Ferroptosis is a newly proposed type of programmed cell death,which has been associated with a variety of diseases including tumors.Researchers have thereby presented nanoplatforms to mediate ferroptosis for anti-canc...Ferroptosis is a newly proposed type of programmed cell death,which has been associated with a variety of diseases including tumors.Researchers have thereby presented nanoplatforms to mediate ferroptosis for anti-cancer therapy.However,the development of ferroptosis-based nanotherapeutics is generally hindered by the limited penetration depth in tumors,poor active pharmaceutical ingredient(API)loading content and the systemic toxicity.Herein,self-propelled ferroptosis nanoinducers composed of two endogenous proteins,glucose oxidase and ferritin,are presented to show enhanced tumor inhibition via ferroptosis while maintaining high API and biocompatibility.The accumulation of our proteomotors at tumor regions is facilitated by the active tumor-targeting effect of ferritin.The enhanced diffusion of proteomotors is then actuated by efficiently decomposing glucose into gluconic acid and H_(2)O_(2),leading to deeper penetration and enhanced uptake into tumors.Under the synergistic effect of glucose oxidase and ferritin,the equilibrium between reactive oxygen species and GSH is damaged,leading to lipid peroxidation.As a result,by inducing ferroptosis,our self-propelled ferroptosis nanoinducers exhibit enhanced tumor inhibitory effects.This work paves a way for the construction of a biocompatible anticancer platform with enhanced diffusion utilizing only two endogenous proteins,centered around the concept of ferroptosis.展开更多
In this paper, we experimentally investigate the dark diffusional enhancement of the optimized multiplexed grating in the phenanthrenequinone doped poly （methyl methacrylate） （PQ-PMMA） photopolymer. The possibilit...In this paper, we experimentally investigate the dark diffusional enhancement of the optimized multiplexed grating in the phenanthrenequinone doped poly （methyl methacrylate） （PQ-PMMA） photopolymer. The possibility of improving the holographic characteristics of the material through the dark enhancement is demonstrated. The optimal preillumination exposure and the optimal time interval between exposures are extracted to obtain the optimized diffraction efficiency, and their values are 3.4×103 mJ/cm2 and 2 min, respectively. The dark enhancement of the multiplexed grating is presented as an effective method to improve the response region and the dynamic range and to prevent saturation of the material. The dependence of the phenanthrenequinone concentration on the increment of the refractive index modulation is quantitatively studied, which provides a significant basis for improving the homogeneity in the multiplexed gratings using a quantitative strategy. Finally, a simple experimental procedure using the dark enhancement is introduced to improve the homogeneity of the diffraction efficiency and to avoid the complex schedule exposure.展开更多
Diffusion of a particle on a tilted periodic surface such as the egg-carton potential is investigated using Langevin Monte Carlo simulations. It is found that the effective diffusion coefficient of the particle relate...Diffusion of a particle on a tilted periodic surface such as the egg-carton potential is investigated using Langevin Monte Carlo simulations. It is found that the effective diffusion coefficient of the particle related to the one- dimensional case can be greatly enhanced, when the local minima of such potential along the x and y directions are close to vanishing. A relation between the group diffusion and the phase diffusion is used to analyze the enhancement mechanism of the diffusion.展开更多
Na_(2)FePO_(4)F is a promising sodium ion cathode due to its low cost,non-toxicity,and high stability.However,the sluggish Na^(+)diffusion kinetics and limited intrinsic electronic conductivity critically restrict its...Na_(2)FePO_(4)F is a promising sodium ion cathode due to its low cost,non-toxicity,and high stability.However,the sluggish Na^(+)diffusion kinetics and limited intrinsic electronic conductivity critically restrict its worldwide application.Herein,an anion-substitution strategy is proposed with SiO_(4)^(4-)as the dopant.SiO_(4)^(4-)substitution for PO_(4)^(3-)can apparently alter the localized electronic density and structural configuration in the lattice of Na_(2)FePO_(4)F,effectively elevating the charge transfer efficiency.As a result,the electrochemical reaction kinetics of Na_(2)FePO_(4)F is significantly enhanced,which is well demonstrated by a series of electrochemical characterizations.As-obtained Na_(2.2)Fe(PO_(4))_(0.8)(SiO_(4))_(0.2)F renders a specific capacity of 84.9 m A h g^(-1)within the region of 2.5-4.0 V at 60 mA g^(-1)(0.5 C),good rate capability,and a capacity retention of 70.0% after 1000 cycles at 1.24 A g^(-1)(10 C).Furthermore,the stabilities of the cathode-electrolyte interface and structure are strengthened,which are verified by in situ EIS and ex situ XRD analysis.These findings highlight silicate anion substitution as a promising and cost-effective strategy for overcoming the limitations of Na_(2)FePO_(4)F,contributing to the development of sustainable energy storage solutions.展开更多
Na-ion cathode materials with a fast charge and discharge behavior are needed to develop future high energy sodium-ion batteries(SIBs).However,inevitably complicated phase transitions and sluggish kinet ics during ins...Na-ion cathode materials with a fast charge and discharge behavior are needed to develop future high energy sodium-ion batteries(SIBs).However,inevitably complicated phase transitions and sluggish kinet ics during insertion and removal of Na+in P_(2)-type layered transition metal oxides generate structura instability and severe capacity decay.To get rid of such a dilemma,we report a structural optimization strategy to promote P2-type layered transition metal oxides with more(010)active planes as an efficien cathode for SIBs.As a result,as-prepared hexagonal-prism P2-type layered Na_(0.71)Ni_(0.16)Li_(0.09)Co_(0.16)Mn0.6O_(2)cathode with more(010)active planes delivers a reversible capacity of 120.1 mAh/g at 0.1 C,impressive rate capability of 52.7 m Ah/g at 10 C,and long-term cycling stability(capacity retention of 95.6%ove200 cycles).The outstanding electrochemical performance benefited from the unique hexagonal-prism with more(010)active facets,which can effectively shorten the diffusion distances of Na+,increase the Na-ion migration dynamics and nanostructural stability during cycling verified by morphology character ization,Rietveld refinement,GITT,density functional theory calculations and operando XRD.展开更多
Enzyme-driven micro/nanomotors consuming in situ chemical fuels have attracted lots of attention for biomedical applications.However,motor systems composed by organism-derived organics that maximize the therapeutic ef...Enzyme-driven micro/nanomotors consuming in situ chemical fuels have attracted lots of attention for biomedical applications.However,motor systems composed by organism-derived organics that maximize the therapeutic efficacy of enzymatic products remain challenging.Herein,swimming proteomotors based on biocompatible urease and human serum albumin are constructed for enhanced antitumor therapy via active motion and ammonia amplification.By decomposing urea into carbon dioxide and ammonia,the designed proteomotors are endowed with self-propulsive capability,which leads to improved internalization and enhanced penetration in vitro.As a glutamine synthetase inhibitor,the loaded L-methionine sulfoximine further prevents the conversion of toxic ammonia into non-toxic glutamine in both tumor and stromal cells,resulting in local ammonia amplification.After intravesical instillation,the proteomotors achieve longer bladder retention and thus significantly inhibit the growth of orthotopic bladder tumor in vivo without adverse effects.We envision that the as-developed swimming proteomotors with amplification of the product toxicity may be a potential platform for active cancer treatment.展开更多
CONSPECTUS:Nanocatalysts have shown remarkable potential for various catalytic reactions due to their high specific surface area.But the inherently high surface energy of these nanocatalysts promotes spontaneous growt...CONSPECTUS:Nanocatalysts have shown remarkable potential for various catalytic reactions due to their high specific surface area.But the inherently high surface energy of these nanocatalysts promotes spontaneous growth,leading to their instability under harsh catalytic conditions.Additionally,high-temperature treatment is an important way to prepare nanocatalysts because it can enhance atomic diffusion and generate a wide range of nanocatalysts.Unfortunately,many nanocatalysts suffer from inevitable aggregation and fusion during the high-temperature treatment procedure and thus face challenges in controlling their sizes and morphologies.In recent decades,significant progress has been achieved in synthesizing silica with a controllable thickness and mesoporous structures.The construction of silica on nanocatalysts as a protective shell,including core@shell,yolk@shell,or reverse bubble-ball structures,proves to be an effective strategy to prevent aggregation under harsh catalytic conditions.Furthermore,the subsequent etching of the silica shell,similar to protection/deprotection procedures in organic synthesis,enables the successful synthesis of nanocatalysts with controllable size and morphology under high-temperature conditions.In this Account,we provide an overview of the key role of silica in protecting and controllably synthesizing nanocatalysts,focusing on the optimization of their sizes,phases,and morphologies for improved catalytic performance and broader applications.First,we highlight the design principles of yolk@shell and reverse-bumpy-ball nanoreactors.These nanoreactors incorporate single or multiple nanoparticles effectively and impart enhanced properties to the synthesized nanocatalysts.Furthermore,we discuss recent advancements in silica encapsulation strategies that facilitate the fabrication of diverse nanocatalysts with tunable sizes and superior catalytic capabilities even under high-temperature conditions.The materials synthesized by these strategies include noble metalbased alloys and intermetallic compounds,non-noble-metal-based interstitial compounds,sulfides,oxides,and carbon-based materials.By examining the protective effects of silica and underscoring its critical role,we shed light on the potential as well as the challenges associated with employing silica encapsulation techniques in the design of high-performance nanocatalysts.We hope that this Account serves as an informative resource for researchers interested in the controllable synthesis of nanocatalysts;meanwhile,it can inspire the development of novel nanocatalysts through the utilization of encapsulation strategies.展开更多
基金supported by National Key Research and Development Program of China(No.2022YFA1206900)National Natural Science Foundation of China(Nos.22175083,82204415,51973241,22375224)GuangDong Basic and Applied Basic Research Foundation(No.2021A1515220187)。
文摘Ferroptosis is a newly proposed type of programmed cell death,which has been associated with a variety of diseases including tumors.Researchers have thereby presented nanoplatforms to mediate ferroptosis for anti-cancer therapy.However,the development of ferroptosis-based nanotherapeutics is generally hindered by the limited penetration depth in tumors,poor active pharmaceutical ingredient(API)loading content and the systemic toxicity.Herein,self-propelled ferroptosis nanoinducers composed of two endogenous proteins,glucose oxidase and ferritin,are presented to show enhanced tumor inhibition via ferroptosis while maintaining high API and biocompatibility.The accumulation of our proteomotors at tumor regions is facilitated by the active tumor-targeting effect of ferritin.The enhanced diffusion of proteomotors is then actuated by efficiently decomposing glucose into gluconic acid and H_(2)O_(2),leading to deeper penetration and enhanced uptake into tumors.Under the synergistic effect of glucose oxidase and ferritin,the equilibrium between reactive oxygen species and GSH is damaged,leading to lipid peroxidation.As a result,by inducing ferroptosis,our self-propelled ferroptosis nanoinducers exhibit enhanced tumor inhibitory effects.This work paves a way for the construction of a biocompatible anticancer platform with enhanced diffusion utilizing only two endogenous proteins,centered around the concept of ferroptosis.
基金supported by the National Basic Research Program of China(Grant No.2007CB3070001)the Fundamental Research Funds for the Central Universities,China(Grant No.HIT.NSRIF.2010009)+1 种基金the Program of Excellent Team in Harbin Institute of Technology,Chinathe Research Startup Foundation of Civil Aviation University of China(Grant No.2010QN03X)
文摘In this paper, we experimentally investigate the dark diffusional enhancement of the optimized multiplexed grating in the phenanthrenequinone doped poly （methyl methacrylate） （PQ-PMMA） photopolymer. The possibility of improving the holographic characteristics of the material through the dark enhancement is demonstrated. The optimal preillumination exposure and the optimal time interval between exposures are extracted to obtain the optimized diffraction efficiency, and their values are 3.4×103 mJ/cm2 and 2 min, respectively. The dark enhancement of the multiplexed grating is presented as an effective method to improve the response region and the dynamic range and to prevent saturation of the material. The dependence of the phenanthrenequinone concentration on the increment of the refractive index modulation is quantitatively studied, which provides a significant basis for improving the homogeneity in the multiplexed gratings using a quantitative strategy. Finally, a simple experimental procedure using the dark enhancement is introduced to improve the homogeneity of the diffraction efficiency and to avoid the complex schedule exposure.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11575024 and 11175021the Plan of Beijing College Students'Scientific Research and EntrePrenurial Action under Grant No 105820
文摘Diffusion of a particle on a tilted periodic surface such as the egg-carton potential is investigated using Langevin Monte Carlo simulations. It is found that the effective diffusion coefficient of the particle related to the one- dimensional case can be greatly enhanced, when the local minima of such potential along the x and y directions are close to vanishing. A relation between the group diffusion and the phase diffusion is used to analyze the enhancement mechanism of the diffusion.
基金funding support from the Beijing Natural Science Foundation(2252055)the National Natural Science Foundation of China(52072033 and 52271234)+1 种基金the State Key Laboratory of Clean Energy Utilization(Open Fund Project,ZJUCEU2024010)the BIT Research and Innovation Promoting Project(2024YCXY040,GIIP2023-34)。
文摘Na_(2)FePO_(4)F is a promising sodium ion cathode due to its low cost,non-toxicity,and high stability.However,the sluggish Na^(+)diffusion kinetics and limited intrinsic electronic conductivity critically restrict its worldwide application.Herein,an anion-substitution strategy is proposed with SiO_(4)^(4-)as the dopant.SiO_(4)^(4-)substitution for PO_(4)^(3-)can apparently alter the localized electronic density and structural configuration in the lattice of Na_(2)FePO_(4)F,effectively elevating the charge transfer efficiency.As a result,the electrochemical reaction kinetics of Na_(2)FePO_(4)F is significantly enhanced,which is well demonstrated by a series of electrochemical characterizations.As-obtained Na_(2.2)Fe(PO_(4))_(0.8)(SiO_(4))_(0.2)F renders a specific capacity of 84.9 m A h g^(-1)within the region of 2.5-4.0 V at 60 mA g^(-1)(0.5 C),good rate capability,and a capacity retention of 70.0% after 1000 cycles at 1.24 A g^(-1)(10 C).Furthermore,the stabilities of the cathode-electrolyte interface and structure are strengthened,which are verified by in situ EIS and ex situ XRD analysis.These findings highlight silicate anion substitution as a promising and cost-effective strategy for overcoming the limitations of Na_(2)FePO_(4)F,contributing to the development of sustainable energy storage solutions.
基金financially supported by the National Natural Science Foundation of China(Nos.52372188,51902090)Henan Key Research Project Plan for Higher Education Institutions(No.23A150038)+6 种基金2023 Introduction of Studying Abroad Talent Program“111”Project(No.D17007)Henan Provincial Key Scientific Research Project of Colleges and Universities(No23A150038)Key Scientific Research Project of Education Department of Henan Province(No.22A150042)the National Students’Platform for Innovation and Entrepreneurship Training Program(No.201910476010)the China Postdoctoral Science Foundation(No.2019 M652546)the Henan Province Postdoctoral StartUp Foundation(No.1901017)。
文摘Na-ion cathode materials with a fast charge and discharge behavior are needed to develop future high energy sodium-ion batteries(SIBs).However,inevitably complicated phase transitions and sluggish kinet ics during insertion and removal of Na+in P_(2)-type layered transition metal oxides generate structura instability and severe capacity decay.To get rid of such a dilemma,we report a structural optimization strategy to promote P2-type layered transition metal oxides with more(010)active planes as an efficien cathode for SIBs.As a result,as-prepared hexagonal-prism P2-type layered Na_(0.71)Ni_(0.16)Li_(0.09)Co_(0.16)Mn0.6O_(2)cathode with more(010)active planes delivers a reversible capacity of 120.1 mAh/g at 0.1 C,impressive rate capability of 52.7 m Ah/g at 10 C,and long-term cycling stability(capacity retention of 95.6%ove200 cycles).The outstanding electrochemical performance benefited from the unique hexagonal-prism with more(010)active facets,which can effectively shorten the diffusion distances of Na+,increase the Na-ion migration dynamics and nanostructural stability during cycling verified by morphology character ization,Rietveld refinement,GITT,density functional theory calculations and operando XRD.
基金supported by the National Natural Science Foundation of China(22175083,51973241,31900567 and 82102051)the Guangzhou Basic and Applied Basic Research Foundation(202201011078)。
文摘Enzyme-driven micro/nanomotors consuming in situ chemical fuels have attracted lots of attention for biomedical applications.However,motor systems composed by organism-derived organics that maximize the therapeutic efficacy of enzymatic products remain challenging.Herein,swimming proteomotors based on biocompatible urease and human serum albumin are constructed for enhanced antitumor therapy via active motion and ammonia amplification.By decomposing urea into carbon dioxide and ammonia,the designed proteomotors are endowed with self-propulsive capability,which leads to improved internalization and enhanced penetration in vitro.As a glutamine synthetase inhibitor,the loaded L-methionine sulfoximine further prevents the conversion of toxic ammonia into non-toxic glutamine in both tumor and stromal cells,resulting in local ammonia amplification.After intravesical instillation,the proteomotors achieve longer bladder retention and thus significantly inhibit the growth of orthotopic bladder tumor in vivo without adverse effects.We envision that the as-developed swimming proteomotors with amplification of the product toxicity may be a potential platform for active cancer treatment.
基金financial support from the National Key R&D Program of China(2021YFF0500402)the National Natural Science Foundation of China(51825205,2120105002,22088102,22279150)+1 种基金the Beijing Natural Science Foundation(2222080)the Youth Innovation Promotion Association of the CAS(Y2021011).
文摘CONSPECTUS:Nanocatalysts have shown remarkable potential for various catalytic reactions due to their high specific surface area.But the inherently high surface energy of these nanocatalysts promotes spontaneous growth,leading to their instability under harsh catalytic conditions.Additionally,high-temperature treatment is an important way to prepare nanocatalysts because it can enhance atomic diffusion and generate a wide range of nanocatalysts.Unfortunately,many nanocatalysts suffer from inevitable aggregation and fusion during the high-temperature treatment procedure and thus face challenges in controlling their sizes and morphologies.In recent decades,significant progress has been achieved in synthesizing silica with a controllable thickness and mesoporous structures.The construction of silica on nanocatalysts as a protective shell,including core@shell,yolk@shell,or reverse bubble-ball structures,proves to be an effective strategy to prevent aggregation under harsh catalytic conditions.Furthermore,the subsequent etching of the silica shell,similar to protection/deprotection procedures in organic synthesis,enables the successful synthesis of nanocatalysts with controllable size and morphology under high-temperature conditions.In this Account,we provide an overview of the key role of silica in protecting and controllably synthesizing nanocatalysts,focusing on the optimization of their sizes,phases,and morphologies for improved catalytic performance and broader applications.First,we highlight the design principles of yolk@shell and reverse-bumpy-ball nanoreactors.These nanoreactors incorporate single or multiple nanoparticles effectively and impart enhanced properties to the synthesized nanocatalysts.Furthermore,we discuss recent advancements in silica encapsulation strategies that facilitate the fabrication of diverse nanocatalysts with tunable sizes and superior catalytic capabilities even under high-temperature conditions.The materials synthesized by these strategies include noble metalbased alloys and intermetallic compounds,non-noble-metal-based interstitial compounds,sulfides,oxides,and carbon-based materials.By examining the protective effects of silica and underscoring its critical role,we shed light on the potential as well as the challenges associated with employing silica encapsulation techniques in the design of high-performance nanocatalysts.We hope that this Account serves as an informative resource for researchers interested in the controllable synthesis of nanocatalysts;meanwhile,it can inspire the development of novel nanocatalysts through the utilization of encapsulation strategies.
