For decades,Xu has been committed to fulfilling the duty and mission of a scientist and educator—diving into the laws of nature,caring deeply for the nation,and earnestly cultivating younger generations.
From cracking the code of viruses to mentoring the next generation of scientists,the former president of Nankai University has contributed a lot to turning microscopic discoveries into monumental shields for global he...From cracking the code of viruses to mentoring the next generation of scientists,the former president of Nankai University has contributed a lot to turning microscopic discoveries into monumental shields for global health.OVER the past 40 years,one man has distinguished himself through a deep commitment to researching protein structures of high pathogenic viruses,and published numerous significant works in top international scientific journals.展开更多
While biomaterials are endowed with sophisticated functions by the temporal dynamics and autonomy derived from non-equilibrium assemblies in biological systems,fabricating advanced materials counterparts with these fe...While biomaterials are endowed with sophisticated functions by the temporal dynamics and autonomy derived from non-equilibrium assemblies in biological systems,fabricating advanced materials counterparts with these features through kinetic control remains rare.Herein,we report a non-equilibrium hydrogel that exhibits autonomous time-dependent ultrabright fluorescence(quantum yield 0.90),achieved through the kinetically controlled incorporation of thermodynamic equilibrium host-vip complexes into a poly(2-hydroxyethyl methacrylate)(PHEMA)network.Transient complexes are programmed by coupling rapid assembly kinetics with the slow competitive binding of the polymer matrix.This kinetic mismatch converts a thermodynamic equilibrium supramolecular system into a non-equilibrium state,generating temporally dynamic fluorescence that cyclically shifts from yellow to green and self-reverts.The programmed temporal dynamics endow the hydrogel with high potential for information encryption applications.展开更多
The diagnostic efficacy of contemporary bioimaging technologies remains constrained by inherent limitations of conventional imaging agents,including suboptimal sensitivity,off-target biodistribution,and inherent cytot...The diagnostic efficacy of contemporary bioimaging technologies remains constrained by inherent limitations of conventional imaging agents,including suboptimal sensitivity,off-target biodistribution,and inherent cytotoxicity.These limitations have catalyzed the development of intelligent stimuli-responsive block copolymers-based bioimaging agents,which was engineered to dynamically respond to endogenous biochemical cues(e.g.,p H gradients,redox potential,enzyme activity,hypoxia environment) or exogenous physical triggers(e.g.,photoirradiation,thermal gradients,ultrasound(US)/magnetic stimuli).Through spatiotemporally controlled structural transformations,stimuli-responsive block copolymers enable precise contrast targeting,activatable signal amplification,and theranostic integration,thereby substantially enhancing signal-to-noise ratios of bioimaging and diagnostic specificity.Hence,this mini-review systematically examines molecular engineering principles for designing p H-,redox-,enzyme-,light-,thermo-,and US/magnetic-responsive polymers,with emphasis on structure-property relationships governing imaging performance modulation.Furthermore,we critically analyze emerging strategies for optical imaging,US synergies,and magnetic resonance imaging(MRI).Multimodal bioimaging has also been elaborated,which could overcome the inherent trade-offs between resolution,penetration depth,and functional specificity in single-modal approaches.By elucidating mechanistic insights and translational challenges,this mini-review aims to establish a design framework of stimuli-responsive block copolymersbased for high fidelity bioimaging agents and accelerate their clinical translation in precise diagnosis and therapy.展开更多
Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science.Recently,supramolecular polymeric materials(SPMs)have drawn increased ...Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science.Recently,supramolecular polymeric materials(SPMs)have drawn increased attention due to their unique properties and potential applications in self-healing,shape memory,sensors,and flexible electronics.Here,we develop an ionic cluster-optimized microphase separation strategy to enhance the toughening and energy dissipation capabilities of polydisulfide-based supramolecular polymers.The mechanical properties,including Young's modulus and toughness,are significantly improved by integrating the quadruple H-bonding 2-ureido-4-pyrimidone(UPy)induced microphase separation with iron(III)-to-carboxylate ionic clusters.By combining established chemical approaches with adjustable polymer phase ratios,it is revealed that the synergistic effect of these factors expands the interchain spacing,facilitates the formation of microphase domains,and enhances the tolerance of polythioctic acid-based polymers to external mechanical and thermal stimuli,meeting the practical requirements for industrial plastic applications.Moreover,the UPy-functionalized polymers incorporating iron carboxylate clusters exhibit good one-way shape memory behavior with practical applicability at a relatively low recovery temperature.Our work demonstrates a novel strategy for constructing industrially viable shape memory dynamic SPMs and paves the way for future innovations in developing SPMs.展开更多
As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term...As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.展开更多
Controllable photoreaction transition of photosensitizers(PSs)provides a highly promising approach for achieving efficient photodynamic therapy(PDT).However,tumor microenvironment-triggered phototransition remains a s...Controllable photoreaction transition of photosensitizers(PSs)provides a highly promising approach for achieving efficient photodynamic therapy(PDT).However,tumor microenvironment-triggered phototransition remains a significant challenge and has not yet been reported.In this work,we develop a hydrogen bond self-assembly(HBSA)strategy that is triggered by the acidic tumor microenvironment to enable the photodynamic transition of tetra(4-carboxylphenyl)porphyrin(TCPP)PSs from type Ⅱ to type Ⅰ reactions.Upon self-assembly of TCPP monomers into TCPP assemblies(TCPP-ass),the generated reactive oxygen species shift from singlet oxygen to superoxide anions,which induces caspase-3/GSDME-mediated programmed pyroptosis,enabling rapid and complete solid tumor elimination with minimized adverse effects and enhanced therapeutic efficacy.Crucially,the HBSA process occurs exclusively within tumor cells,and this tumor-specific self-assembly strategy not only utilizes high tissue penetration of TCPP molecular-PSs,but also avoids phototoxicity caused by the formation and accumulation of TCPP-ass nano-PSs in normal tissue,providing an innovative approach for precise cancer therapy.展开更多
Objectives:Colorectal cancer(CRC)is a major global health burden,and Urolithin A(Uro-A)has emerged as a promising anticancer agent.This systematic review aims to synthesize current in vitro evidence on the anticancer ...Objectives:Colorectal cancer(CRC)is a major global health burden,and Urolithin A(Uro-A)has emerged as a promising anticancer agent.This systematic review aims to synthesize current in vitro evidence on the anticancer effects of Uro-A in CRC,highlighting effective concentration ranges,exposure times,relevant outcomes,and underlying molecular mechanisms.Methods:Following PRISMA 2020 guidelines,a systematic search was conducted in PubMed,Scopus,and Web of Science using the following strategy:(colorectal cancer)AND(urolithin a)OR(3,8-dihydroxy-6H-dibenzo(b,d)pyran-6-one).Eligibility criteria were defined by the PICO framework:(P)in vitro CRC cell models;(I)Uro-A alone or combined treatments;(C)No intervention,vehicle or other treatments;(O)Relevant anticancer outcomes of Uro-A in CRC.Only original,full-text,in vitro studies in English were included.Risk of bias was assessed using ToxRTool.A qualitative synthesis was performed due to the heterogeneity of the included studies.Results:Fifteen studies met inclusion criteria,involving CRC cell lines(Caco-2,HCT-116,HT-29,SW480,SW620)and normal colon fibroblasts(CCD18-Co).Uro-A inhibited CRC cell proliferation,clonogenic growth,cancer stem cells properties,migration,and invasion,and induced cell cycle arrest,apoptosis,autophagy,and senescence,through modulation of key signaling pathways and proteins.Co-treatments with conventional chemotherapeutics and microbiota-derived metabolites showed additive or synergistic effects.Discussion:The findings support UroA’s potential as a preventive or adjuvant agent in CRC treatment.However,preclinical nature of the evidence and methodological heterogeneity hinder clinical extrapolation to in vivo contexts.Human clinical trials are necessary to overcome these limitations.Other:This review was registered in PROSPERO(CRD420251070874)and supported by FCT/MCTES UIDP/05608/2020 and UIDB/05608/2020.Institutional.展开更多
The renowned scientist is academician of the Chinese Academy of Sciences,former president of Tsinghua University,and chair of the Tengchong Scientists Forum.ACADEMICIAN of the Chinese Academy of Sciences,former presid...The renowned scientist is academician of the Chinese Academy of Sciences,former president of Tsinghua University,and chair of the Tengchong Scientists Forum.ACADEMICIAN of the Chinese Academy of Sciences,former president of Tsinghua University,and chair of the Tengchong Scientists Forum,Gu Binglin is one of the world’s top physicists and materials scientist,and a pioneer in the field of materials design.展开更多
Organic nanophotocatalysts are promising candidates for solar fuels production,but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths.Here,we introduce a b...Organic nanophotocatalysts are promising candidates for solar fuels production,but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths.Here,we introduce a binary nanophotocatalyst fabricated by blending two polymers,PS-PEG5(PS)and PBT-PEG5(PBT),with matched absorption and emission spectra,enabling a Forster resonance energy transfer(FRET)process for enhanced photocatalysis.These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation(FNP)technique with precious kinetic control over binary nanoparticle formation.The resulting nanoparticles exhibit an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g^(-1) h^(-1),2.5 times higher than that single component nanoparticles.Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles,which prolongs the excited-state lifetime and extends the namely“effective exciton diffusion length”.Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.展开更多
文摘For decades,Xu has been committed to fulfilling the duty and mission of a scientist and educator—diving into the laws of nature,caring deeply for the nation,and earnestly cultivating younger generations.
文摘From cracking the code of viruses to mentoring the next generation of scientists,the former president of Nankai University has contributed a lot to turning microscopic discoveries into monumental shields for global health.OVER the past 40 years,one man has distinguished himself through a deep commitment to researching protein structures of high pathogenic viruses,and published numerous significant works in top international scientific journals.
基金supported by the National Natural Science Foundation of China(22025503,22220102004,22401093)the Science and Technology Commission of Shanghai Municipality(24DX1400200)+2 种基金the Innovation Program of Shanghai Municipal Education Commission(2023ZKZD40)the Programme of Introducing Talents of Discipline to Universities(B16017)the China Postdoctoral Science Foundation(2023M741167,GZB20230211,2024T170273)。
文摘While biomaterials are endowed with sophisticated functions by the temporal dynamics and autonomy derived from non-equilibrium assemblies in biological systems,fabricating advanced materials counterparts with these features through kinetic control remains rare.Herein,we report a non-equilibrium hydrogel that exhibits autonomous time-dependent ultrabright fluorescence(quantum yield 0.90),achieved through the kinetically controlled incorporation of thermodynamic equilibrium host-vip complexes into a poly(2-hydroxyethyl methacrylate)(PHEMA)network.Transient complexes are programmed by coupling rapid assembly kinetics with the slow competitive binding of the polymer matrix.This kinetic mismatch converts a thermodynamic equilibrium supramolecular system into a non-equilibrium state,generating temporally dynamic fluorescence that cyclically shifts from yellow to green and self-reverts.The programmed temporal dynamics endow the hydrogel with high potential for information encryption applications.
基金supported by the National Natural Science Foundation of China (Nos.22208218,22078196,and 22278268)the Natural Science Foundation of Shanghai (No.22ZR1460400)Collaborative Innovation Center of Fragrance Flavour and Cosmetics,and Collaborative Innovation Project of Shanghai Institute of Technology (No.XTCX2023-07)。
文摘The diagnostic efficacy of contemporary bioimaging technologies remains constrained by inherent limitations of conventional imaging agents,including suboptimal sensitivity,off-target biodistribution,and inherent cytotoxicity.These limitations have catalyzed the development of intelligent stimuli-responsive block copolymers-based bioimaging agents,which was engineered to dynamically respond to endogenous biochemical cues(e.g.,p H gradients,redox potential,enzyme activity,hypoxia environment) or exogenous physical triggers(e.g.,photoirradiation,thermal gradients,ultrasound(US)/magnetic stimuli).Through spatiotemporally controlled structural transformations,stimuli-responsive block copolymers enable precise contrast targeting,activatable signal amplification,and theranostic integration,thereby substantially enhancing signal-to-noise ratios of bioimaging and diagnostic specificity.Hence,this mini-review systematically examines molecular engineering principles for designing p H-,redox-,enzyme-,light-,thermo-,and US/magnetic-responsive polymers,with emphasis on structure-property relationships governing imaging performance modulation.Furthermore,we critically analyze emerging strategies for optical imaging,US synergies,and magnetic resonance imaging(MRI).Multimodal bioimaging has also been elaborated,which could overcome the inherent trade-offs between resolution,penetration depth,and functional specificity in single-modal approaches.By elucidating mechanistic insights and translational challenges,this mini-review aims to establish a design framework of stimuli-responsive block copolymersbased for high fidelity bioimaging agents and accelerate their clinical translation in precise diagnosis and therapy.
基金supported by the National Natural Science Foundation of China(No.22375063)Science and Technology Commission of Shanghai Municipality(No.23JC140170O)the Fundamental Research Funds for the Central Universities.
文摘Developing advanced polymeric materials with enhanced mechanical properties and functionalities has been a long-standing goal in materials science.Recently,supramolecular polymeric materials(SPMs)have drawn increased attention due to their unique properties and potential applications in self-healing,shape memory,sensors,and flexible electronics.Here,we develop an ionic cluster-optimized microphase separation strategy to enhance the toughening and energy dissipation capabilities of polydisulfide-based supramolecular polymers.The mechanical properties,including Young's modulus and toughness,are significantly improved by integrating the quadruple H-bonding 2-ureido-4-pyrimidone(UPy)induced microphase separation with iron(III)-to-carboxylate ionic clusters.By combining established chemical approaches with adjustable polymer phase ratios,it is revealed that the synergistic effect of these factors expands the interchain spacing,facilitates the formation of microphase domains,and enhances the tolerance of polythioctic acid-based polymers to external mechanical and thermal stimuli,meeting the practical requirements for industrial plastic applications.Moreover,the UPy-functionalized polymers incorporating iron carboxylate clusters exhibit good one-way shape memory behavior with practical applicability at a relatively low recovery temperature.Our work demonstrates a novel strategy for constructing industrially viable shape memory dynamic SPMs and paves the way for future innovations in developing SPMs.
基金the Young Elite Scientists Sponsorship Program by JXAST(2024QT11)the National Natural Science Foundation of China(22465001,22309003)the Jiangxi Provincial Natural Science Foundation(20232BAB203042,20242BAB22002).
文摘As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.
基金supported by the National Natural Science Foundation of China(22176058)the Science and Technology Commission of Shanghai Municipality(24DX1400200,23ZR1416100,25ZR1401082)+1 种基金the Program of Introducing Talents of Discipline to Universities(B16017)the Fundamental Research Funds for the Central Universities(222201717003)。
文摘Controllable photoreaction transition of photosensitizers(PSs)provides a highly promising approach for achieving efficient photodynamic therapy(PDT).However,tumor microenvironment-triggered phototransition remains a significant challenge and has not yet been reported.In this work,we develop a hydrogen bond self-assembly(HBSA)strategy that is triggered by the acidic tumor microenvironment to enable the photodynamic transition of tetra(4-carboxylphenyl)porphyrin(TCPP)PSs from type Ⅱ to type Ⅰ reactions.Upon self-assembly of TCPP monomers into TCPP assemblies(TCPP-ass),the generated reactive oxygen species shift from singlet oxygen to superoxide anions,which induces caspase-3/GSDME-mediated programmed pyroptosis,enabling rapid and complete solid tumor elimination with minimized adverse effects and enhanced therapeutic efficacy.Crucially,the HBSA process occurs exclusively within tumor cells,and this tumor-specific self-assembly strategy not only utilizes high tissue penetration of TCPP molecular-PSs,but also avoids phototoxicity caused by the formation and accumulation of TCPP-ass nano-PSs in normal tissue,providing an innovative approach for precise cancer therapy.
基金supported by FCT/MCTES UIDP/05608/2020(https://doi.org/10.54499/UIDP/05608/2020,accessed on 01 July 2025)UIDB/05608/2020(https://doi.org/10.54499/UIDB/05608/2020,accessed on 01 July 2025).Institutional.
文摘Objectives:Colorectal cancer(CRC)is a major global health burden,and Urolithin A(Uro-A)has emerged as a promising anticancer agent.This systematic review aims to synthesize current in vitro evidence on the anticancer effects of Uro-A in CRC,highlighting effective concentration ranges,exposure times,relevant outcomes,and underlying molecular mechanisms.Methods:Following PRISMA 2020 guidelines,a systematic search was conducted in PubMed,Scopus,and Web of Science using the following strategy:(colorectal cancer)AND(urolithin a)OR(3,8-dihydroxy-6H-dibenzo(b,d)pyran-6-one).Eligibility criteria were defined by the PICO framework:(P)in vitro CRC cell models;(I)Uro-A alone or combined treatments;(C)No intervention,vehicle or other treatments;(O)Relevant anticancer outcomes of Uro-A in CRC.Only original,full-text,in vitro studies in English were included.Risk of bias was assessed using ToxRTool.A qualitative synthesis was performed due to the heterogeneity of the included studies.Results:Fifteen studies met inclusion criteria,involving CRC cell lines(Caco-2,HCT-116,HT-29,SW480,SW620)and normal colon fibroblasts(CCD18-Co).Uro-A inhibited CRC cell proliferation,clonogenic growth,cancer stem cells properties,migration,and invasion,and induced cell cycle arrest,apoptosis,autophagy,and senescence,through modulation of key signaling pathways and proteins.Co-treatments with conventional chemotherapeutics and microbiota-derived metabolites showed additive or synergistic effects.Discussion:The findings support UroA’s potential as a preventive or adjuvant agent in CRC treatment.However,preclinical nature of the evidence and methodological heterogeneity hinder clinical extrapolation to in vivo contexts.Human clinical trials are necessary to overcome these limitations.Other:This review was registered in PROSPERO(CRD420251070874)and supported by FCT/MCTES UIDP/05608/2020 and UIDB/05608/2020.Institutional.
文摘The renowned scientist is academician of the Chinese Academy of Sciences,former president of Tsinghua University,and chair of the Tengchong Scientists Forum.ACADEMICIAN of the Chinese Academy of Sciences,former president of Tsinghua University,and chair of the Tengchong Scientists Forum,Gu Binglin is one of the world’s top physicists and materials scientist,and a pioneer in the field of materials design.
基金supported by National Natural Science Foundation of China(NSFC,22338006,92356301,9235630033 and 22375062)Shanghai Municipal Science and Technology Major Project(21JC1401700)+4 种基金Shanghai Pilot Program for Basic Research(22TQ1400100-10)Fundamental Research Funds for the Central UniversitiesShanghai Pujiang Program(22PJ1402400)“Chenguang Program”supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(22CGA32)the Young Elite Scientists Sponsorship Program by CAST(2023QNRC001).
文摘Organic nanophotocatalysts are promising candidates for solar fuels production,but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths.Here,we introduce a binary nanophotocatalyst fabricated by blending two polymers,PS-PEG5(PS)and PBT-PEG5(PBT),with matched absorption and emission spectra,enabling a Forster resonance energy transfer(FRET)process for enhanced photocatalysis.These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation(FNP)technique with precious kinetic control over binary nanoparticle formation.The resulting nanoparticles exhibit an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g^(-1) h^(-1),2.5 times higher than that single component nanoparticles.Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles,which prolongs the excited-state lifetime and extends the namely“effective exciton diffusion length”.Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.
