Photocatalysis is a promising green approach for water purification.The diversity of water pH values is a key factor that restricts its practical application since pH affects the adsorption of organic molecules,the st...Photocatalysis is a promising green approach for water purification.The diversity of water pH values is a key factor that restricts its practical application since pH affects the adsorption of organic molecules,the stability of catalysts and photocatalytic performance.Here,we report a pH–independent,efficient and stable photocatalytic system with a liquid(water)–liquid(oil)–solid(semiconductor)(L–L–S)triphase interface microenvironment.The system is fabricated by coating a thin layer of silicon oil on the surface of ZnO nanowire arrays,a model chemically unstable semiconductor in both acidic and alkaline solutions.We show that the unique interface makes the dye adsorption pH independent and prevents the semiconductor from being corroded by strong acidic/alkaline solutions,leading to a stable and efficient photocatalytic reaction over a wide pH range(1—14).These findings reveal a promising path for the development of high-performance catalysis systems applicable in complex water environments.展开更多
The development of cost-effective,robust,and durable electrocatalysts to replace the expensive Pt-based catalysts towards oxygen reduction reaction(ORR)is the trending frontier research topic in renewable energy and e...The development of cost-effective,robust,and durable electrocatalysts to replace the expensive Pt-based catalysts towards oxygen reduction reaction(ORR)is the trending frontier research topic in renewable energy and electrocatalysis.Particular attention has been paid to metal-nitrogen-carbon(M-N-C)single atom catalysts(SACs)due to their maximized atom utilization efficiency,biomimetic active site,and distinct electronic structure.More importantly,their catalytic properties can be further tailored by rationally regulating the microenvironment of active sites(i.e.,M-N coordination number,heteroatom doping and substitution.Herein,we present a comprehensive summary of the recent advancement in the microenvironment regulation of MN-C SACs towards improved ORR performance.The coordination environment manipulation regarding central metal and coordinated atoms is first discussed,focusing on the structure-function relationship.Apart from the near-range coordination,longrange substrate modulation including heteroatom doping,defect engineering is discussed as well.Besides,the synergy mechanism of nanoparticles and single atom sites to tune the electron cloud density at the active sites is summarized.Finally,we provide the challenges and outlook of the development of M-N-C SACs.展开更多
The immune response after implantation is a primary determinant of the tissue-repair effects of threedimensional(3D)-printed scaffolds.Thus,scaffolds that can subtly regulate immune responses may display extraordinary...The immune response after implantation is a primary determinant of the tissue-repair effects of threedimensional(3D)-printed scaffolds.Thus,scaffolds that can subtly regulate immune responses may display extraordinary functions.Inspired by the angiogenesis promotion effect of humoral immune response,we covalently combined mesoporous silica micro rod(MSR)/polyethyleneimine(PEI)/ovalbumin(OVA)self-assembled vaccines with 3D-printed calcium phosphate cement(CPC)scaffolds for local antigen-specific immune response activation.With the response activated,antigen-specific CD4+T helper2(Th2)cells can be recruited to promote early angiogenesis.The silicon(Si)ions from MSRs can accelerate osteogenesis,with an adequate blood supply being provided.At room temperature,scaffolds with uniformly interconnected macropores were printed using a self-setting CPC-based printing paste,which promoted the uniform dispersion and structural preservation of functional polysaccharides oxidized hyaluronic acid(OHA)inside.Sustained release of OVA was achieved with MSR/PEI covalently attached to scaffolds rich in aldehyde groups as the vaccine carrier.The vaccine-loaded scaffolds effectively recruited and activated dendritic cells(DCs)for antigen presentation and promoted the osteogenic differentiation of bone marrow mesenchymal stem cells(BMSCs)in vitro.When embedded subcutaneously in vivo,the vaccine-loaded scaffolds increased the proportion of Th2 cells in the spleen and locally recruited antigenspecific T cells to promote angiogenesis in and around the scaffold.Furthermore,the result in a rat skull defect-repair model indicated that the antigen-specific vaccine-loaded scaffolds promoted the regeneration of vascularized bone.This method may provide a novel concept for patient-specific implant design for angiogenesis promotion.展开更多
The occurrence and development of liver cancer are essentially the most serious outcomes of uncontrolled liver regeneration. The progression of liver cancer is inevitably related to the abnormal microenvironment of li...The occurrence and development of liver cancer are essentially the most serious outcomes of uncontrolled liver regeneration. The progression of liver cancer is inevitably related to the abnormal microenvironment of liver regeneration. The deterioration observed in the microenvironment of liver regeneration is a necessary condition for the occurrence, development and metastasis of cancer. Therefore, the use of a technique to prevent and treat liver cancer via changes in the microenvironment of liver regeneration is a novel strategy. This strategy would be an effective way to delay, prevent or even reverse cancer occurrence, development and metastasis through an improvement in the liver regeneration microenvironment along with the integrated regulation of multiple components, targets, levels, channels and time sequences. In addition, the treatment of ＂tonifying Shen（Kidney） to regulate liver regeneration and repair by affecting stem cells and their microenvironment＂ can regulate ＂the dynamic imbalance between the normal liver regeneration and the abnormal liver regeneration＂; this would improve the microenvironment of liver regeneration, which is also a mechanism by which liver cancer may be prevented or treated.展开更多
Supported by the National Natural Science Foundation of China,a collaborative study by the laboratories of Dr.Hu Guohong(胡国宏)from Shanghai Institutes for Biological Sciences,Chinese Academy of Sciences and Dr.Yang ...Supported by the National Natural Science Foundation of China,a collaborative study by the laboratories of Dr.Hu Guohong(胡国宏)from Shanghai Institutes for Biological Sciences,Chinese Academy of Sciences and Dr.Yang Qifeng(杨其峰)from Shangdong University demonstrates that Dickkopf1(DKK1)展开更多
Electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)represents one of the most promising technologies for sustainable conversion of CO_(2) to value-added products.Although metal-organic frameworks(MOFs)can be...Electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)represents one of the most promising technologies for sustainable conversion of CO_(2) to value-added products.Although metal-organic frameworks(MOFs)can be vastly functionalized to create active sites for CO_(2)RR,low intrinsic electrical conductivity always makes MOFs unfavorable candidates for eCO_(2)RR.Besides,studies on how to regulate eCO_(2)RR activity of MOFs from linkers'functionalities viewpoint lag far behind when compared with the assembly of multinuclear metal-centered clusters.In this work,non-toxic bismuth(Ⅲ)oxide(Bi2O3)was incorporated into a series of two-dimensional(2D)MOFs(ZrLX)established from Zr-oxo clusters and triazine-centered 3-c linkers with different functionalities(LX=1-5)to give composites ZrLX/Bi2O3.To investigate how functionalities on linkers distantly tune the eCO_(2)RR performance of MOFs,electron-donating/withdrawing groups were installed at triazine core or benzoate terminals.It is found that ZrL2/Bi2O3(-F functionalized on triazine core)exhibits the best eCO_(2)RR performance with the highest Faradaic efficiency(FE)of 96.73%at-1.07 V vs.RHE,the largest electroactive surface(Cdi=4.23 mF cm-2)and the highest electrical conductivity(5.54 x 10-7 S cm-1),highlighting tuning linker functionalities and hence electronic structure as an alternative way to regulate eCO_(2)RR.展开更多
A long-standing paucity of effective therapies results in the poor outcomes of triple-negative breast cancer brain metastases.Immunotherapy has made progress in the treatment of tumors,but limited by the non-immunogen...A long-standing paucity of effective therapies results in the poor outcomes of triple-negative breast cancer brain metastases.Immunotherapy has made progress in the treatment of tumors,but limited by the non-immunogenicity of tumors and strong immunosuppressive environment,patients with TNBC brain metastases have not yet benefited from immunotherapy.Dual immunoregulatory strategies with enhanced immune activation and reversal of the immunosuppressive microenvironment provide new therapeutic options for patients.Here,we propose a cocktail-like therapeutic strategy of microenvironment regulation-chemotherapy-immune synergistic sensitization and construct reduction-sensitive immune microenvironment regulation nanomaterials(SIL@T).SIL@T modified with targeting peptide penetrates the BBB and is subsequently internalized into metastatic breast cancer cells,releasing silybin and oxaliplatin responsively in the cells.SIL@T preferentially accumulates at the metastatic site and can significantly prolong the survival period of model animals.Mechanistic studies have shown that SIL@T can effectively induce immunogenic cell death of metastatic cells,activate immune responses and increase infiltration of CD8+T cells.Meanwhile,the activation of STAT3 in the metastatic foci is attenuated and the immunosuppressive microenvironment is reversed.This study demonstrates that SIL@T with dual immunomodulatory functions provides a promising immune synergistic therapy strategy for breast cancer brain metastases.展开更多
基金supported by the National Key R&D Program of China(2019YFA0709200)the National Natural Science Foundation of China(21988102,51772198,21975171)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Photocatalysis is a promising green approach for water purification.The diversity of water pH values is a key factor that restricts its practical application since pH affects the adsorption of organic molecules,the stability of catalysts and photocatalytic performance.Here,we report a pH–independent,efficient and stable photocatalytic system with a liquid(water)–liquid(oil)–solid(semiconductor)(L–L–S)triphase interface microenvironment.The system is fabricated by coating a thin layer of silicon oil on the surface of ZnO nanowire arrays,a model chemically unstable semiconductor in both acidic and alkaline solutions.We show that the unique interface makes the dye adsorption pH independent and prevents the semiconductor from being corroded by strong acidic/alkaline solutions,leading to a stable and efficient photocatalytic reaction over a wide pH range(1—14).These findings reveal a promising path for the development of high-performance catalysis systems applicable in complex water environments.
基金supported by the National Natural Science Foundation of China(No.22272161).
文摘The development of cost-effective,robust,and durable electrocatalysts to replace the expensive Pt-based catalysts towards oxygen reduction reaction(ORR)is the trending frontier research topic in renewable energy and electrocatalysis.Particular attention has been paid to metal-nitrogen-carbon(M-N-C)single atom catalysts(SACs)due to their maximized atom utilization efficiency,biomimetic active site,and distinct electronic structure.More importantly,their catalytic properties can be further tailored by rationally regulating the microenvironment of active sites(i.e.,M-N coordination number,heteroatom doping and substitution.Herein,we present a comprehensive summary of the recent advancement in the microenvironment regulation of MN-C SACs towards improved ORR performance.The coordination environment manipulation regarding central metal and coordinated atoms is first discussed,focusing on the structure-function relationship.Apart from the near-range coordination,longrange substrate modulation including heteroatom doping,defect engineering is discussed as well.Besides,the synergy mechanism of nanoparticles and single atom sites to tune the electron cloud density at the active sites is summarized.Finally,we provide the challenges and outlook of the development of M-N-C SACs.
基金supported by the National Key Research and Development Program of China(2019YFA0112000 and 2018YFB1105600)the National Natural Science Foundation of China(81930051)+2 种基金Shanghai Municipal Education Commission-Gaofeng Clinical Medicine Grant Support(20171906)Shanghai Jiao Tong University “Medical and Research”Program(ZH2018ZDA04)Foundation of National Facility for Translational Medicine(Shanghai)(TMSK-2020-117)。
文摘The immune response after implantation is a primary determinant of the tissue-repair effects of threedimensional(3D)-printed scaffolds.Thus,scaffolds that can subtly regulate immune responses may display extraordinary functions.Inspired by the angiogenesis promotion effect of humoral immune response,we covalently combined mesoporous silica micro rod(MSR)/polyethyleneimine(PEI)/ovalbumin(OVA)self-assembled vaccines with 3D-printed calcium phosphate cement(CPC)scaffolds for local antigen-specific immune response activation.With the response activated,antigen-specific CD4+T helper2(Th2)cells can be recruited to promote early angiogenesis.The silicon(Si)ions from MSRs can accelerate osteogenesis,with an adequate blood supply being provided.At room temperature,scaffolds with uniformly interconnected macropores were printed using a self-setting CPC-based printing paste,which promoted the uniform dispersion and structural preservation of functional polysaccharides oxidized hyaluronic acid(OHA)inside.Sustained release of OVA was achieved with MSR/PEI covalently attached to scaffolds rich in aldehyde groups as the vaccine carrier.The vaccine-loaded scaffolds effectively recruited and activated dendritic cells(DCs)for antigen presentation and promoted the osteogenic differentiation of bone marrow mesenchymal stem cells(BMSCs)in vitro.When embedded subcutaneously in vivo,the vaccine-loaded scaffolds increased the proportion of Th2 cells in the spleen and locally recruited antigenspecific T cells to promote angiogenesis in and around the scaffold.Furthermore,the result in a rat skull defect-repair model indicated that the antigen-specific vaccine-loaded scaffolds promoted the regeneration of vascularized bone.This method may provide a novel concept for patient-specific implant design for angiogenesis promotion.
基金Supported by the National Natural Science Foundation of China(No.81373513)Research Projects of Key Diseases of the National Traditional Chinese Medicine Clinical Research Center,Hubei Province(No.JDZX2012054,JDZX2015172)
文摘The occurrence and development of liver cancer are essentially the most serious outcomes of uncontrolled liver regeneration. The progression of liver cancer is inevitably related to the abnormal microenvironment of liver regeneration. The deterioration observed in the microenvironment of liver regeneration is a necessary condition for the occurrence, development and metastasis of cancer. Therefore, the use of a technique to prevent and treat liver cancer via changes in the microenvironment of liver regeneration is a novel strategy. This strategy would be an effective way to delay, prevent or even reverse cancer occurrence, development and metastasis through an improvement in the liver regeneration microenvironment along with the integrated regulation of multiple components, targets, levels, channels and time sequences. In addition, the treatment of ＂tonifying Shen（Kidney） to regulate liver regeneration and repair by affecting stem cells and their microenvironment＂ can regulate ＂the dynamic imbalance between the normal liver regeneration and the abnormal liver regeneration＂; this would improve the microenvironment of liver regeneration, which is also a mechanism by which liver cancer may be prevented or treated.
文摘Supported by the National Natural Science Foundation of China,a collaborative study by the laboratories of Dr.Hu Guohong(胡国宏)from Shanghai Institutes for Biological Sciences,Chinese Academy of Sciences and Dr.Yang Qifeng(杨其峰)from Shangdong University demonstrates that Dickkopf1(DKK1)
基金supported by the National Natural Science Foundation of China(22371054,22301045)the Foundation of Basic and Applied Basic Research of Guangdong Province(2020B1515120024,2024A1515012801)+1 种基金Science and Technology Planning Project of Guangdong Province(2021A0505030066,2023A0505050164)Science and Technology Program of Guangzhou(202201010244).
文摘Electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)represents one of the most promising technologies for sustainable conversion of CO_(2) to value-added products.Although metal-organic frameworks(MOFs)can be vastly functionalized to create active sites for CO_(2)RR,low intrinsic electrical conductivity always makes MOFs unfavorable candidates for eCO_(2)RR.Besides,studies on how to regulate eCO_(2)RR activity of MOFs from linkers'functionalities viewpoint lag far behind when compared with the assembly of multinuclear metal-centered clusters.In this work,non-toxic bismuth(Ⅲ)oxide(Bi2O3)was incorporated into a series of two-dimensional(2D)MOFs(ZrLX)established from Zr-oxo clusters and triazine-centered 3-c linkers with different functionalities(LX=1-5)to give composites ZrLX/Bi2O3.To investigate how functionalities on linkers distantly tune the eCO_(2)RR performance of MOFs,electron-donating/withdrawing groups were installed at triazine core or benzoate terminals.It is found that ZrL2/Bi2O3(-F functionalized on triazine core)exhibits the best eCO_(2)RR performance with the highest Faradaic efficiency(FE)of 96.73%at-1.07 V vs.RHE,the largest electroactive surface(Cdi=4.23 mF cm-2)and the highest electrical conductivity(5.54 x 10-7 S cm-1),highlighting tuning linker functionalities and hence electronic structure as an alternative way to regulate eCO_(2)RR.
基金support from the National Natural Science Foundation of China(32030059,82273865,82121002)Key Projects of Shanghai Science Foundation(19JC1410800)Shanghai Municipal Science and Technology Major Project(Grant 2018SHZDZX01)and ZJLab.
文摘A long-standing paucity of effective therapies results in the poor outcomes of triple-negative breast cancer brain metastases.Immunotherapy has made progress in the treatment of tumors,but limited by the non-immunogenicity of tumors and strong immunosuppressive environment,patients with TNBC brain metastases have not yet benefited from immunotherapy.Dual immunoregulatory strategies with enhanced immune activation and reversal of the immunosuppressive microenvironment provide new therapeutic options for patients.Here,we propose a cocktail-like therapeutic strategy of microenvironment regulation-chemotherapy-immune synergistic sensitization and construct reduction-sensitive immune microenvironment regulation nanomaterials(SIL@T).SIL@T modified with targeting peptide penetrates the BBB and is subsequently internalized into metastatic breast cancer cells,releasing silybin and oxaliplatin responsively in the cells.SIL@T preferentially accumulates at the metastatic site and can significantly prolong the survival period of model animals.Mechanistic studies have shown that SIL@T can effectively induce immunogenic cell death of metastatic cells,activate immune responses and increase infiltration of CD8+T cells.Meanwhile,the activation of STAT3 in the metastatic foci is attenuated and the immunosuppressive microenvironment is reversed.This study demonstrates that SIL@T with dual immunomodulatory functions provides a promising immune synergistic therapy strategy for breast cancer brain metastases.
