Bone regeneration for non-load-bearing defects remains a significant clinical challenge requiring advanced biomaterials and cellular strategies.Adiposederived mesenchymal stem cells(AD-MSCs)have garnered significant i...Bone regeneration for non-load-bearing defects remains a significant clinical challenge requiring advanced biomaterials and cellular strategies.Adiposederived mesenchymal stem cells(AD-MSCs)have garnered significant interest in bone tissue engineering(BTE)because of their abundant availability,minimally invasive harvesting procedures,and robust differentiation potential into osteogenic lineages.Unlike bone marrow-derived mesenchymal stem cells,AD-MSCs can be easily obtained in large quantities,making them appealing alternatives for therapeutic applications.This review explores hydrogels containing polymers,such as chitosan,collagen,gelatin,and hyaluronic acid,and their composites,tailored for BTE,and emphasizes the importance of these hydrogels as scaffolds for the delivery of AD-MSCs.Various hydrogel fabrication techniques and biocompatibility assessments are discussed,along with innovative modifications to enhance osteogenesis.This review also briefly outlines AD-MSC isolation methods and advanced embedding techniques for precise cell placement,such as direct encapsulation and three-dimensional bioprinting.We discuss the mechanisms of bone regeneration in the AD-MSC-laden hydrogels,including osteoinduction,vascularization,and extracellular matrix remodeling.We also review the preclinical and clinical applications of AD-MSC-hydrogel systems,emphasizing their success and limitations.In this review,we provide a comprehensive overview of AD-MSC-based hydrogel systems to guide the development of effective therapies for bone regeneration.展开更多
Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electro...Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electrocatalytic oxidations of saturated alcohols(C_(1)-C_(6))to selectively form formate using Ni Co hydroxide(Ni Co-OH)derived Ni Co_(2)O_(4)solid-acid electrocatalysts with balanced Lewis acid(LASs)and Brønsted acid sites(BASs).Thermal treatment transforms BASs-rich(89.6%)Ni Co-OH into Ni Co_(2)O_(4)with nearly equal distribution of LASs(53.1%)and BASs(46.9%)which synergistically promote adsorption and activation of OH-and alcohol molecules for enhanced oxidation activity.In contrast,BASs-enriched Ni Co-OH facilitates formation of higher valence metal sites,beneficial for water oxidation.The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6alcohols increases as increased number of hydroxyl groups and decreased HOMO-LUMO gaps:methanol(C_(1))<ethylene glycol(C_(2))<glycerol(C3)<meso-erythritol(C4)<xylitol(C5)<sorbitol(C6),while the formate selectivity shows the opposite trend from 100 to 80%.This study unveils synergistic roles of LASs and BASs,as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.展开更多
Octopuses,due to their flexible arms,marvelous adaptability,and powerful suckers,are able to effortlessly grasp and disengage various objects in the marine surrounding without causing devastation.However,manipulating ...Octopuses,due to their flexible arms,marvelous adaptability,and powerful suckers,are able to effortlessly grasp and disengage various objects in the marine surrounding without causing devastation.However,manipulating delicate objects such as soft and fragile foods underwater require gentle contact and stable adhesion,which poses a serious challenge to now available soft grippers.Inspired by the sucker infundibulum structure and flexible tentacles of octopus,herein we developed a hydraulically actuated hydrogel soft gripper with adaptive maneuverability by coupling multiple hydrogen bond-mediated supramolecular hydrogels and vat polymerization three-dimensional printing,in which hydrogel bionic sucker is composed of a tunable curvature membrane,a negative pressure cavity,and a pneumatic chamber.The design of the sucker structure with the alterable curvature membrane is conducive to realize the reliable and gentle switchable adhesion of the hydrogel soft gripper.As a proof-of-concept,the adaptive hydrogel soft gripper is capable of implement diversified underwater tasks,including gingerly grasping fragile foods like egg yolks and tofu,as well as underwater robots and vehicles that station-keeping and crawling based on switchable adhesion.This study therefore provides a transformative strategy for the design of novel soft grippers that will render promising utilities for underwater exploration soft robotics.展开更多
Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via lo...Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.展开更多
Aerogels are ultra-lightweight,porous materials defined by a complex network of interconnected pores and nanostructures,which effectively suppress heat transfer,making them exceptional for thermal insulation.Furthermo...Aerogels are ultra-lightweight,porous materials defined by a complex network of interconnected pores and nanostructures,which effectively suppress heat transfer,making them exceptional for thermal insulation.Furthermore,their porous architecture can trap and scatter light via multiple internal reflections,extending the optical path within the material.When combined with suitable light-absorbing materials,this feature significantly enhances light absorption(darkness).To validate this concept,mesoporous silica aerogel particles were incorporated into a resorcinol-formaldehyde(RF)sol,and the silica-to-RF ratio was optimized to achieve uniform carbon compound coatings on the silica pore walls.Notably,increasing silica loading raised the sol viscosity,enabling formulations ideal for direct ink writing processes with excellent shape fidelity for super-black topographical designs.The printed silica-RF green bodies exhibited remarkable mechanical strength and ultra-low thermal conductivity(15.8 m W m^(-1) K^(-1))prior to pyrolysis.Following pyrolysis,the composites maintained structural integrity and printed microcellular geometries while achieving super-black coloration(abs.99.56%in the 280-2500 nm range)and high photothermal conversion efficiency(94.2%).Additionally,these silica-carbon aerogel microcellulars demonstrated stable electrical conductivity and low electrochemical impedance.The synergistic combination of 3D printability and super-black photothermal features makes these composites highly versatile for multifunctional applications,including on-demand thermal management,and efficient solar-driven water production.展开更多
Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(...Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.展开更多
By combining the merits of radiative cooling(RC)and evaporation cooling(EC),radiative coupled evaporative cooling(REC)has attracted considerable attention for sub-ambient cooling purposes.However,for outdoor devices,t...By combining the merits of radiative cooling(RC)and evaporation cooling(EC),radiative coupled evaporative cooling(REC)has attracted considerable attention for sub-ambient cooling purposes.However,for outdoor devices,the interior heating power would increase the working temperature and fire risk,which would suppress their above-ambient heat dissipation capabilities and passive water cycle properties.In this work,we introduced a REC design based on an all-in-one photonic hydrogel for above-ambient heat dissipation and flame retardancy.Unlike conventional design RC film for heat dissipation with limited cooling power and fire risk,REC hydrogel can greatly improve the heat dissipation performance in the daytime with a high workload,indicating a 12.0℃lower temperature than the RC film under the same conditions in the outdoor experiment.In the nighttime with a low workload,RC-assisted adsorption can improve atmospheric water harvesting to ensure EC in the daytime.In addition,our REC hydrogel significantly enhanced flame retardancy by absorbing heat without a corresponding temperature rise,thus mitigating fire risks.Thus,our design shows a promising solution for the thermal management of outdoor devices,delivering outstanding performance in both heat dissipation and flame retardancy.展开更多
文摘Bone regeneration for non-load-bearing defects remains a significant clinical challenge requiring advanced biomaterials and cellular strategies.Adiposederived mesenchymal stem cells(AD-MSCs)have garnered significant interest in bone tissue engineering(BTE)because of their abundant availability,minimally invasive harvesting procedures,and robust differentiation potential into osteogenic lineages.Unlike bone marrow-derived mesenchymal stem cells,AD-MSCs can be easily obtained in large quantities,making them appealing alternatives for therapeutic applications.This review explores hydrogels containing polymers,such as chitosan,collagen,gelatin,and hyaluronic acid,and their composites,tailored for BTE,and emphasizes the importance of these hydrogels as scaffolds for the delivery of AD-MSCs.Various hydrogel fabrication techniques and biocompatibility assessments are discussed,along with innovative modifications to enhance osteogenesis.This review also briefly outlines AD-MSC isolation methods and advanced embedding techniques for precise cell placement,such as direct encapsulation and three-dimensional bioprinting.We discuss the mechanisms of bone regeneration in the AD-MSC-laden hydrogels,including osteoinduction,vascularization,and extracellular matrix remodeling.We also review the preclinical and clinical applications of AD-MSC-hydrogel systems,emphasizing their success and limitations.In this review,we provide a comprehensive overview of AD-MSC-based hydrogel systems to guide the development of effective therapies for bone regeneration.
基金the financial support from the National Natural Science Foundation of China(52172110,52472231,52311530113)Shanghai"Science and Technology Innovation Action Plan"intergovernmental international science and technology cooperation project(23520710600)+1 种基金Science and Technology Commission of Shanghai Municipality(22DZ1205600)the Central Guidance on Science and Technology Development Fund of Zhejiang Province(2024ZY01011)。
文摘Investigating structural and hydroxyl group effects in electrooxidation of alcohols to value-added products by solid-acid electrocatalysts is essential for upgrading biomass alcohols.Herein,we report efficient electrocatalytic oxidations of saturated alcohols(C_(1)-C_(6))to selectively form formate using Ni Co hydroxide(Ni Co-OH)derived Ni Co_(2)O_(4)solid-acid electrocatalysts with balanced Lewis acid(LASs)and Brønsted acid sites(BASs).Thermal treatment transforms BASs-rich(89.6%)Ni Co-OH into Ni Co_(2)O_(4)with nearly equal distribution of LASs(53.1%)and BASs(46.9%)which synergistically promote adsorption and activation of OH-and alcohol molecules for enhanced oxidation activity.In contrast,BASs-enriched Ni Co-OH facilitates formation of higher valence metal sites,beneficial for water oxidation.The combined experimental studies and theoretical calculation imply the oxidation ability of C1-C6alcohols increases as increased number of hydroxyl groups and decreased HOMO-LUMO gaps:methanol(C_(1))<ethylene glycol(C_(2))<glycerol(C3)<meso-erythritol(C4)<xylitol(C5)<sorbitol(C6),while the formate selectivity shows the opposite trend from 100 to 80%.This study unveils synergistic roles of LASs and BASs,as well as hydroxyl group effect in electro-upgrading of alcohols using solid-acid electrocatalysts.
基金the financial support from the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0470303)the National Key Research and Development Program of China (2022YFB4600101)+5 种基金the National Natural Science Foundation of China (52175201)the Research Program of Science and Technology Department of Gansu Province (24JRRA059, 24JRRA044, and 24YFFA014)the Science Fund of Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai (AMGM2024F12)the Major Program (ZYFZFX-2) of the Lanzhou Institute of Chemical Physics, CASthe Special Research Assistant Project of the Chinese Academy of Sciencesthe Oasis Scholar of Shihezi University
文摘Octopuses,due to their flexible arms,marvelous adaptability,and powerful suckers,are able to effortlessly grasp and disengage various objects in the marine surrounding without causing devastation.However,manipulating delicate objects such as soft and fragile foods underwater require gentle contact and stable adhesion,which poses a serious challenge to now available soft grippers.Inspired by the sucker infundibulum structure and flexible tentacles of octopus,herein we developed a hydraulically actuated hydrogel soft gripper with adaptive maneuverability by coupling multiple hydrogen bond-mediated supramolecular hydrogels and vat polymerization three-dimensional printing,in which hydrogel bionic sucker is composed of a tunable curvature membrane,a negative pressure cavity,and a pneumatic chamber.The design of the sucker structure with the alterable curvature membrane is conducive to realize the reliable and gentle switchable adhesion of the hydrogel soft gripper.As a proof-of-concept,the adaptive hydrogel soft gripper is capable of implement diversified underwater tasks,including gingerly grasping fragile foods like egg yolks and tofu,as well as underwater robots and vehicles that station-keeping and crawling based on switchable adhesion.This study therefore provides a transformative strategy for the design of novel soft grippers that will render promising utilities for underwater exploration soft robotics.
基金the National Nature Science Foundation of China for Excellent Young Scientists Fund(32222058)Fundamental Research Foundation of CAF(CAFYBB2022QB001).
文摘Developing biomass platform compounds into high value-added chemicals is a key step in renewable resource utilization.Herein,we report porous carbon-supported Ni-ZnO nanoparticles catalyst(Ni-ZnO/AC)synthesized via low-temperature coprecipitation,exhibiting excellent performance for the selective hydrogenation of 5-hydroxymethylfurfural(HMF).A linear correlation is first observed between solvent polarity(E_(T)(30))and product selectivity within both polar aprotic and protic solvent classes,suggesting that solvent properties play a vital role in directing reaction pathways.Among these,1,4-dioxane(aprotic)favors the formation of 2,5-bis(hydroxymethyl)furan(BHMF)with 97.5%selectivity,while isopropanol(iPrOH,protic)promotes 2,5-dimethylfuran production with up to 99.5%selectivity.Mechanistic investigations further reveal that beyond polarity,proton-donating ability is critical in facilitating hydrodeoxygenation.iPrOH enables a hydrogen shuttle mechanism where protons assist in hydroxyl group removal,lowering the activation barrier.In contrast,1,4-dioxane,lacking hydrogen bond donors,stabilizes BHMF and hinders further conversion.Density functional theory calculations confirm a lower activation energy in iPrOH(0.60 eV)compared to 1,4-dioxane(1.07 eV).This work offers mechanistic insights and a practical strategy for solvent-mediated control of product selectivity in biomass hydrogenation,highlighting the decisive role of solvent-catalyst-substrate interactions.
基金financially supported by the Swiss National Science Foundation(grant number IZLRZ2_164058)the China Scholarship Council Ph.D.student exchange programthe Priority Academic Program Development of Jiangsu Higher Education Institution(PAPD)。
文摘Aerogels are ultra-lightweight,porous materials defined by a complex network of interconnected pores and nanostructures,which effectively suppress heat transfer,making them exceptional for thermal insulation.Furthermore,their porous architecture can trap and scatter light via multiple internal reflections,extending the optical path within the material.When combined with suitable light-absorbing materials,this feature significantly enhances light absorption(darkness).To validate this concept,mesoporous silica aerogel particles were incorporated into a resorcinol-formaldehyde(RF)sol,and the silica-to-RF ratio was optimized to achieve uniform carbon compound coatings on the silica pore walls.Notably,increasing silica loading raised the sol viscosity,enabling formulations ideal for direct ink writing processes with excellent shape fidelity for super-black topographical designs.The printed silica-RF green bodies exhibited remarkable mechanical strength and ultra-low thermal conductivity(15.8 m W m^(-1) K^(-1))prior to pyrolysis.Following pyrolysis,the composites maintained structural integrity and printed microcellular geometries while achieving super-black coloration(abs.99.56%in the 280-2500 nm range)and high photothermal conversion efficiency(94.2%).Additionally,these silica-carbon aerogel microcellulars demonstrated stable electrical conductivity and low electrochemical impedance.The synergistic combination of 3D printability and super-black photothermal features makes these composites highly versatile for multifunctional applications,including on-demand thermal management,and efficient solar-driven water production.
基金financially supported by National Natural Science Foundation of China(22466010)Guizhou Provincial Basic Research Program(Natural Science)ZK[2023]47 and key program ZD[2025]075+6 种基金Innovation and Entrepreneurship Project for overseas Talents in Guizhou Province[2022]02Specific Natural Science Foundation of Guizhou University(X202207)the national undergraduate innovation and entrepreneurship training program(gzugc2023006gzusc2024012)SRT project of Guizhou university(2023SRT0292023SRT024)supported by Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.
基金financially supported by the Science and Technology Innovation Program of Hunan Province(2024RC3003)the Central South University Innovation-Driven Research Programme(2023CXQD012)the Initiative for Sustainable Energy for its financial support。
文摘By combining the merits of radiative cooling(RC)and evaporation cooling(EC),radiative coupled evaporative cooling(REC)has attracted considerable attention for sub-ambient cooling purposes.However,for outdoor devices,the interior heating power would increase the working temperature and fire risk,which would suppress their above-ambient heat dissipation capabilities and passive water cycle properties.In this work,we introduced a REC design based on an all-in-one photonic hydrogel for above-ambient heat dissipation and flame retardancy.Unlike conventional design RC film for heat dissipation with limited cooling power and fire risk,REC hydrogel can greatly improve the heat dissipation performance in the daytime with a high workload,indicating a 12.0℃lower temperature than the RC film under the same conditions in the outdoor experiment.In the nighttime with a low workload,RC-assisted adsorption can improve atmospheric water harvesting to ensure EC in the daytime.In addition,our REC hydrogel significantly enhanced flame retardancy by absorbing heat without a corresponding temperature rise,thus mitigating fire risks.Thus,our design shows a promising solution for the thermal management of outdoor devices,delivering outstanding performance in both heat dissipation and flame retardancy.
