Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability cau...Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.展开更多
Blood vessels are essential for nutrient and oxygen delivery and waste removal.Scaffold-repairing materials with functional vascular networks are widely used in bone tissue engineering.Additive manufacturing is a manu...Blood vessels are essential for nutrient and oxygen delivery and waste removal.Scaffold-repairing materials with functional vascular networks are widely used in bone tissue engineering.Additive manufacturing is a manufacturing technology that creates three-dimensional solids by stacking substances layer by layer,mainly including but not limited to 3D printing,but also 4D printing,5D printing and 6D printing.It can be effectively combined with vascularization to meet the needs of vascularized tissue scaffolds by precisely tuning the mechanical structure and biological properties of smart vascular scaffolds.Herein,the development of neovascularization to vascularization to bone tissue engineering is systematically discussed in terms of the importance of vascularization to the tissue.Additionally,the research progress and future prospects of vascularized 3D printed scaffold materials are highlighted and presented in four categories:functional vascularized 3D printed scaffolds,cell-based vascularized 3D printed scaffolds,vascularized 3D printed scaffolds loaded with specific carriers and bionic vascularized 3D printed scaffolds.Finally,a brief review of vascularized additive manufacturing-tissue scaffolds in related tissues such as the vascular tissue engineering,cardiovascular system,skeletal muscle,soft tissue and a discussion of the challenges and development efforts leading to significant advances in intelligent vascularized tissue regeneration is presented.展开更多
It is known that α-RuCl_(3) has been studied extensively because of its proximity to the Kitaev quantum-spin-liquid(QSL)phase and the possibility of approaching it by tuning the competing interactions.Here we present...It is known that α-RuCl_(3) has been studied extensively because of its proximity to the Kitaev quantum-spin-liquid(QSL)phase and the possibility of approaching it by tuning the competing interactions.Here we present the first polarized inelastic neutron scattering study on α-RuCl_(3) single crystals to explore the scattering continuum around the Γ point at the Brillouin zone center,which was hypothesized to be resulting from the Kitaev QSL state but without concrete evidence.With polarization analyses,we find that,while the spin-wave excitations around the Γ point vanish above the transition temperature T_(N),the pure magnetic continuous excitations around the Γ point are robust against temperature.Furthermore,by calculating the dynamical spin-spin correlation function using the cluster perturbation theory,we derive magnetic dispersion spectra based on the K-Γ model,which involves with a ferromagnetic Kitaev interaction of −7.2 meV and an off-diagonal interaction of 5.6 meV.We find this model can reproduce not only the spin-wave excitation spectra around the Γ point,but also the non-spin-wave continuous magnetic excitations around the Γ point.These results provide evidence for the existence of fractional excitations around the Γ point originating from the Kitaev QSL state,and further support the validity of the K-Γ model as the effective minimal spin model to describe α-RuCl_(3).展开更多
Quantum spin liquids(QSLs) represent a novel state of matter in which quantum fluctuations prevent the conventional magnetic order from being established, and the spins remain disordered even at zero temperature. Th...Quantum spin liquids(QSLs) represent a novel state of matter in which quantum fluctuations prevent the conventional magnetic order from being established, and the spins remain disordered even at zero temperature. There have been many theoretical developments proposing various QSL states. On the other hand, experimental movement was relatively slow largely due to limitations on the candidate materials and difficulties in the measurements. In recent years, the experimental progress has been accelerated. In this topical review, we give a brief summary of experiments on the QSL candidates under magnetic fields. We arrange our discussions by two categories: i) Geometrically-frustrated systems, including triangularlattice compounds YbMgGaO4 and YbZnGaO4, κ-(BEDT-TTF)2 Cu2(CN)3, and EtMe3 Sb[Pd(dmit)2]2, and the kagom′e system ZnCu3(OH)6 Cl2; ii) the Kitaev material α-RuCl3. Among these, we will pay special attention to α-RuCl3, which has been intensively studied by ours and other groups recently. We will present evidence that both supports and rejects the QSL ground state for these materials, based on which we give several perspectives to stimulate further research activities.展开更多
Regulating macrophage activation precisely is crucial in treating chronic inflammation in osteoarthritis(OA).However,the stable pro-inflammatory state and deep distribution of macrophages in vivo pose a great challeng...Regulating macrophage activation precisely is crucial in treating chronic inflammation in osteoarthritis(OA).However,the stable pro-inflammatory state and deep distribution of macrophages in vivo pose a great challenge to treatment.In this study,inspired by the innate immune,immune cell mobilized hydrogel microspheres were constructed by microfluidic methods and load chemokines,macrophage antibodies and engineered cell membrane vesicles(sEVs)via covalent and non-covalent junctions.The immune cell mobilized hydrogel microspheres,based on a mixture of streptavidin grafted hyaluronic acid methacrylate(HAMA-SA)and Chondroitin sulfate methacrylate(ChSMA)microspheres(HCM),can recruit,capture and reprogram proinflammatory macrophages in the joint cavity to improve the joint inflammatory microenvironment.In vitro experiments demonstrated that immune cell mobilized hydrogel microspheres had excellent macrophage recruitment,capture,and reprogramming abilities.Pro-inflammatory macrophages can be transformed into anti-inflammatory macrophages with an efficiency of 88.5%.Animal experiments also revealed significant reduction in synovial inflammation and cartilage matrix degradation of OA.Therefore,the immune cell mobilized hydrogel microspheres may be an effective treatment of OA inflammation for the future.展开更多
Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related issues.The electrocatalytic reduction of NO_(3)^(-)holds promise as a s...Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related issues.The electrocatalytic reduction of NO_(3)^(-)holds promise as a sustainable approach to both eliminating NO_(3)^(-)and generating valuable ammonia(NH_(3)).Nevertheless,the reduction reaction of NO_(3)^(-)(NO_(3)^(-)RR),involving 8-electron transfer process,is intricate,necessitating highly efficient electrocatalysts to facilitate the conversion of NO_(3)^(-)to NH_(3).In this study,Fe-doped Co_(3)O_(4) nanowire strutted three-dimensional(3D)pinewood-derived carbon(Fe-Co_(3)O_(4)/PC)is proposed as a high-efficiency NO_(3)^(-)RR electrocatalyst for NH_(3) production.Operating within 0.1 M NaOH containing NO_(3)^(-),Fe-Co_(3)O_(4)/PC demonstrates exceptional performance,obtain an impressively large NH_(3) yield of 0.55 mmol·h^(-1)·cm^(-2) and an exceptionally high Faradaic efficiency of 96.5%at-0.5 V,superior to its Co_(3)O_(4)/PC counterpart(0.2 mmol·h^(-1)·cm^(-2),73.3%).Furthermore,the study delves into the reaction mechanism of Fe-Co_(3)O_(4) for NO_(3)^(-)RR through theoretical calculations.展开更多
Subcellular mitochondria serve as sensors for energy metabolism and redox balance, and the dynamic regulation of functional and dysfunctional mitochondria plays a crucial role in determining cells' fate. Selective...Subcellular mitochondria serve as sensors for energy metabolism and redox balance, and the dynamic regulation of functional and dysfunctional mitochondria plays a crucial role in determining cells' fate. Selective removal of dysfunctional mitochondria at the subcellular level can provide chondrocytes with energy to prevent degeneration, thereby treating osteoarthritis. Herein, to achieve an ideal subcellular therapy, cartilage affinity peptide (WYRGRL)-decorated liposomes loaded with mitophagy activator (urolithin A) were integrated into hyaluronic acid methacrylate hydrogel microspheres through microfluidic technology, named HM@WY-Lip/UA, that could efficiently target chondrocytes and selectively remove subcellular dysfunctional mitochondria. As a result, this system demonstrated an advantage in mitochondria function restoration, reactive oxygen species scavenging, cell survival rescue, and chondrocyte homeostasis maintenance through increasing mitophagy. In a rat post-traumatic osteoarthritis model, the intra-articular injection of HM@WY-Lip/UA ameliorated cartilage matrix degradation, osteophyte formation, and subchondral bone sclerosis at 8 weeks. Overall, this study indicated that HM@WY-Lip/UA provided a protective effect on cartilage degeneration in an efficacious and clinically relevant manner, and a mitochondrial-oriented strategy has great potential in the subcellular therapy of osteoarthritis.展开更多
Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited a...Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.展开更多
Irregular bone defects,characterized by unpredictable size,shape,and depth,pose a major challenge to clinical treatment.Although various bone grafts are available,none can fully meet the repair needs of the defective ...Irregular bone defects,characterized by unpredictable size,shape,and depth,pose a major challenge to clinical treatment.Although various bone grafts are available,none can fully meet the repair needs of the defective area.Here,this study fabricates a dough-type hydrogel(DR-Net),in which the first dynamic network is generated by coordination between thiol groups and silver ions,thereby possessing kneadability to adapt to various irregular bone defects.The second rigid covalent network is formed through photocrosslinking,maintaining the osteogenic space under external forces and achieving a better match with the bone regeneration process.In vitro,an irregular alveolar bone defect is established in the fresh porcine mandible,and the dough-type hydrogel exhibits outstanding shape adaptability,perfectly matching the morphology of the bone defect.After photocuring,the storage modulus of the hydrogel increases 8.6 times,from 3.7 kPa(before irradiation)to 32 kPa(after irradiation).Furthermore,this hydrogel enables effective loading of P24 peptide,which potently accelerates bone repair in Sprague–Dawley(SD)rats with critical calvarial defects.Overall,the dough-type hydrogel with kneadability,space-maintaining capability,and osteogenic activity exhibits exceptional potential for clinical translation in treating irregular bone defects.展开更多
Local lactate accumulation greatly hinders tissue repair and regeneration under ischemic condition.Herein,an injectable microsphere(MS@MCL)for local lactate exhaustion was constructed by grafting manganese dioxide(MnO...Local lactate accumulation greatly hinders tissue repair and regeneration under ischemic condition.Herein,an injectable microsphere(MS@MCL)for local lactate exhaustion was constructed by grafting manganese dioxide(MnO_(2))-lactate oxidase(LOX)composite nanozyme on microfluidic hyaluronic acid methacrylate(HAMA)microspheres via chemical bonds,achieving a long-term oxygen-promoted lactate exhaustion effect and a long half-life in vivo.The uniform and porous microspheres synthesized by microfluidic technology is beneficial to in situ injection therapy and improving encapsulation efficiency.Furthermore,chemical grafting into HAMA microspheres through amide reactions promoted local enzymatic concentration and activity enhancement.It was showed that the MS@MCL eliminated oxidative and inflammatory stress and promoted extracellular matrix metabolism and cell survival when co-cultured with nucleus pulposus cells(NPCs)in vitro.In the rat degenerative intervertebral disc model caused by lactate injection,MS@MCL showed a long-term therapeutic effect in reducing intervertebral height narrowing and preventing extracellular matrix(ECM)degradation as well as inflammatory damage in vivo.Altogether,this study confirms that this nanozyme-functionalized injectable MS@MCL effectively improves the regenerative and reparative effect in ischemic tissues by disposing of enriched lactate in local microenvironment.展开更多
Lipid-based boundary layers formed on liposome-containing hydrogels can facilitate lubrication.However,these boundary layers can be damaged by shear,resulting in decreased lubrication.Here,a shear-responsive boundary-...Lipid-based boundary layers formed on liposome-containing hydrogels can facilitate lubrication.However,these boundary layers can be damaged by shear,resulting in decreased lubrication.Here,a shear-responsive boundary-lubricated drug-loaded hydrogel is created by incorporating celecoxib(CLX)-loaded liposomes within dynamic covalent bond-based hyaluronic acid(HA)hydrogels(CLX@Lipo@HA-gel).The dynamic cross-linked network enables the hydrogel to get restructured in response to shear,and the HA matrix allows the accumulation of internal liposome microreservoirs on the sliding surfaces,which results in the formation of boundary layers to provide stable lubrication.Moreover,hydration shells formed surrounding the hydrogel can retard the degradation process,thus helping in sustaining lubrication.Furthermore,in vitro and in vivo experiments found that CLX@Lipo@HA-gels can maintain anabolic-catabolic balance,alleviate cartilage wear,and attenuate osteoarthritis progression by delivering CLX and shear-responsive boundary lubrication.Overall,CLX@Lipo@HA-gels can serve as shear-responsive boundary lubricants and drug-delivery vehicles to alleviate friction-related diseases like osteoarthritis.展开更多
Soft tissue remodeling is a sophisticated process that sequentially provides dynamic biological signals to guide cell behavior.However,capturing these signals within hydrogel and directing over time has still been unr...Soft tissue remodeling is a sophisticated process that sequentially provides dynamic biological signals to guide cell behavior.However,capturing these signals within hydrogel and directing over time has still been unrealized owing to the poor comprehension of physiological processes.Here,a bio-mimicking hydrogel is designed via thiol-ene click reaction to capture the early physical signal triggered by inflammation,and the chemical signals provided with chemokine and natural adhesion sites,which guaranteed the precise soft tissue remodeling.This bio-mimicking hydrogel efficiently facilitated cell anchoring,migration,and invasion in the 3D matrix due to the permissive space and the interaction with integrin receptors.Besides,the covalently grafted chemokine-like peptide is optimal for colonization and functional differentiation of endothelial cells through a HIF-1αdependent signal pathway.Furthermore,the early polarization of macrophages,collagen deposition and angiogenesis in rat acute wound model,and the increased blood perfusion in mouse skin flap model have confirmed that the bio-mimicking hydrogel realized precise soft tissue remodeling and opens new avenues for the phased repair of different tissues such as nerve,myocardium,and even bone.展开更多
Since their discovery,Black Phosphorus(BP)-based nanomaterials have received extensive attentions in the fields of electromechanics,optics and biomedicine,due to their remarkable properties and excellent biocompatibil...Since their discovery,Black Phosphorus(BP)-based nanomaterials have received extensive attentions in the fields of electromechanics,optics and biomedicine,due to their remarkable properties and excellent biocompatibility.The most essential feature of BP is that it is composed of a single phosphorus element,which has a high degree of homology with the inorganic components of natural bone,therefore it has a full advantage in the treatment of bone defects.This review will first introduce the source,physicochemical properties,and degradation products of BP,then introduce the remodeling process of bone,and comprehensively summarize the progress of BP-based materials for bone therapy in the form of hydrogels,polymer membranes,microspheres,and three-dimensional(3D)printed scaffolds.Finally,we discuss the challenges and prospects of BP-based implant materials in bone immune regulation and outlook the future clinical application.展开更多
Dirac nodal-line semimetals with the linear bands crossing along a line or loop, represent a new topological state of matter. Here, by carrying out magnetotransport measurements and performing first-principle calculat...Dirac nodal-line semimetals with the linear bands crossing along a line or loop, represent a new topological state of matter. Here, by carrying out magnetotransport measurements and performing first-principle calculations, we demonstrate that such a state has been realized in high-quality single crystals of SrAs_3.We obtain the nontrivial ∏ Berry phase by analysing the Shubnikov-de Haas quantum oscillations. We also observe a robust negative longitudinal magnetoresistance induced by the chiral anomaly.Accompanying first-principles calculations identifies that a single hole pocket enclosing the loop nodes is responsible for these observations.展开更多
The electrocatalytic reduction of nitrate(NO_(3)^(-))not only facilitates the environmentally sustainable production of ammonia(NH_(3))but also purifies water by removing NO_(3)^(-),thereby transforming waste into val...The electrocatalytic reduction of nitrate(NO_(3)^(-))not only facilitates the environmentally sustainable production of ammonia(NH_(3))but also purifies water by removing NO_(3)^(-),thereby transforming waste into valuable resources.The process of converting NO_(3)^(-)to NH_(3)is complex,involving eight electron transfers and multiple intermediates,making the choice of electrocatalyst critical.In this study,we report a cobalt selenide(Co Se_(2))nanowire array on carbon cloth(CoSe_(2)/CC)as an effective electrocatalyst for the NO_(3)^(-)to NH_(3)conversion.In an alkaline medium with 0.1 mol/L NO_(3)^(-),CoSe_(2)/CC demonstrates exceptional NH_(3)Faradaic efficiency of 97.6%and a high NH_(3)yield of 517.7μmol h^(-1)cm^(-2)at-0.6 V versus the reversible hydrogen electrode.Furthermore,insights into the reaction mechanism of CoSe_(2)in the electrocatalytic NO_(3)^(-)reduction are elucidated through density functional theory calculations.展开更多
基金support from the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811)。
文摘Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.
基金supported by grants from the National Key Research and Development Program of China (2020YFA0908200)Shanghai Municipal Education Commission-Gaofeng Clinical Medicine Grant Support (20171906)+2 种基金Shanghai Municipal Health and Family Planning Commission (2022XD055)Natural Science Foundation of Shandong Province (Shandong) (ZR2020QH121)GuangCi Professorship Program of Ruijin Hospital Shanghai Jiao Tong University School of Medicine
文摘Blood vessels are essential for nutrient and oxygen delivery and waste removal.Scaffold-repairing materials with functional vascular networks are widely used in bone tissue engineering.Additive manufacturing is a manufacturing technology that creates three-dimensional solids by stacking substances layer by layer,mainly including but not limited to 3D printing,but also 4D printing,5D printing and 6D printing.It can be effectively combined with vascularization to meet the needs of vascularized tissue scaffolds by precisely tuning the mechanical structure and biological properties of smart vascular scaffolds.Herein,the development of neovascularization to vascularization to bone tissue engineering is systematically discussed in terms of the importance of vascularization to the tissue.Additionally,the research progress and future prospects of vascularized 3D printed scaffold materials are highlighted and presented in four categories:functional vascularized 3D printed scaffolds,cell-based vascularized 3D printed scaffolds,vascularized 3D printed scaffolds loaded with specific carriers and bionic vascularized 3D printed scaffolds.Finally,a brief review of vascularized additive manufacturing-tissue scaffolds in related tissues such as the vascular tissue engineering,cardiovascular system,skeletal muscle,soft tissue and a discussion of the challenges and development efforts leading to significant advances in intelligent vascularized tissue regeneration is presented.
基金supported by National Key Research and Development Program of China(Grant No.2021YFA1400400)the National Natural Science Foundation of China(Grant Nos.11822405,12074174,12074175,11774152,11904170,12004249,12004251,and 12004191)+3 种基金the Natural Science Foundation of Jiangsu Province(Grant Nos.BK20180006,BK20190436 and BK20200738)the Shanghai Sailing Program(Grant Nos.20YF1430600 and21YF1429200)the Fundamental Research Funds for the Central Universities(Grant No.020414380183)the Office of International Cooperation and Exchanges of Nanjing University。
文摘It is known that α-RuCl_(3) has been studied extensively because of its proximity to the Kitaev quantum-spin-liquid(QSL)phase and the possibility of approaching it by tuning the competing interactions.Here we present the first polarized inelastic neutron scattering study on α-RuCl_(3) single crystals to explore the scattering continuum around the Γ point at the Brillouin zone center,which was hypothesized to be resulting from the Kitaev QSL state but without concrete evidence.With polarization analyses,we find that,while the spin-wave excitations around the Γ point vanish above the transition temperature T_(N),the pure magnetic continuous excitations around the Γ point are robust against temperature.Furthermore,by calculating the dynamical spin-spin correlation function using the cluster perturbation theory,we derive magnetic dispersion spectra based on the K-Γ model,which involves with a ferromagnetic Kitaev interaction of −7.2 meV and an off-diagonal interaction of 5.6 meV.We find this model can reproduce not only the spin-wave excitation spectra around the Γ point,but also the non-spin-wave continuous magnetic excitations around the Γ point.These results provide evidence for the existence of fractional excitations around the Γ point originating from the Kitaev QSL state,and further support the validity of the K-Γ model as the effective minimal spin model to describe α-RuCl_(3).
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11674157 and 11822405)the Fundamental Research Funds for the Central Universities(Grant No.020414380105)
文摘Quantum spin liquids(QSLs) represent a novel state of matter in which quantum fluctuations prevent the conventional magnetic order from being established, and the spins remain disordered even at zero temperature. There have been many theoretical developments proposing various QSL states. On the other hand, experimental movement was relatively slow largely due to limitations on the candidate materials and difficulties in the measurements. In recent years, the experimental progress has been accelerated. In this topical review, we give a brief summary of experiments on the QSL candidates under magnetic fields. We arrange our discussions by two categories: i) Geometrically-frustrated systems, including triangularlattice compounds YbMgGaO4 and YbZnGaO4, κ-(BEDT-TTF)2 Cu2(CN)3, and EtMe3 Sb[Pd(dmit)2]2, and the kagom′e system ZnCu3(OH)6 Cl2; ii) the Kitaev material α-RuCl3. Among these, we will pay special attention to α-RuCl3, which has been intensively studied by ours and other groups recently. We will present evidence that both supports and rejects the QSL ground state for these materials, based on which we give several perspectives to stimulate further research activities.
基金supported by the National Natural Science Foundation of China-Joint Fund Project(U22A20284)the National Natural Science Foundation of China(81972069,82202724)+1 种基金Doctoral Cultivating Project of the First Affiliated Hospital of Chongqing Medical University(CYYY-BSYJSCXXM-202227202204).
文摘Regulating macrophage activation precisely is crucial in treating chronic inflammation in osteoarthritis(OA).However,the stable pro-inflammatory state and deep distribution of macrophages in vivo pose a great challenge to treatment.In this study,inspired by the innate immune,immune cell mobilized hydrogel microspheres were constructed by microfluidic methods and load chemokines,macrophage antibodies and engineered cell membrane vesicles(sEVs)via covalent and non-covalent junctions.The immune cell mobilized hydrogel microspheres,based on a mixture of streptavidin grafted hyaluronic acid methacrylate(HAMA-SA)and Chondroitin sulfate methacrylate(ChSMA)microspheres(HCM),can recruit,capture and reprogram proinflammatory macrophages in the joint cavity to improve the joint inflammatory microenvironment.In vitro experiments demonstrated that immune cell mobilized hydrogel microspheres had excellent macrophage recruitment,capture,and reprogramming abilities.Pro-inflammatory macrophages can be transformed into anti-inflammatory macrophages with an efficiency of 88.5%.Animal experiments also revealed significant reduction in synovial inflammation and cartilage matrix degradation of OA.Therefore,the immune cell mobilized hydrogel microspheres may be an effective treatment of OA inflammation for the future.
文摘Nitrate(NO_(3)^(-)),a nitrogen-containing pollutant,is prevalent in aqueous solutions,contributing to a range of environmental and health-related issues.The electrocatalytic reduction of NO_(3)^(-)holds promise as a sustainable approach to both eliminating NO_(3)^(-)and generating valuable ammonia(NH_(3)).Nevertheless,the reduction reaction of NO_(3)^(-)(NO_(3)^(-)RR),involving 8-electron transfer process,is intricate,necessitating highly efficient electrocatalysts to facilitate the conversion of NO_(3)^(-)to NH_(3).In this study,Fe-doped Co_(3)O_(4) nanowire strutted three-dimensional(3D)pinewood-derived carbon(Fe-Co_(3)O_(4)/PC)is proposed as a high-efficiency NO_(3)^(-)RR electrocatalyst for NH_(3) production.Operating within 0.1 M NaOH containing NO_(3)^(-),Fe-Co_(3)O_(4)/PC demonstrates exceptional performance,obtain an impressively large NH_(3) yield of 0.55 mmol·h^(-1)·cm^(-2) and an exceptionally high Faradaic efficiency of 96.5%at-0.5 V,superior to its Co_(3)O_(4)/PC counterpart(0.2 mmol·h^(-1)·cm^(-2),73.3%).Furthermore,the study delves into the reaction mechanism of Fe-Co_(3)O_(4) for NO_(3)^(-)RR through theoretical calculations.
基金the National Natural Science Foundation of China(82072443 and 82372425)the China Postdoctoral Science Foundation(Grant No.2022M710557)+1 种基金the Natural Science Foundation of Chongqing,China(Grant No.CSTB2023NSCQ-BHX0011)the Young Excellent Science and Technology Talent Project of the First Affiliated Hospital of Chongqing Medical University(Grant No.ZYRC2022-05).
文摘Subcellular mitochondria serve as sensors for energy metabolism and redox balance, and the dynamic regulation of functional and dysfunctional mitochondria plays a crucial role in determining cells' fate. Selective removal of dysfunctional mitochondria at the subcellular level can provide chondrocytes with energy to prevent degeneration, thereby treating osteoarthritis. Herein, to achieve an ideal subcellular therapy, cartilage affinity peptide (WYRGRL)-decorated liposomes loaded with mitophagy activator (urolithin A) were integrated into hyaluronic acid methacrylate hydrogel microspheres through microfluidic technology, named HM@WY-Lip/UA, that could efficiently target chondrocytes and selectively remove subcellular dysfunctional mitochondria. As a result, this system demonstrated an advantage in mitochondria function restoration, reactive oxygen species scavenging, cell survival rescue, and chondrocyte homeostasis maintenance through increasing mitophagy. In a rat post-traumatic osteoarthritis model, the intra-articular injection of HM@WY-Lip/UA ameliorated cartilage matrix degradation, osteophyte formation, and subchondral bone sclerosis at 8 weeks. Overall, this study indicated that HM@WY-Lip/UA provided a protective effect on cartilage degeneration in an efficacious and clinically relevant manner, and a mitochondrial-oriented strategy has great potential in the subcellular therapy of osteoarthritis.
基金supported by the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811).
文摘Seawater electrolysis,especially in coastlines,is widely considered as a sustainable way of making clean and high-purity H2 from renewable energy;however,the practical viability is challenged severely by the limited anode durability resulting from side reactions of chlorine species.Herein,we report an effective Cl^(−) blocking barrier of NiFe-layer double hydroxide(NiFe-LDH)to harmful chlorine chemistry during alkaline seawater oxidation(ASO),a pre-formed surface-derived NiFe-phosphate(Pi)outerlayer.Specifically,the PO_(4)^(3−)-enriched outer-layer is capable of physically and electrostatically inhibiting Cl−adsorption,which protects active Ni^(3+)sites during ASO.The NiFe-LDH with the NiFe-Pi outer-layer(NiFe-LDH@NiFe-Pi)exhibits higher current densities(j)and lower overpotentials to afford 1 A·cm^(−2)(η1000 of 370 mV versusη1000 of 420 mV)than the NiFe-LDH in 1 M KOH+seawater.Notably,the NiFe-LDH@NiFe-Pi also demonstrates longer-term electrochemical durability than NiFe-LDH,attaining 100-h duration at the j of 1 A·cm^(−2).Additionally,the importance of surface-derived PO_(4)^(3−)-enriched outer-layer in protecting the active centers,γ-NiOOH,is explained by ex situ characterizations and in situ electrochemical spectroscopic studies.
基金supported by the National Natural Science Foundation of China(82071104/32101104/82202663)Science and Technology Commission of Shanghai Municipality(23XD1434200/22Y21901000)+2 种基金Program of Shanghai Academic/Technology Research Leader(22XD1422600)Shanghai Municipal Health Planning Commission(202140127)Shanghai Hospital Development Center(SHDC12022120).
文摘Irregular bone defects,characterized by unpredictable size,shape,and depth,pose a major challenge to clinical treatment.Although various bone grafts are available,none can fully meet the repair needs of the defective area.Here,this study fabricates a dough-type hydrogel(DR-Net),in which the first dynamic network is generated by coordination between thiol groups and silver ions,thereby possessing kneadability to adapt to various irregular bone defects.The second rigid covalent network is formed through photocrosslinking,maintaining the osteogenic space under external forces and achieving a better match with the bone regeneration process.In vitro,an irregular alveolar bone defect is established in the fresh porcine mandible,and the dough-type hydrogel exhibits outstanding shape adaptability,perfectly matching the morphology of the bone defect.After photocuring,the storage modulus of the hydrogel increases 8.6 times,from 3.7 kPa(before irradiation)to 32 kPa(after irradiation).Furthermore,this hydrogel enables effective loading of P24 peptide,which potently accelerates bone repair in Sprague–Dawley(SD)rats with critical calvarial defects.Overall,the dough-type hydrogel with kneadability,space-maintaining capability,and osteogenic activity exhibits exceptional potential for clinical translation in treating irregular bone defects.
基金financially supported by the National Natural Science Foundation of China(82102578,81922045,81772314 and 21604052)the National Natural Science Foundation of Chongqing(cstc2018jcyjAX0059 and cstc2018jcyjAX0797)Applied Basic Research Programs of the Science and Technology Department of Sichuan Province(2021YJ0467).
文摘Local lactate accumulation greatly hinders tissue repair and regeneration under ischemic condition.Herein,an injectable microsphere(MS@MCL)for local lactate exhaustion was constructed by grafting manganese dioxide(MnO_(2))-lactate oxidase(LOX)composite nanozyme on microfluidic hyaluronic acid methacrylate(HAMA)microspheres via chemical bonds,achieving a long-term oxygen-promoted lactate exhaustion effect and a long half-life in vivo.The uniform and porous microspheres synthesized by microfluidic technology is beneficial to in situ injection therapy and improving encapsulation efficiency.Furthermore,chemical grafting into HAMA microspheres through amide reactions promoted local enzymatic concentration and activity enhancement.It was showed that the MS@MCL eliminated oxidative and inflammatory stress and promoted extracellular matrix metabolism and cell survival when co-cultured with nucleus pulposus cells(NPCs)in vitro.In the rat degenerative intervertebral disc model caused by lactate injection,MS@MCL showed a long-term therapeutic effect in reducing intervertebral height narrowing and preventing extracellular matrix(ECM)degradation as well as inflammatory damage in vivo.Altogether,this study confirms that this nanozyme-functionalized injectable MS@MCL effectively improves the regenerative and reparative effect in ischemic tissues by disposing of enriched lactate in local microenvironment.
基金supported by the National Key Research and Development Program of China(2020YFA0908200)the National Natural Science Foundation of China(81873998,32101104 and 81972069)Shanghai Jiao Tong University“Medical and Research”Program(ZH2018ZDA04).
文摘Lipid-based boundary layers formed on liposome-containing hydrogels can facilitate lubrication.However,these boundary layers can be damaged by shear,resulting in decreased lubrication.Here,a shear-responsive boundary-lubricated drug-loaded hydrogel is created by incorporating celecoxib(CLX)-loaded liposomes within dynamic covalent bond-based hyaluronic acid(HA)hydrogels(CLX@Lipo@HA-gel).The dynamic cross-linked network enables the hydrogel to get restructured in response to shear,and the HA matrix allows the accumulation of internal liposome microreservoirs on the sliding surfaces,which results in the formation of boundary layers to provide stable lubrication.Moreover,hydration shells formed surrounding the hydrogel can retard the degradation process,thus helping in sustaining lubrication.Furthermore,in vitro and in vivo experiments found that CLX@Lipo@HA-gels can maintain anabolic-catabolic balance,alleviate cartilage wear,and attenuate osteoarthritis progression by delivering CLX and shear-responsive boundary lubrication.Overall,CLX@Lipo@HA-gels can serve as shear-responsive boundary lubricants and drug-delivery vehicles to alleviate friction-related diseases like osteoarthritis.
基金This research was funded by The National Key Research and Development Program of China(2020YFA0908200)National Natural Science Foundation of China General Program(81930051)+3 种基金Postdoctoral Research Foundation of China(2020M681319)the Interdisciplinary Program of Shanghai Jiao Tong University(YG2019ZDA05 and ZH2018ZDA04)“The Project Supported by the Foundation of National Facility for Translational Medicine(Shanghai)(TMSK-2020-117)”Shanghai Municipal Education Commission-Gaofeng Clinical Medicine Grant Support(20171906).
文摘Soft tissue remodeling is a sophisticated process that sequentially provides dynamic biological signals to guide cell behavior.However,capturing these signals within hydrogel and directing over time has still been unrealized owing to the poor comprehension of physiological processes.Here,a bio-mimicking hydrogel is designed via thiol-ene click reaction to capture the early physical signal triggered by inflammation,and the chemical signals provided with chemokine and natural adhesion sites,which guaranteed the precise soft tissue remodeling.This bio-mimicking hydrogel efficiently facilitated cell anchoring,migration,and invasion in the 3D matrix due to the permissive space and the interaction with integrin receptors.Besides,the covalently grafted chemokine-like peptide is optimal for colonization and functional differentiation of endothelial cells through a HIF-1αdependent signal pathway.Furthermore,the early polarization of macrophages,collagen deposition and angiogenesis in rat acute wound model,and the increased blood perfusion in mouse skin flap model have confirmed that the bio-mimicking hydrogel realized precise soft tissue remodeling and opens new avenues for the phased repair of different tissues such as nerve,myocardium,and even bone.
基金financially supported by the National Key R&D Program of China(2018YFC1106200)Shanghai Municipal Health and Family Planning Commission(201840027)+1 种基金Shanghai Municipal Education Commission-Gaofeng Clinical Medicine Grant Support(20171906)Shanghai Jiao Tong University“Medical and Research”Program(ZH2018ZDA04).
文摘Since their discovery,Black Phosphorus(BP)-based nanomaterials have received extensive attentions in the fields of electromechanics,optics and biomedicine,due to their remarkable properties and excellent biocompatibility.The most essential feature of BP is that it is composed of a single phosphorus element,which has a high degree of homology with the inorganic components of natural bone,therefore it has a full advantage in the treatment of bone defects.This review will first introduce the source,physicochemical properties,and degradation products of BP,then introduce the remodeling process of bone,and comprehensively summarize the progress of BP-based materials for bone therapy in the form of hydrogels,polymer membranes,microspheres,and three-dimensional(3D)printed scaffolds.Finally,we discuss the challenges and prospects of BP-based implant materials in bone immune regulation and outlook the future clinical application.
基金supported by the National Natural Science Foundation of China(11674157,51372112 and 11574133)the National Key Research and Development Plan(2016YFA0300404)the National Basic Research Program of China(2015CB921202)
文摘Dirac nodal-line semimetals with the linear bands crossing along a line or loop, represent a new topological state of matter. Here, by carrying out magnetotransport measurements and performing first-principle calculations, we demonstrate that such a state has been realized in high-quality single crystals of SrAs_3.We obtain the nontrivial ∏ Berry phase by analysing the Shubnikov-de Haas quantum oscillations. We also observe a robust negative longitudinal magnetoresistance induced by the chiral anomaly.Accompanying first-principles calculations identifies that a single hole pocket enclosing the loop nodes is responsible for these observations.
基金funding support through large group research project(No.RGP2/119/45)。
文摘The electrocatalytic reduction of nitrate(NO_(3)^(-))not only facilitates the environmentally sustainable production of ammonia(NH_(3))but also purifies water by removing NO_(3)^(-),thereby transforming waste into valuable resources.The process of converting NO_(3)^(-)to NH_(3)is complex,involving eight electron transfers and multiple intermediates,making the choice of electrocatalyst critical.In this study,we report a cobalt selenide(Co Se_(2))nanowire array on carbon cloth(CoSe_(2)/CC)as an effective electrocatalyst for the NO_(3)^(-)to NH_(3)conversion.In an alkaline medium with 0.1 mol/L NO_(3)^(-),CoSe_(2)/CC demonstrates exceptional NH_(3)Faradaic efficiency of 97.6%and a high NH_(3)yield of 517.7μmol h^(-1)cm^(-2)at-0.6 V versus the reversible hydrogen electrode.Furthermore,insights into the reaction mechanism of CoSe_(2)in the electrocatalytic NO_(3)^(-)reduction are elucidated through density functional theory calculations.