Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally ...Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally interconnected ordered macroporous structure and a robust framework were fabricated and used as stable and selective catalysts in the oxidative dehydrogenation(ODH)of propane.Due to the improved mass diffusion and higher number of exposed active sites in the ordered macroporous structure,the catalyst exhibited a remarkable olefin productivity of^16 golefin gcat^-1 h^-1,which is up to 2–100 times higher than that of ODH catalysts reported to date.The selectivity for olefins was 91.5%(propene:82.5%,ethene:9.0%)at 515℃,with a propane conversion of 14.3%.At the same time,the selectivity for the unwanted deep-oxidized CO2 product remained less than 1.0%.The tri-coordinated surface boron species were identified as the active catalytic sites for the ODH of propane.This study provides a route for preparing a new type of metal-free catalyst with stable structure against oxidation and remarkable catalytic activity,which may represent a potential candidate to promote the industrialization of the ODH process.展开更多
Hepatocellular carcinoma(HCC)is the most common primary liver cancer with a poor prognosis.Chemotherapy is one of the first-line clinical therapeutic strategies for HCC.Still,the effectiveness of chemotherapy is hampe...Hepatocellular carcinoma(HCC)is the most common primary liver cancer with a poor prognosis.Chemotherapy is one of the first-line clinical therapeutic strategies for HCC.Still,the effectiveness of chemotherapy is hampered by the tumor immunosuppressive microenvironment and drug resistance caused by insufficient delivery.Herein,we developed a metal-drug self-delivery nanomedicine(FDAH)to improve the chemo/chemodynamic therapeutic efficacy of HCC.The core of FDAH is an iron-based nanoparticle chelated with two clinical drugs,Doxorubicin(DOX)and Plerixafor(AMD3100).Additionally,the nanomedicine is externally modified with a hyaluronic acid(HA)shell,which can prolong the circulation time of the nanoparticles in the bloodstream after intravenous administration.After entering the bloodstream,the nanomedicine reaches the tumor tissue through the EPR effect and is phagocytosed by the tumor cells via HA/CD44-specific interaction.Iron ion-mediated chemodynamic therapy is mediated by the Fenton reaction to generate ROS,causing an imbalance of redox homeostasis within the tumor cells and enhancing the sensitivity of tumor cells to DOX.In addition,AMD3100 intervenes in the CXCL12/CXCR4 axis to influence the infiltration level of immune cells and promote DOX chemotherapy in tumor cells.This work suggests that alleviating immunosuppression via a metal-drug self-delivery system of the CXCR4 inhibitor can effectively improve the DOX chemotherapy and iron ions-mediated chemodynamic therapy.展开更多
Reversal of cancer drug resistance remains a critical challenge in chemotherapy.Mitochondria-targeted drug delivery has been suggested to mitigate drug resistance in cancer.To overcome the intrinsic limitations in con...Reversal of cancer drug resistance remains a critical challenge in chemotherapy.Mitochondria-targeted drug delivery has been suggested to mitigate drug resistance in cancer.To overcome the intrinsic limitations in conventional mitochondrial targeting strategies,we develop mitochondrial temperature-responsive drug delivery to reverse doxorubicin(DOX)resistance in lung cancer.Results demonstrate that the thermoresponsive nanocarrier can prevent DOX efflux and facilitate DOX accumulation and mitochondrial targeting in DOX-resistant tumors.As a consequence,thermoresponsive nanocarrier enhances the cytotoxicity of DOX and reverses the drug resistance in tumor-bearing mice.This work represents the first example of mitochondrial temperature-responsive drug delivery for reversing cancer drug resistance.展开更多
文摘Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally interconnected ordered macroporous structure and a robust framework were fabricated and used as stable and selective catalysts in the oxidative dehydrogenation(ODH)of propane.Due to the improved mass diffusion and higher number of exposed active sites in the ordered macroporous structure,the catalyst exhibited a remarkable olefin productivity of^16 golefin gcat^-1 h^-1,which is up to 2–100 times higher than that of ODH catalysts reported to date.The selectivity for olefins was 91.5%(propene:82.5%,ethene:9.0%)at 515℃,with a propane conversion of 14.3%.At the same time,the selectivity for the unwanted deep-oxidized CO2 product remained less than 1.0%.The tri-coordinated surface boron species were identified as the active catalytic sites for the ODH of propane.This study provides a route for preparing a new type of metal-free catalyst with stable structure against oxidation and remarkable catalytic activity,which may represent a potential candidate to promote the industrialization of the ODH process.
基金supported by the Beijing Natural Science Foundation(L248075)the National Natural Science Foundation of China(32171370)+2 种基金the Guangdong Basic and Applied Basic Research Foundation(2022A1515140073 and 2022A1515010415)the Scientific and Technological Innovation Project of China Academy of Chinese Medical Sciences(CI2023C012YL)the Science and Technology Program of Guangzhou(2023A03J0493).
文摘Hepatocellular carcinoma(HCC)is the most common primary liver cancer with a poor prognosis.Chemotherapy is one of the first-line clinical therapeutic strategies for HCC.Still,the effectiveness of chemotherapy is hampered by the tumor immunosuppressive microenvironment and drug resistance caused by insufficient delivery.Herein,we developed a metal-drug self-delivery nanomedicine(FDAH)to improve the chemo/chemodynamic therapeutic efficacy of HCC.The core of FDAH is an iron-based nanoparticle chelated with two clinical drugs,Doxorubicin(DOX)and Plerixafor(AMD3100).Additionally,the nanomedicine is externally modified with a hyaluronic acid(HA)shell,which can prolong the circulation time of the nanoparticles in the bloodstream after intravenous administration.After entering the bloodstream,the nanomedicine reaches the tumor tissue through the EPR effect and is phagocytosed by the tumor cells via HA/CD44-specific interaction.Iron ion-mediated chemodynamic therapy is mediated by the Fenton reaction to generate ROS,causing an imbalance of redox homeostasis within the tumor cells and enhancing the sensitivity of tumor cells to DOX.In addition,AMD3100 intervenes in the CXCL12/CXCR4 axis to influence the infiltration level of immune cells and promote DOX chemotherapy in tumor cells.This work suggests that alleviating immunosuppression via a metal-drug self-delivery system of the CXCR4 inhibitor can effectively improve the DOX chemotherapy and iron ions-mediated chemodynamic therapy.
基金We are grateful to Beijing Natural Science Foundation(7212212)National Natural Science Foundation of China(11875269 and 21574136)Hundred Talents Program of CAS for financial support。
文摘Reversal of cancer drug resistance remains a critical challenge in chemotherapy.Mitochondria-targeted drug delivery has been suggested to mitigate drug resistance in cancer.To overcome the intrinsic limitations in conventional mitochondrial targeting strategies,we develop mitochondrial temperature-responsive drug delivery to reverse doxorubicin(DOX)resistance in lung cancer.Results demonstrate that the thermoresponsive nanocarrier can prevent DOX efflux and facilitate DOX accumulation and mitochondrial targeting in DOX-resistant tumors.As a consequence,thermoresponsive nanocarrier enhances the cytotoxicity of DOX and reverses the drug resistance in tumor-bearing mice.This work represents the first example of mitochondrial temperature-responsive drug delivery for reversing cancer drug resistance.
