This study observed the immune response induced by a HSP65 DNA vaccine fused with UbGR against Mycobacterium tuberculosis. BALB/c mice were inoculated with HSP65 DNA vaccine, UbGR-fused HSP65 DNA vaccine (Ub-GR-HSP65)...This study observed the immune response induced by a HSP65 DNA vaccine fused with UbGR against Mycobacterium tuberculosis. BALB/c mice were inoculated with HSP65 DNA vaccine, UbGR-fused HSP65 DNA vaccine (Ub-GR-HSP65) and blank vector respectively. HSP65 DNA vaccine elicited a Thl-polarized immune response. The Thl-type cytokine (IFN-γ) and proliferative T cell responses from spleen were improved significantly in UbGR-HSP65 group, compared with those in HSP65 DNA vaccine group. Furthermore, this fusion DNA vaccine also led to an increased ratio of IgG2ato IgGl and the cytotoxicity of T cells. IFN-γ intracellular staining of splenocytes indicated that UbGR-HSP65 fusion DNA vaccine could activate CD4+ and CD8+ T cells, with much higher CD8+ T cells. Thus, this study demonstrated that the UbGR fusion could improve HSP65-specific cellular immune responses, which is helpful to protect against TB infection.展开更多
All-dielectric metamaterials have emerged as a promising platform for low-loss and highly efficient terahertz devices. However, existing fabrication methods have difficulty in achieving a good balance between precisio...All-dielectric metamaterials have emerged as a promising platform for low-loss and highly efficient terahertz devices. However, existing fabrication methods have difficulty in achieving a good balance between precision and cost. Here, inspired by the nano-template-assisted self-assembly method, we develop a micro-templateassisted self-assembly(MTAS) method to prepare large-scale, high-precision, and flexible ceramic microsphere all-dielectric metamaterials with an area exceeding 900 cm × 900 cm. Free from organic solvents, vacuum, and complex equipment, the MTAS method ensures low-cost and environmentally friendly fabrication. The ceramic microsphere resonators can be readily assembled into nearly arbitrary arrangements and complex aggregates, such as dimers, trimers, quadrumers, and chains. Finally, using the heat-shrinkable substrate and dipole coupling effect, a broadband reflector with a bandwidth of 0.15 THz and a reflection of up to 95% is demonstrated.This work provides a versatile and powerful platform for terahertz all-dielectric metamaterials, with potential to be applied in a wide variety of high-efficiency terahertz devices.展开更多
A kind of pollution known as electromagnetic interference(EMI),which results from ubiquitous usage of various electronic communication and military radar equipment,has been receiving increasing attention recently.Howe...A kind of pollution known as electromagnetic interference(EMI),which results from ubiquitous usage of various electronic communication and military radar equipment,has been receiving increasing attention recently.However,large-area EMI shielding on transparent and/or curved surfaces,including building windows,curved glass wall,and special requirements spaces(SRSs),remains hard to achieve.In this paper,a silver nanofiber(AgNF)based flexible and transparent EMI shielding film was successfully assembled via a room-temperature roll-to-roll production method.For transparent application scenario,AgNF with 89%transmittance in visible range and 1μm thickness shows~20 dB shielding efficiency(EMI SE).On the other hand,total shielding(>50 dB)is obtained when the thickness of AgNF increases to 10μm,while its transmittance in visible range remains higher than 75%.Considering the facile and scale-free production technology,this material can be readily applied in large-scale,transparent,and/or SRSs EMI shielding.展开更多
In this review, the methodologies for fluorine incorporation of 40 fluorine-containing agrochemicals that received an international standardization organization(ISO) name during the last decade are described.The predo...In this review, the methodologies for fluorine incorporation of 40 fluorine-containing agrochemicals that received an international standardization organization(ISO) name during the last decade are described.The predominant approach for fluorine introduction of these agrochemicals is to use a fluorine-containing building block. Here we present how the fluorine-containing building blocks are introduced into these agrochemicals. The synthetic methods of fluorine-containing building blocks that are not easily available are also specifically discussed. Fluoroarenes, difluomethylarenes and trifluomethylarenes are the main building blocks that have been used in this review. Fluorine-containing small molecules, such as alcohol,amine, ketoester, olefin are also widely used. The only example of late-stage fluorination is the synthesis of fungicide quinofumelin. We believe the fluorine introduction methods described here can provide ideas for the development of new and economical pesticide synthetic routes, and stimulate researchers to develop new fluorine incorporation methods and create new pesticides.展开更多
Several different alkoxycarbonyl-substituted 2-benzoxazolinone moieties have been incorporated into a tetrahy- droisoindoline-1,3-dione scaffold to provide 25 compounds (1a-lu and 2a-2d). The structures of these com...Several different alkoxycarbonyl-substituted 2-benzoxazolinone moieties have been incorporated into a tetrahy- droisoindoline-1,3-dione scaffold to provide 25 compounds (1a-lu and 2a-2d). The structures of these compounds were confirmed by 1H and 13C NMR, HRMS and X-ray single-crystal diffraction. Some of these compounds (1g, 1h, 1j, 1k) exhibited excellent herbicidal activities against Abutilon theophrasti, Amaranthus retroflexus and Eehinochloa crus-galli at a rate of 375 g AI·ha^-1. Among them, compounds lh and 1j displayed the best post-emergence herbicidal effect against Abutilon theophrasti with ED50 values of 1.8 and 5.3 g AI·ha^-1, respectively, which are superior to that of the commercial acifluorfen (44.3 g AI·ha^-1). Field trials demonstrated that compound lh exhibited similar herbicidal activity to a high concentration atrazine, and found to be safer for maize than atrazine. The results of this study therefore show that compound lh could potentially be used as a post-emergence herbicide for maize fields.展开更多
Manufacturing a flexible,light,large-area,and high-efficiency electromagnetic shielding materials in a straightforward and cost-effective manner presently remains a significant challenge.In this work,we propose a cond...Manufacturing a flexible,light,large-area,and high-efficiency electromagnetic shielding materials in a straightforward and cost-effective manner presently remains a significant challenge.In this work,we propose a conductive network design and verify its electromagnetic interference(EMI)shielding effectiveness(SE)by simulation.Using the structure and parameters obtained by simulation,we prepare a flexible EMI shielding material using silver nanowires(AgNWs)/polyvinyl butyral(PVB)ethanol solution and textile substructure via a facile immersing method.In the frequency range of 5-18 GHz,the AgNWs/PVB textile with 1.4 mm thickness achieves an EMI SE of 59 dB,which exceeds the requirements for commercial applications.Due to the low density of 56 mg/cm^(3),specific shielding effectiveness(SSE)of this material reaches 1053 dB m^(3)/g.It is found that the AgNWs/PVB textile is more resistant to washing with water and oxidation than AgNWs textile without a PVB protector.As a result,the conductivity of AgNWs/PVB textile exhibits no change after washing with water and varies slightly after being kept in hot air.We find that a signal monitor is unable to detect a signal emitted by a mobile phone from a jacket lined with AgNWs/PVB textile.AgNWs/PVB textile with these properties can be mass-produced as high-efficiency EMI shielding material for commercial applications.展开更多
Herein,we report a practical electro-reductive protocol for the direct C-H cyanoalkylation of quinoxalin-2(1 H)-ones via iminyl radical-mediated ring opening.These mild reactions proceed under metal-,reductant-,and re...Herein,we report a practical electro-reductive protocol for the direct C-H cyanoalkylation of quinoxalin-2(1 H)-ones via iminyl radical-mediated ring opening.These mild reactions proceed under metal-,reductant-,and reagent-free conditions to provide synthetically useful cyanoalkylated quinoxalin-2(1 H)-ones.展开更多
The biological activities of a series of 3,3-spirocyclic indole derivatives containing CF_(2), phosphine oxide,indole, and cyano functional groups were evaluated, and these derivatives were found to exhibit antiTMV, f...The biological activities of a series of 3,3-spirocyclic indole derivatives containing CF_(2), phosphine oxide,indole, and cyano functional groups were evaluated, and these derivatives were found to exhibit antiTMV, fungicidal, and insecticidal activities.展开更多
We have developed a versatile,mild protocol for trifluoromethylthiolation reactions of aldehydes with catalysis by a decatungstate hydrogen atom transfer photocatalyst under redox-neutral conditions.The protocol is hi...We have developed a versatile,mild protocol for trifluoromethylthiolation reactions of aldehydes with catalysis by a decatungstate hydrogen atom transfer photocatalyst under redox-neutral conditions.The protocol is highly selective,operationally simple,and compatible with a wide array of sensitive functional groups.It can be used for late-stage functionalization of bioactive molecules,which makes it convenient for drug discovery.展开更多
It has previously been shown that tryptophan, the biosynthesis precursor ofPeganum harmala alkaloids, and its derivatives have anti-TMV activity bothin vitro and in vivo. Further exploration of this led to the identif...It has previously been shown that tryptophan, the biosynthesis precursor ofPeganum harmala alkaloids, and its derivatives have anti-TMV activity bothin vitro and in vivo. Further exploration of this led to the identification of NK0238as a highly effective agent for the prevention and control of diseases caused byplant viruses, but the existing routes are unsuitable for its large-scale synthesis.This study optimized a route for two-step synthesis of this virucide candidate viareaction of L-tryptophan with triphosgene to produce L-tryptophan-N-carboxylicanhydride, which then reacts with n-octylamine to give NK0238 at up to 94%yield and nearly 97% HPLC purity. In addition, the route was used for thepreparation of NK0238 on a > 40 g scale permitting further assessment of itsantivirus activity in the greenhouse and field experiments, and toxicity tests.NK0238 exhibited useful antiviral activities against a variety of viruses both ingreenhouse and field experiments. The toxicity tests showed that NK0238 wasnot acutely toxic to birds, fish, honey bees and silkworms. The optimized routeprovides a solid foundation for its large-scale synthesis and subsequent efficacyand toxicity studies, its excellent activity and safety make NK0238 a promisingdrug candidate for further development.展开更多
Herein,we report the first Rh~Ⅲ-catalyzed regioselective C8 arylation of quinoline N-oxides with commercially available arylboronic acids as coupling partners.This procedure is simple,and the reaction shows perfect r...Herein,we report the first Rh~Ⅲ-catalyzed regioselective C8 arylation of quinoline N-oxides with commercially available arylboronic acids as coupling partners.This procedure is simple,and the reaction shows perfect regioselectivity,a broad substrate scope,and isolated yields of up to 92%.We demonstrate the utility of the reaction by using it for late-stage functionalization of a fungicide.展开更多
文摘This study observed the immune response induced by a HSP65 DNA vaccine fused with UbGR against Mycobacterium tuberculosis. BALB/c mice were inoculated with HSP65 DNA vaccine, UbGR-fused HSP65 DNA vaccine (Ub-GR-HSP65) and blank vector respectively. HSP65 DNA vaccine elicited a Thl-polarized immune response. The Thl-type cytokine (IFN-γ) and proliferative T cell responses from spleen were improved significantly in UbGR-HSP65 group, compared with those in HSP65 DNA vaccine group. Furthermore, this fusion DNA vaccine also led to an increased ratio of IgG2ato IgGl and the cytotoxicity of T cells. IFN-γ intracellular staining of splenocytes indicated that UbGR-HSP65 fusion DNA vaccine could activate CD4+ and CD8+ T cells, with much higher CD8+ T cells. Thus, this study demonstrated that the UbGR fusion could improve HSP65-specific cellular immune responses, which is helpful to protect against TB infection.
基金National Natural Science Foundation of China(NSFC)(61774020,51502179)Department of Education of Hebei Province(QN2016156)+3 种基金Natural Science Foundation of Hebei Province(E2017210096)Fund of IPOC Beijing University of Posts and Telecommunications(BUPT)(IPOC2017ZT06)Fundamental Research Funds for the Central Universities(2018XKJC05)General Financial Grant from the China Postdoctoral Science Foundation(2017M620693)
文摘All-dielectric metamaterials have emerged as a promising platform for low-loss and highly efficient terahertz devices. However, existing fabrication methods have difficulty in achieving a good balance between precision and cost. Here, inspired by the nano-template-assisted self-assembly method, we develop a micro-templateassisted self-assembly(MTAS) method to prepare large-scale, high-precision, and flexible ceramic microsphere all-dielectric metamaterials with an area exceeding 900 cm × 900 cm. Free from organic solvents, vacuum, and complex equipment, the MTAS method ensures low-cost and environmentally friendly fabrication. The ceramic microsphere resonators can be readily assembled into nearly arbitrary arrangements and complex aggregates, such as dimers, trimers, quadrumers, and chains. Finally, using the heat-shrinkable substrate and dipole coupling effect, a broadband reflector with a bandwidth of 0.15 THz and a reflection of up to 95% is demonstrated.This work provides a versatile and powerful platform for terahertz all-dielectric metamaterials, with potential to be applied in a wide variety of high-efficiency terahertz devices.
基金This study was supported by the National Basic Research of China(Grants 2015CB932500)National Natural Science Foundations of China(Grant 51661135025 and 51522207)+1 种基金BUPT Excellent Ph.D.Students Foundation(Grant GX2017205)State Key Laboratory of Information Photonics and Optical Communications(Beijing University of Posts and Telecommunications).
文摘A kind of pollution known as electromagnetic interference(EMI),which results from ubiquitous usage of various electronic communication and military radar equipment,has been receiving increasing attention recently.However,large-area EMI shielding on transparent and/or curved surfaces,including building windows,curved glass wall,and special requirements spaces(SRSs),remains hard to achieve.In this paper,a silver nanofiber(AgNF)based flexible and transparent EMI shielding film was successfully assembled via a room-temperature roll-to-roll production method.For transparent application scenario,AgNF with 89%transmittance in visible range and 1μm thickness shows~20 dB shielding efficiency(EMI SE).On the other hand,total shielding(>50 dB)is obtained when the thickness of AgNF increases to 10μm,while its transmittance in visible range remains higher than 75%.Considering the facile and scale-free production technology,this material can be readily applied in large-scale,transparent,and/or SRSs EMI shielding.
基金National Natural Science Foundation of China (Nos.21732002,22077071)Frontiers Science Center for New Organic Matter,Nankai University (No.63181206) for generous financial support for our programs。
文摘In this review, the methodologies for fluorine incorporation of 40 fluorine-containing agrochemicals that received an international standardization organization(ISO) name during the last decade are described.The predominant approach for fluorine introduction of these agrochemicals is to use a fluorine-containing building block. Here we present how the fluorine-containing building blocks are introduced into these agrochemicals. The synthetic methods of fluorine-containing building blocks that are not easily available are also specifically discussed. Fluoroarenes, difluomethylarenes and trifluomethylarenes are the main building blocks that have been used in this review. Fluorine-containing small molecules, such as alcohol,amine, ketoester, olefin are also widely used. The only example of late-stage fluorination is the synthesis of fungicide quinofumelin. We believe the fluorine introduction methods described here can provide ideas for the development of new and economical pesticide synthetic routes, and stimulate researchers to develop new fluorine incorporation methods and create new pesticides.
基金This work was supported by the National Key Technologies R&D Program (No. 2011BAE06B03), and National Natural Science Foundation of China (No. 21172256).
文摘Several different alkoxycarbonyl-substituted 2-benzoxazolinone moieties have been incorporated into a tetrahy- droisoindoline-1,3-dione scaffold to provide 25 compounds (1a-lu and 2a-2d). The structures of these compounds were confirmed by 1H and 13C NMR, HRMS and X-ray single-crystal diffraction. Some of these compounds (1g, 1h, 1j, 1k) exhibited excellent herbicidal activities against Abutilon theophrasti, Amaranthus retroflexus and Eehinochloa crus-galli at a rate of 375 g AI·ha^-1. Among them, compounds lh and 1j displayed the best post-emergence herbicidal effect against Abutilon theophrasti with ED50 values of 1.8 and 5.3 g AI·ha^-1, respectively, which are superior to that of the commercial acifluorfen (44.3 g AI·ha^-1). Field trials demonstrated that compound lh exhibited similar herbicidal activity to a high concentration atrazine, and found to be safer for maize than atrazine. The results of this study therefore show that compound lh could potentially be used as a post-emergence herbicide for maize fields.
基金This work was financially supported by National Natural Science Foundation of China(Grant 61672108,61874014)China Postdoctoral Science Foundation(2018M640124,2019T120083)Program for Fund of State Key Laboratory of Information Photonics and Optical Communications(Beijing University of Posts and Telecommunications,China).
文摘Manufacturing a flexible,light,large-area,and high-efficiency electromagnetic shielding materials in a straightforward and cost-effective manner presently remains a significant challenge.In this work,we propose a conductive network design and verify its electromagnetic interference(EMI)shielding effectiveness(SE)by simulation.Using the structure and parameters obtained by simulation,we prepare a flexible EMI shielding material using silver nanowires(AgNWs)/polyvinyl butyral(PVB)ethanol solution and textile substructure via a facile immersing method.In the frequency range of 5-18 GHz,the AgNWs/PVB textile with 1.4 mm thickness achieves an EMI SE of 59 dB,which exceeds the requirements for commercial applications.Due to the low density of 56 mg/cm^(3),specific shielding effectiveness(SSE)of this material reaches 1053 dB m^(3)/g.It is found that the AgNWs/PVB textile is more resistant to washing with water and oxidation than AgNWs textile without a PVB protector.As a result,the conductivity of AgNWs/PVB textile exhibits no change after washing with water and varies slightly after being kept in hot air.We find that a signal monitor is unable to detect a signal emitted by a mobile phone from a jacket lined with AgNWs/PVB textile.AgNWs/PVB textile with these properties can be mass-produced as high-efficiency EMI shielding material for commercial applications.
基金the National Natural Science Foundation of China(Nos.21732002,22077071)Frontiers Science Center for New Organic Matter,Nankai University(No.63181206)for generous financial support for our programs。
文摘Herein,we report a practical electro-reductive protocol for the direct C-H cyanoalkylation of quinoxalin-2(1 H)-ones via iminyl radical-mediated ring opening.These mild reactions proceed under metal-,reductant-,and reagent-free conditions to provide synthetically useful cyanoalkylated quinoxalin-2(1 H)-ones.
基金National Natural Science Foundation of China (Nos.21732002,22077071,21977056)Frontiers Science Center for New Organic Matter,Nankai University (No.63181206)the Fundamental Research Funds for the Central Universities,Nankai University (No.63201043)。
文摘The biological activities of a series of 3,3-spirocyclic indole derivatives containing CF_(2), phosphine oxide,indole, and cyano functional groups were evaluated, and these derivatives were found to exhibit antiTMV, fungicidal, and insecticidal activities.
基金the National Natural Science Foundation of China (Nos.21732002, 22077071) for generous financial support for our programs。
文摘We have developed a versatile,mild protocol for trifluoromethylthiolation reactions of aldehydes with catalysis by a decatungstate hydrogen atom transfer photocatalyst under redox-neutral conditions.The protocol is highly selective,operationally simple,and compatible with a wide array of sensitive functional groups.It can be used for late-stage functionalization of bioactive molecules,which makes it convenient for drug discovery.
基金The authors are grateful to the National Natural Science Foundation of China(21977056,21732002)the Fundamental Research Funds for the Central Universities,Nankai University(63201043)for generous financial support for their programs.
文摘It has previously been shown that tryptophan, the biosynthesis precursor ofPeganum harmala alkaloids, and its derivatives have anti-TMV activity bothin vitro and in vivo. Further exploration of this led to the identification of NK0238as a highly effective agent for the prevention and control of diseases caused byplant viruses, but the existing routes are unsuitable for its large-scale synthesis.This study optimized a route for two-step synthesis of this virucide candidate viareaction of L-tryptophan with triphosgene to produce L-tryptophan-N-carboxylicanhydride, which then reacts with n-octylamine to give NK0238 at up to 94%yield and nearly 97% HPLC purity. In addition, the route was used for thepreparation of NK0238 on a > 40 g scale permitting further assessment of itsantivirus activity in the greenhouse and field experiments, and toxicity tests.NK0238 exhibited useful antiviral activities against a variety of viruses both ingreenhouse and field experiments. The toxicity tests showed that NK0238 wasnot acutely toxic to birds, fish, honey bees and silkworms. The optimized routeprovides a solid foundation for its large-scale synthesis and subsequent efficacyand toxicity studies, its excellent activity and safety make NK0238 a promisingdrug candidate for further development.
基金the National Natural Science Foundation of China(Nos.21977056,21732002,21672117,21602117,21772104,31760527)the Tianjin Natural Science Foundation(No.16JCZDJC32400)for generous financial support for our programs。
文摘Herein,we report the first Rh~Ⅲ-catalyzed regioselective C8 arylation of quinoline N-oxides with commercially available arylboronic acids as coupling partners.This procedure is simple,and the reaction shows perfect regioselectivity,a broad substrate scope,and isolated yields of up to 92%.We demonstrate the utility of the reaction by using it for late-stage functionalization of a fungicide.