanisms,the earth’s energy equilibrium,earth-quake mechanisms,and tectonic activities-but also a necessary prerequisite for the evaluation,exploitation,and disposal of deep energy and resources,such as coal and metal minerals.Due to the complexity and uncertainty of the origin of in situ rock stress,it is a difficult quantity to evaluate,in comparison with other rock properties.Currently,reliable information on the stress state in a region can only be determined through field stress measurement.Therefore,a variety of stress measurement techniques have been developed and applied worldwide to provide information on crus-tal contemporary stress at specific depth ranges[6].展开更多
Due to the heterogeneity of rock masses and the variability of in situ stress,the traditional linear inversion method is insufficiently accurate to achieve high accuracy of the in situ stress field.To address this cha...Due to the heterogeneity of rock masses and the variability of in situ stress,the traditional linear inversion method is insufficiently accurate to achieve high accuracy of the in situ stress field.To address this challenge,nonlinear stress boundaries for a numerical model are determined through regression analysis of a series of nonlinear coefficient matrices,which are derived from the bubbling method.Considering the randomness and flexibility of the bubbling method,a parametric study is conducted to determine recommended ranges for these parameters,including the standard deviation(σb)of bubble radii,the non-uniform coefficient matrix number(λ)for nonlinear stress boundaries,and the number(m)and positions of in situ stress measurement points.A model case study provides a reference for the selection of these parameters.Additionally,when the nonlinear in situ stress inversion method is employed,stress distortion inevitably occurs near model boundaries,aligning with the Saint Venant's principle.Two strategies are proposed accordingly:employing a systematic reduction of nonlinear coefficients to achieve high inversion accuracy while minimizing significant stress distortion,and excluding regions with severe stress distortion near the model edges while utilizing the central part of the model for subsequent simulations.These two strategies have been successfully implemented in the nonlinear in situ stress inversion of the Xincheng Gold Mine and have achieved higher inversion accuracy than the linear method.Specifically,the linear and nonlinear inversion methods yield root mean square errors(RMSE)of 4.15 and 3.2,and inversion relative errors(δAve)of 22.08%and 17.55%,respectively.Therefore,the nonlinear inversion method outperforms the traditional multiple linear regression method,even in the presence of a systematic reduction in the nonlinear stress boundaries.展开更多
The paper presents experimental investigation results of crack pattern change in cement pastes caused by external sulfate attack(ESA).To visualize the formation and development of cracks in cement pastes under ESA,an ...The paper presents experimental investigation results of crack pattern change in cement pastes caused by external sulfate attack(ESA).To visualize the formation and development of cracks in cement pastes under ESA,an X-ray computed tomography(X-ray CT)was used,i e,the tomography system of Zeiss Xradia 510 versa.The results indicate that X-CT can monitor the development process and distribution characteristics of the internal cracks of cement pastes under ESA with attack time.In addition,the C3A content in the cement significantly affects the damage mode of cement paste specimens during sulfate erosion.The damage of ordinary Portland cement(OPC)pastes subjected to sulfate attack with high C3A content are severe,while the damage of sulfate resistant Portland cement(SRPC)pastes is much smaller than that of OPC pastes.Furthermore,a quadratic function describes the correlation between the crack volume fraction and development depth for two cement pastes immermed in sulfate solution.展开更多
Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal s...Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.展开更多
One of the detection objectives of the Chinese Asteroid Exploration mission is to investigate the space environment near the Main-belt Comet(MBC,Active Asteroid)311P/PANSTARRS.This paper outlines the scientific object...One of the detection objectives of the Chinese Asteroid Exploration mission is to investigate the space environment near the Main-belt Comet(MBC,Active Asteroid)311P/PANSTARRS.This paper outlines the scientific objectives,measurement targets,and measurement requirements for the proposed Gas and Ion Analyzer(GIA).The GIA is designed for in-situ mass spectrometry of neutral gases and low-energy ions,such as hydrogen,carbon,and oxygen,in the vicinity of 311P.Ion sampling techniques are essential for the GIA's Time-of-Flight(TOF)mass analysis capabilities.In this paper,we present an enhanced ion sampling technique through the development of an ion attraction model and an ion source model.The ion attraction model demonstrates that adjusting attraction grid voltage can enhance the detection efficiency of low-energy ions and mitigate the repulsive force of ions during sampling,which is influenced by the satellite's surface positive charging.The ion source model simulates the processes of gas ionization and ion multiplication.Simulation results indicate that the GIA can achieve a lower pressure limit below 10-13Pa and possess a dynamic range exceeding 10~9.These performances ensure the generation of ions with stable and consistent current,which is crucial for high-resolution and broad dynamic range mass spectrometer analysis.Preliminary testing experiments have verified GIA's capability to detect gas compositions such as H2O and N2.In-situ measurements near 311P using GIA are expected to significantly contribute to our understanding of asteroid activity mechanisms,the evolution of the atmospheric and ionized environments of main-belt comets,the interactions with solar wind,and the origin of Earth's water.展开更多
Despite sulfurization offers the advantage of improving the photovoltaic performance in preparing Cu(In,Ga)Se2(CIGS)absorbers,deep level defects in the absorber and poor energy level alignment on the front surface are...Despite sulfurization offers the advantage of improving the photovoltaic performance in preparing Cu(In,Ga)Se2(CIGS)absorbers,deep level defects in the absorber and poor energy level alignment on the front surface are still main obstacles limiting the improvement of power co nversion efficiency(PCE)in sulfided CIGS solar cells.Herein,an in-situ Na doping strategy is proposed,in which the tailing effect of crystal growth is used to promote the sulfurization of CIGS absorbers.It is found that the grain growth is supported by Na incorporating due to the enrichment of NaSe_(x)near the upper surface.The high soluble Na during grain growth can not only suppress intrinsic In_(Cu) donor defects in the absorber,but also tailor S distribution in bulk and the band alignment at the heterojunction,which are both beneficial for the effective electron carriers.Meanwhile,the Na aggregation near the bottom of the absorber also contributes to the crystalline quality increasing and favorable ultra-thin MoSe_(2) formation at back contact,resulting in a reduced barrier height conducive to hole transport.PCE of the champion device is as high as 16.76%with a 28%increase.This research offers new insights into synthesizing CIGS solar cells and other chalcogenide solar cells with superior cell performance when using an intense sulfurization process.展开更多
The low temperature,high salt content,and bacterial composition of a seawater environment can induce severe infections in open wounds,thus impeding wound healing.To date,numerous wound dressings have been developed fo...The low temperature,high salt content,and bacterial composition of a seawater environment can induce severe infections in open wounds,thus impeding wound healing.To date,numerous wound dressings have been developed for injuries and various antibacterial functions.However,ordinary antibacterial strategies could not provide long-term resistance to infections and could not promote wound healing.Here,we proposed a strategy for enhancing resistance to seawater immersion wound infection by killing bacteria and delivering bacterial antigens in situ.Specifically,MXene-embedded tannin-Eu^(3+)(M@TA-Eu)particles were constructed to effectively alleviate injuries infected through seawater immersion and persistently fight infection by forming in situ bacterial vaccines and immune memory.In the particle,the platform composed of TA and Eu3+exhibited provascularization and antigen presentation effects.MXenes with near-infrared photothermal effect were introduced to kill the bacteria,promote the recruitment of antigen presentation cells,and ultimately enhance vaccination efficacy.Experimental results showed that the particles not only effectively accelerated the healing of injuries by relieving wound inflammation and inhibiting bacteria but also produced a potent vaccination by forming in situ bacterial vaccines.Therefore,the M@TA-Eu particles are novel materials for high-grade anti-infection dressing.展开更多
In recent years,cellulose-based fluorescent polymers have received considerable attention.However,conventional modification methods face challenges such as insolubility in most solvents,fluorescence instability,and en...In recent years,cellulose-based fluorescent polymers have received considerable attention.However,conventional modification methods face challenges such as insolubility in most solvents,fluorescence instability,and environmental risks.In this study,a novel biosynthesis strategy was developed to fabricate fluorescent cellulose by adding fluorescent glucose derivatives to a bacterial fermentation broth.The metabolic activity of bacteria is utilized to achieve in situ polymerization of glucose and its derivatives during the synthesis of bacterial cellulose.Owing to the structural similarity between triphenylamine-modified glucose(TPA-Glc N)and glucose monomers,the TPA-Glc N were efficiently assimilated by the bacterial cells and incorporated into the cellulose matrix,resulting in a uniform distribution of fluorescence.The fluorescence color and intensity of the obtained cellulose could be adjusted by varying the amount of the fluorescent glucose derivatives.Compared to the fluorescent cellulose synthesized through physical dyeing,the fluorescence of the products obtained by in situ polymerization showed higher intensity and stability.Furthermore,fluorescent bacterial cellulose can be hydrolyzed into nanocellulose-based ink,which demonstrates exceptional anti-counterfeiting capabilities under UV light.This biosynthesis method not only overcomes the limitations of traditional modification techniques but also highlights the potential of microbial systems as platforms for synthesizing functional polymers.展开更多
This study presents an approach to enhanced cancer immunotherapy through the in situ synthesis of potassium permanganate(KMnO_(4))derived manganese dioxide(MnO_(2))micro/nano-adjuvants.Addressing the limitations of tr...This study presents an approach to enhanced cancer immunotherapy through the in situ synthesis of potassium permanganate(KMnO_(4))derived manganese dioxide(MnO_(2))micro/nano-adjuvants.Addressing the limitations of traditional immunotherapy due to patient variability and the complexity of the tumor microenvironment,our research establishes KMnO_(4)as a potent immunomodulator that enhances the efficacy of anti-programmed death-ligand 1(αPD-L1)antibodies.The in situ synthesized MnO_(2)adjuvants in the tumor exhibit direct interactions with biological systems,leading to the reduction of MnO_(2)to Mn^(2+)within the tumor,and thereby improving the microenvironment for immune cell activity.Our in vitro and in vivo models demonstrate KMnO_(4)’s capability to induce concentration-dependent cytotoxicity in tumor cells,triggering DNA damage and apoptosis.It also potentiates immunogenic cell death by upregulating calreticulin and high mobility group box 1(HMGB1)on the cell surface.The combination of KMnO_(4)withαPD-L1 antibodies substantially inhibits tumor growth,promotes dendritic cell maturation,and enhances CD8^(+)T cell infiltration,resulting in a significant phenotypic shift in tumor-associated macrophages towards a pro-inflammatory M1 profile.Our findings advocate for further research into the long-term efficacy of KMnO_(4)and its application in diverse tumor models,emphasizing its potential to redefine immune checkpoint blockade therapy and offering a new vista in the fight against cancer.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos.92580120 and 52471188)。
文摘Optimizing the microchannel design of the next generation of chips requires an understanding of the in situ property evolution of the chip-based materials under fast cooling.This work overcomes the conventional reliance on reheating data of melt-quenched glasses by demonstrating direct observations of glass transition on cooling curves utilizing the most advanced fast differential scanning calorimetry.By leveraging an MEMS chip sensor that allows for rapid heat extraction from microgram-sized samples to a purged gas coolant,the device is able to reach ultra-fast cooling rates of up to 40,000 K·s^(−1).Four thermal regions are identified by examining the cooling behaviors of two metallic glasses.This is because the actual rate of the specimen can differ from the programmed rate,especially at high set rate when the actual rate decreases before the glass transition is completed.We define the operational window for reliable cooling curve analysis,build models with empirical and theoretical analyses to determine the maximum feasible cooling rate,and demonstrate how optimizing sample mass and environment temperature broaden this window.The method avoids deceptive structural relaxation effects verified by fictivetemperature analysis and permits the capture of full glass transition during cooling.
基金funding support from Natural Science Foundation of Shanghai(Grant No.23ZR1443900)the National Natural Science Foundation of China(Grant Nos.22178309,22476131 and 22176127)。
文摘Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.
基金supported by the National Nature Science Foundation of China(NSFC)(Grant Nos.22275004,62274040,and 62304046)the Shanghai Science and Technology Committee(Grant No.22JC1410300)+2 种基金the Shanghai Key Laboratory of Novel Extreme Condition Materials(Grant No.22dz2260800)the National Key Research and Development Program of China(Grant No.2022YFE0137400)the Shanghai Science and Technology Innovationaction Plan(Grant No.24DZ3001200).
文摘High-pressure research has emerged as a pivotal approach for advancing our understanding and development of optoelectronic materials,which are vital for a wide range of applications,including photovoltaics,light-emitting devices,and photodetectors.This review highlights various in situ characterization methods employed in high-pressure research to investigate the optical,electronic,and structural properties of optoelectronic materials.We explore the advances that have been made in techniques such as X-ray diffraction,absorption spectroscopy,nonlinear optics,photoluminescence spectroscopy,Raman spectroscopy,and photoresponse measurement,emphasizing how these methods have enhanced the elucidation of structural transitions,bandgap modulation,performance optimization,and carrier dynamics engineering.These insights underscore the pivotal role of high-pressure techniques in optimizing and tailoring optoelectronic materials for future applications.
基金supported by Guangzhou Development Zone Science and Technology(2021GH10,2020GH10,2023GH02)the University of Macao(MYRG2022-00271-FST)The Science and Technology Development Fund(FDCT)of Macao(0032/2022/A).
文摘Introduction Early cancer detection represents a critical evolution in healthcare,addressing a significant pain point in cancer treatment:the tendency for diagnoses to occur at advanced stages.Traditionally,many cancers are not identified until they have progressed to late stages,where treatment options become limited,less effective,and more costly.This late detection results in poorer prognoses,higher mortality rates,and increased healthcare costs.Without early detection tools like Fluorescence In Situ Hybridization(FISH),these challenges persist,leaving patients with fewer opportunities for successful outcomes.
基金supported by the National Natural Science Foundation of China(22238002 and 22208047)the China Postdoctoral Science Foundation(2024T170086 and 2022M720639)+1 种基金the Research and Innovation Team Project of Dalian University of Technology(DUT2022TB10)the Fundamental Research Funds for the Central Universities(DUT22LAB610)。
文摘Despite the ongoing increase in the efficiency of perovskite solar cells(PSCs),residual lead iodide(PbI2and moisture sensitivity issues continue to constrain their further commercialization.Herein,we propose a thermally mediated in situ repair and encapsulation strategy to construct high-performance PSCs by incorporating piperazine thioctic acid salt(TAPPZ)as a dopant into the perovskite precursor Thermally dissociated piperazine(PPZ)from TAPPZ integrates microcrystals to form larger grain(>2000 nm),while the carboxylic acid in thioctic acid(TA)and the amine salt in TAPPZ synergistically passivate and transform PbI_(2),significantly reducing its residual amount.Additionally,TAPPZ undergoe thermal self-crosslinking during perovskite annealing,enabling melt-polymerization to form in situ encapsulation for enhanced water resistance.The TAPPZ-incorporated device achieves a remarkable efficiency of 25.65% and exhibits excellent operational stability,retaining over 90% of its initial efficiency after 2000 h under ambient conditions(20-30℃,20%-30% relative humidity).This study provide new insights into the construction of high-performance perovskite solar cells by designing and synthe sizing multifunctional single molecules for in situ repair and encapsulation of perovskites.
基金funding support from National Natural Science Foundation of China(Grant Nos.52225403,51827901,and 52304146).
文摘The pressure-preserving controller is the key component of deep in situ pressure-preserving coring(IPP-Coring).With increasing drilling depth,the environmental temperature and pressure increase accordingly.However,due to the strength and sealing problems of pressure-preserving controllers,the coring pressure is generally lower than 70 MPa.Establishing a high-temperature and ultrahigh-pressure test system is highly important for improving the strength and sealing performance of pressure-preserving controllers.This paper introduces a high-temperature and ultrahigh-pressure test system for deep IPP-Coring controller performance analysis.The device includes six parts:an auxiliary air source system,a pressurization system,a temperature control system,a hydraulic system,a data acquisition and electrical control system,and an ultrahigh-pressure vessel.The test system can reconstruct a 150℃ and 200 MPa in situ environment and simulate and test the movement state of the corer and the stability of the pressure-preserving action trigger of the pressure-preserving controller in the deep IPP-Coring process.To verify the performance of this test system,saddle-shaped pressure-preserving controllers made of four different materials were subjected to pressure tests under normal-temperature and high-temperature conditions.The results showed that the ultimate pressure-bearing capability of the pressure-preserving controller greatly varied between normal-temperature and high-temperature conditions.The pressure-preserving ability and sealing performance of the pressure-preserving controller decreased significantly at high temperature,and the pressure-preserving controller exhibited significantly different sealing failure characteristics due to material differences.This study is important for progressing the extraction and evaluation of deep reservoir resources.
基金financially supported by the National Natural Science Foundation of China(No.52174342)Beijing Natural Sci-ence Foundation(No.2232044)Beijing Municipal Education Commission Research Plan General Project(No.KM202410005009).
文摘In this work,silicon-carbon hybrid materials were adopted as an example to illustrate the novel strategy to in situ construct heterostructure with adjustable microstructure.Based on the temperature-dependent thermodynamics and kinetics of reaction between Si and C,the processes for Si nanocrystals growth and C decoration were coupled at different zones of plasma flame according to its temperature and velocity fields by theoretical modeling,aiming to intentionally suppress the formation of undesirable carbide,and enable adjusting the microstructure of each counterpart separately in transient process.As a result,well-controlled Si/C nanocomposites,including nanospheres and nanowires with core-shell structures,were achieved,and this continuous and in-flight route is also potential for large-scale production.Further investigation on the electrochemical properties highlights the advantage of as proposed strategy to efficiently construct heterostructures with superior performance for various applications.
基金supported by National Natural Science Foundation of China(22090011)Liaoning Binhai Laboratory(LBLB-2023-03)Fundamental Research Funds for the Central Universities(DUT22LAB608).
文摘The clinical application of tumor vaccines is hindered by challenges such as timeconsuming and costly production processes.In this context,in situ cancer vaccines represent a promising strategy by leveraging endogenous tumor antigens to elicit robust antitumor T cell responses.Herein,a photoactivatable tumor-targeting in situ nanovaccine,Lipo-D8-6,was constructed using cRGD-functionalized liposomes that co-encapsulated the photosensitizer chlorin e6 and a cleavable immunoadjuvant conjugate D8,allowing light-triggered synchronous activation of three therapeutic modules.Upon near-infrared light irradiation,Lipo-D8-6 generates reactive oxygen species that exert direct cytotoxicity on tumor cells and induce immunogenic cell death,while concurrently cleaving the responsive linker within D8 to achieve the controlled release of R848.In vivo biodistribution analysis confirmed the superior intratumoral accumulation of Lipo-D8-6,facilitating precise treatment.In a large-volume tumor model,the nanovaccine exhibited pronounced antitumor efficacy,accompanied by enhanced tumor infiltration of CD8t T cells.Overall,this work provides a simplified and effective approach for developing in situ nanovaccines that enable synergistic photodynamic immunotherapy with precise spatiotemporal control over immune activation.
基金National Natural Science Foundation of China (52371228, 52402045)fund of Key Laboratory of Advanced Materials of Ministry of Education(Advmat-2414)。
文摘Electrocatalytic nitrate reduction reaction (NO_(3)-RR) to ammonia under ambient conditions is expected to be a green process for ammonia synthesis and alleviate water pollution issues.We report a CuO nanoparticles incorporated on nitrogen-doped porous carbon (CuO@NC) catalyst for NO_(3)-RR.Part of Cu(Ⅱ) is reduced to Cu(Ⅰ) during the NO_(3)-RR process to construct Cu(Ⅰ)-Cu(Ⅱ) pairs,confirmed by in situ X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy.Density functional theory (DFT) calculations indicated that the formation of Cu(Ⅰ) could provide a reaction path with smaller energy barrier for NO_(3)-RR,while Cu(Ⅱ) effectively suppressed the competition of hydrogen evolution reaction (HER).As a result,CuO@NC catalyst achieved a Faradaic efficiency of 84.2% at -0.49 V versus reversible hydrogen electrode (RHE),and a NH_(3)yield rate of 17.2 mg h^(-1)mg^(-1)cat.at -0.79 V vs.RHE,higher than the HaberBosch process (<3.4 g h^(-1)g^(-1)cat.).This work may open a new avenue for effective NO_(3)-RR by modulating oxidation states.
基金supported in part by the National Natural Science Foundation of China(Nos.52205532 and 624B2077)the National Key Research and Development Program of China(No.2023YFB4302003).
文摘The global demand for effective skin injury treatments has prompted the exploration of tissue engineering solutions.While three-dimensional(3D)bioprinting has shown promise,challenges persist with respect to achieving timely and compatible solutions to treat diverse skin injuries.In situ bioprinting has emerged as a key new technology,since it reduces risks during the implantation of printed scaffolds and demonstrates superior therapeutic effects.However,maintaining printing fidelity during in situ bioprinting remains a critical challenge,particularly with respect to model layering and path planning.This study proposes a novel optimization-based conformal path planning strategy for in situ bioprinting-based repair of complex skin injuries.This strategy employs constrained optimization to identify optimal waypoints on a point cloud-approximated curved surface,thereby ensuring a high degree of similarity between predesigned planar and surface-mapped 3D paths.Furthermore,this method is applicable for skin wound treatments,since it generates 3D-equidistant zigzag curves along surface tangents and enables multi-layer conformal path planning to facilitate the treatment of volumetric injuries.Furthermore,the proposed algorithm was found to be a feasible and effective treatment in a murine back injury model as well as in other complex models,thereby showcasing its potential to guide in situ bioprinting,enhance bioprinting fidelity,and facilitate improvement of clinical outcomes.
基金financially supported by the National Natural Science Foundation of China(Nos.22102212 and 22479067).
文摘High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.
基金financially supported by the National Key Research and Development Program of China(2022YFC3004601)the National Natural Science Foundation of China(52204084)the Science,Technology and Innovation Project of Xiongan New Area(2023XAGG0061).
文摘1.Introduction Various geological phenomena on the surface and in the interior of the Earth,as well as their associated physical and chemical pro-cesses,are closely correlated with the action of in situ rock stress[1-5].Understanding the rock stress state at great depths is not only an indispensable foundation for solving scientific problems associated with geology,geophysics,and geodynamics-such as plate-driving mechanisms,the earth’s energy equilibrium,earth-quake mechanisms,and tectonic activities-but also a necessary prerequisite for the evaluation,exploitation,and disposal of deep energy and resources,such as coal and metal minerals.Due to the complexity and uncertainty of the origin of in situ rock stress,it is a difficult quantity to evaluate,in comparison with other rock properties.Currently,reliable information on the stress state in a region can only be determined through field stress measurement.Therefore,a variety of stress measurement techniques have been developed and applied worldwide to provide information on crus-tal contemporary stress at specific depth ranges[6].
基金funded by the National Key R&D Program of China(Grant No.2022YFC2903904)the National Natural Science Foundation of China(Grant Nos.51904057 and U1906208).
文摘Due to the heterogeneity of rock masses and the variability of in situ stress,the traditional linear inversion method is insufficiently accurate to achieve high accuracy of the in situ stress field.To address this challenge,nonlinear stress boundaries for a numerical model are determined through regression analysis of a series of nonlinear coefficient matrices,which are derived from the bubbling method.Considering the randomness and flexibility of the bubbling method,a parametric study is conducted to determine recommended ranges for these parameters,including the standard deviation(σb)of bubble radii,the non-uniform coefficient matrix number(λ)for nonlinear stress boundaries,and the number(m)and positions of in situ stress measurement points.A model case study provides a reference for the selection of these parameters.Additionally,when the nonlinear in situ stress inversion method is employed,stress distortion inevitably occurs near model boundaries,aligning with the Saint Venant's principle.Two strategies are proposed accordingly:employing a systematic reduction of nonlinear coefficients to achieve high inversion accuracy while minimizing significant stress distortion,and excluding regions with severe stress distortion near the model edges while utilizing the central part of the model for subsequent simulations.These two strategies have been successfully implemented in the nonlinear in situ stress inversion of the Xincheng Gold Mine and have achieved higher inversion accuracy than the linear method.Specifically,the linear and nonlinear inversion methods yield root mean square errors(RMSE)of 4.15 and 3.2,and inversion relative errors(δAve)of 22.08%and 17.55%,respectively.Therefore,the nonlinear inversion method outperforms the traditional multiple linear regression method,even in the presence of a systematic reduction in the nonlinear stress boundaries.
基金Funded by Chinese National Natural Science Foundation of China(No.U2006224)。
文摘The paper presents experimental investigation results of crack pattern change in cement pastes caused by external sulfate attack(ESA).To visualize the formation and development of cracks in cement pastes under ESA,an X-ray computed tomography(X-ray CT)was used,i e,the tomography system of Zeiss Xradia 510 versa.The results indicate that X-CT can monitor the development process and distribution characteristics of the internal cracks of cement pastes under ESA with attack time.In addition,the C3A content in the cement significantly affects the damage mode of cement paste specimens during sulfate erosion.The damage of ordinary Portland cement(OPC)pastes subjected to sulfate attack with high C3A content are severe,while the damage of sulfate resistant Portland cement(SRPC)pastes is much smaller than that of OPC pastes.Furthermore,a quadratic function describes the correlation between the crack volume fraction and development depth for two cement pastes immermed in sulfate solution.
文摘Three efficient methods for the synthesis of a series of Cu(Ⅱ) and Cu(Ⅰ) complexes based on imidazo[1,5-a]pyridine derivatives were developed.These methods include the following:(ⅰ)Cu(Ⅱ) salts were used as metal sources and N,N-dimethylformamide was employed as a solvent as well as a reductant to produce Cu(Ⅰ) complexes.(ⅱ) An iodide-containing compound was utilized as a ligand and iodide source to prepare complexes.An in situ metalligand reaction occurred and an iodide-bridged copper complex was generated.(ⅲ) A series of aldehydes were added to the reaction systems to induce in situ metal-ligand reactions between the aldehydes and the imidazo[1,5-a]pyridine derivatives,producing polydentate ligand scaffolds.Eight complexes were prepared and characterized.The catalytic activities of these complexes toward the ketalization of ketones by ethylene glycol were investigated.With the exception of complex4,the remaining seven complexes all showed high catalytic activity.The lower activity of 4 may be due to the larger radius of bridging iodide ions and the shorter Cu(Ⅰ)…Cu(Ⅰ) distance.CCDC:2357696,1·2CH_(2)Cl_(2);2357697,2;2018292,3;2092192,4;2092190,5;2155557,6;2406155,7;2406156,8·EtOH.
基金Supported by the National Natural Science Foundation of China(42474239,41204128)China National Space Administration(Pre-research project on Civil Aerospace Technologies No.D010301)Strategic Priority Research Program of the Chinese Academy of Sciences(XDA17010303)。
文摘One of the detection objectives of the Chinese Asteroid Exploration mission is to investigate the space environment near the Main-belt Comet(MBC,Active Asteroid)311P/PANSTARRS.This paper outlines the scientific objectives,measurement targets,and measurement requirements for the proposed Gas and Ion Analyzer(GIA).The GIA is designed for in-situ mass spectrometry of neutral gases and low-energy ions,such as hydrogen,carbon,and oxygen,in the vicinity of 311P.Ion sampling techniques are essential for the GIA's Time-of-Flight(TOF)mass analysis capabilities.In this paper,we present an enhanced ion sampling technique through the development of an ion attraction model and an ion source model.The ion attraction model demonstrates that adjusting attraction grid voltage can enhance the detection efficiency of low-energy ions and mitigate the repulsive force of ions during sampling,which is influenced by the satellite's surface positive charging.The ion source model simulates the processes of gas ionization and ion multiplication.Simulation results indicate that the GIA can achieve a lower pressure limit below 10-13Pa and possess a dynamic range exceeding 10~9.These performances ensure the generation of ions with stable and consistent current,which is crucial for high-resolution and broad dynamic range mass spectrometer analysis.Preliminary testing experiments have verified GIA's capability to detect gas compositions such as H2O and N2.In-situ measurements near 311P using GIA are expected to significantly contribute to our understanding of asteroid activity mechanisms,the evolution of the atmospheric and ionized environments of main-belt comets,the interactions with solar wind,and the origin of Earth's water.
基金supported by the National Natural Science Foundation of China(62204074)the Hebei Natural Science Foundation(F2022201061,F2023201025)+2 种基金the Open bidding for selecting the best candidates of Baoding(2023chuang206)the High-level Talent Research Startup Project of Hebei University(521100221085)the Post-graduate's Innovation Fund Project of Hebei University(HBU2024BS030).
文摘Despite sulfurization offers the advantage of improving the photovoltaic performance in preparing Cu(In,Ga)Se2(CIGS)absorbers,deep level defects in the absorber and poor energy level alignment on the front surface are still main obstacles limiting the improvement of power co nversion efficiency(PCE)in sulfided CIGS solar cells.Herein,an in-situ Na doping strategy is proposed,in which the tailing effect of crystal growth is used to promote the sulfurization of CIGS absorbers.It is found that the grain growth is supported by Na incorporating due to the enrichment of NaSe_(x)near the upper surface.The high soluble Na during grain growth can not only suppress intrinsic In_(Cu) donor defects in the absorber,but also tailor S distribution in bulk and the band alignment at the heterojunction,which are both beneficial for the effective electron carriers.Meanwhile,the Na aggregation near the bottom of the absorber also contributes to the crystalline quality increasing and favorable ultra-thin MoSe_(2) formation at back contact,resulting in a reduced barrier height conducive to hole transport.PCE of the champion device is as high as 16.76%with a 28%increase.This research offers new insights into synthesizing CIGS solar cells and other chalcogenide solar cells with superior cell performance when using an intense sulfurization process.
基金supported by the National Key Research and Development Program of China(No.2018YFC0311103)the Project of Science and Technology Innovation Cultivation for University Students of Guangdong Province(No.pdjh202010062)+6 种基金the Science and Technology Project of Guangzhou City(No.2018020100)the General Program of China Postdoctoral Science Foundation(No.2021M701599)the National Natural Science Foundation of China(No.32201083)the Science and Technology Program of Heyuan,China(No.230510171473326)the Science and Technology Program of Guangzhou,China(No.2024A03J0232)the Medical Scientific Research Foundation of Guangdong Province of China(No.A2020548)the Fundamental Research Funds for the Central Universities,China(No.21623403).
文摘The low temperature,high salt content,and bacterial composition of a seawater environment can induce severe infections in open wounds,thus impeding wound healing.To date,numerous wound dressings have been developed for injuries and various antibacterial functions.However,ordinary antibacterial strategies could not provide long-term resistance to infections and could not promote wound healing.Here,we proposed a strategy for enhancing resistance to seawater immersion wound infection by killing bacteria and delivering bacterial antigens in situ.Specifically,MXene-embedded tannin-Eu^(3+)(M@TA-Eu)particles were constructed to effectively alleviate injuries infected through seawater immersion and persistently fight infection by forming in situ bacterial vaccines and immune memory.In the particle,the platform composed of TA and Eu3+exhibited provascularization and antigen presentation effects.MXenes with near-infrared photothermal effect were introduced to kill the bacteria,promote the recruitment of antigen presentation cells,and ultimately enhance vaccination efficacy.Experimental results showed that the particles not only effectively accelerated the healing of injuries by relieving wound inflammation and inhibiting bacteria but also produced a potent vaccination by forming in situ bacterial vaccines.Therefore,the M@TA-Eu particles are novel materials for high-grade anti-infection dressing.
基金supported by the National Natural Science Foundation of China(No.22376111)Shandong Provincial Natural Science Foundation(No.ZR2024YQ026)+2 种基金for Excellent Young Scholars,Taishan Scholar Foundation of Shandong Province(No.tsqn202408237)Youth Innovation Team Project for Talent Introduction and Cultivation in Universities of Shandong Province(No.096-1622002)the Research Foundation for Distinguished Scholars of Qingdao Agricultural University(No.663-1117015)。
文摘In recent years,cellulose-based fluorescent polymers have received considerable attention.However,conventional modification methods face challenges such as insolubility in most solvents,fluorescence instability,and environmental risks.In this study,a novel biosynthesis strategy was developed to fabricate fluorescent cellulose by adding fluorescent glucose derivatives to a bacterial fermentation broth.The metabolic activity of bacteria is utilized to achieve in situ polymerization of glucose and its derivatives during the synthesis of bacterial cellulose.Owing to the structural similarity between triphenylamine-modified glucose(TPA-Glc N)and glucose monomers,the TPA-Glc N were efficiently assimilated by the bacterial cells and incorporated into the cellulose matrix,resulting in a uniform distribution of fluorescence.The fluorescence color and intensity of the obtained cellulose could be adjusted by varying the amount of the fluorescent glucose derivatives.Compared to the fluorescent cellulose synthesized through physical dyeing,the fluorescence of the products obtained by in situ polymerization showed higher intensity and stability.Furthermore,fluorescent bacterial cellulose can be hydrolyzed into nanocellulose-based ink,which demonstrates exceptional anti-counterfeiting capabilities under UV light.This biosynthesis method not only overcomes the limitations of traditional modification techniques but also highlights the potential of microbial systems as platforms for synthesizing functional polymers.
基金supported by the Natural Science Foundation of Guangdong Province(No.2023A1515030291)the Dongguan Science and Technology of Social Development Program(No.20211800905282)+8 种基金the National Key Research and Development Program of China(Nos.2022YFC2303600,2020YFA0908000)the Innovation Team and Talents Cultivation Program of National Administration of Traditional Chinese Medicine(No.ZYYCXTDC-202002)the CACMS Innovation Fund(Nos.CI2023E002,CI2021A05101,CI2021A05104)the Scientific and Technological Innovation Project of China Academy of Chinese Medical Sciences(Nos.CI2023D003,CI2021B014)the Science and Technology Foundation of Shenzhen(No.JCYJ20210324115800001)the Science and Technology Foundation of Shenzhen(Shenzhen Clinical Medical Research Center for Geriatric Diseases)the Shenzhen Medical Research Fund(No.B2302051)the Distinguished Expert Project of Sichuan Province Tianfu Scholar(No.CW202002)Shenzhen Science and Technology Program(No.RCBS20210609104424065).
文摘This study presents an approach to enhanced cancer immunotherapy through the in situ synthesis of potassium permanganate(KMnO_(4))derived manganese dioxide(MnO_(2))micro/nano-adjuvants.Addressing the limitations of traditional immunotherapy due to patient variability and the complexity of the tumor microenvironment,our research establishes KMnO_(4)as a potent immunomodulator that enhances the efficacy of anti-programmed death-ligand 1(αPD-L1)antibodies.The in situ synthesized MnO_(2)adjuvants in the tumor exhibit direct interactions with biological systems,leading to the reduction of MnO_(2)to Mn^(2+)within the tumor,and thereby improving the microenvironment for immune cell activity.Our in vitro and in vivo models demonstrate KMnO_(4)’s capability to induce concentration-dependent cytotoxicity in tumor cells,triggering DNA damage and apoptosis.It also potentiates immunogenic cell death by upregulating calreticulin and high mobility group box 1(HMGB1)on the cell surface.The combination of KMnO_(4)withαPD-L1 antibodies substantially inhibits tumor growth,promotes dendritic cell maturation,and enhances CD8^(+)T cell infiltration,resulting in a significant phenotypic shift in tumor-associated macrophages towards a pro-inflammatory M1 profile.Our findings advocate for further research into the long-term efficacy of KMnO_(4)and its application in diverse tumor models,emphasizing its potential to redefine immune checkpoint blockade therapy and offering a new vista in the fight against cancer.
