Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium ...Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.展开更多
The ultra-deep desulfurization of oil needs to be solved urgently due to various problems,including environmental pollution and environmental protection requirements.Oxidative desulfurization(ODS)was considered to be ...The ultra-deep desulfurization of oil needs to be solved urgently due to various problems,including environmental pollution and environmental protection requirements.Oxidative desulfurization(ODS)was considered to be the most promising technology.The facile synthesis of highly efficient and stable HPW-based heterogeneous catalysts for oxidative desulfurization is still a challenging task.In this paper,pentamethylene hexamine(PEHA)and phosphotungstic acid(HPW)were combined by a simple one-step method to prepare a heterogeneous catalyst of PEHA-HPW for the production of ultra-deep desulfurization fuel oil.The composite material exhibited excellent catalytic activity and high recyclability,which could reach a 100% dibenzothiophene(DBT)removal rate in 30 min and be recycled at least 5 times.Experiments and DFT simulations were used to better examine the ODS mechanism of PEHA-HPW.It was proved that the rich amino groups on the surface of PEHA-HPW play a crucial role.This work provides a simple and feasible way for the manufacture of efficient HPW-based catalysts.展开更多
Nanovaccines have gathered significant attention for their potential to elicit tumor-specific immunological responses.Despite notable progress in tumor immunotherapy,nanovaccines still encounter considerable challenge...Nanovaccines have gathered significant attention for their potential to elicit tumor-specific immunological responses.Despite notable progress in tumor immunotherapy,nanovaccines still encounter considerable challenges such as low delivery efficiency,limited targeting ability,and suboptimal efficacy.With an aim of addressing these issues,engineering customized nanovaccines through modification or functionalization has emerged as a promising approach.These tailored nanovaccines not only enhance antigen presentation,but also effectively modulate immunosuppression within the tumor microenvironment.Specifically,they are distinguished by their diverse sizes,shapes,charges,structures,and unique physicochemical properties,along with targeting ligands.These features of nanovaccines facilitate lymph node accumulation and activation/regulation of immune cells.This overview of bespoke nanovaccines underscores their potential in both prophylactic and therapeutic applications,offering insights into their future development and role in cancer immunotherapy.展开更多
Lead halide perovskites have received tremendous attentions recently for their excellent properties such as high light absorption coefficient and long charge carrier diffusion length. However, the stability issues and...Lead halide perovskites have received tremendous attentions recently for their excellent properties such as high light absorption coefficient and long charge carrier diffusion length. However, the stability issues and the existence of toxic lead cations have largely limited their applications in optoelectronic area. Herein, we report the synthesis and investigation of highly stable and lead-free Cs3Bi2I9 perovskite nanoplates for visible light photodetection applications. The Cs3Bi2I9 nanoplates were synthesized through a facile solution-processed method, which is also applicable to various substrates. The achieved nanoplates present very good crystal quality and exhibit excellent long-term stability even exposed in moist air for several months. Photodetectors were constructed based on these high-quality perovskite nanoplates for the first time, and display a maximum photoresponsivity of 33.1 mA/W under the illumination of 450 nm laser, which is six times higher than the solution-synthesized CH3NH3PbI3 nanowire photodetectors. The specific detectivity of these devices can reach up to 10^10 Jones. Additionally, the devices exhibit fast rise and decay time of 10.2 and 37.2 ms, respectively, and highly stable photoswitching behavior with their photoresponse well retaining under alternating light and darkness. This work opens up a new opportunity for stable and low-toxic perovskite-based optoelectronic applications.展开更多
Monolayer MoS2 is a direct band gap semiconductor with large exciton binding energy,which is a promising candidate for the application of ultrathin optoelectronic devices.However,the optoelectronic performance of mono...Monolayer MoS2 is a direct band gap semiconductor with large exciton binding energy,which is a promising candidate for the application of ultrathin optoelectronic devices.However,the optoelectronic performance of monolayer M0S2 is seriously limited to its growth quality and carrier mobility.In this work,we report the direct vapor growth and the optoelectronic device of verticallystacked MoS2/MoSe2 heterostructure,and further discuss the mechanism of improved device performance.The optical and high-resolution atomic characterizations demonstrate that the heterostructure interface is of high-quality without atomic alloying.Electrical transport measurements indicate that the heterostructure transistor exhibits a high mobility of 28.5 cm^2/(V·s)and a high on/off ratio of 10^7.The optoelectronic characterizations prove that the heterostructure device presents an enhanced photoresponsivity of 36 A/W and a remarkable detectivity of 4.8×10^11 Jones,which benefited from the interface induced built-in electric field and carrier dependent Coulomb screening effect.This work demonstrates that the construction of two-dimensional(2D)semiconductor heterostructures plays a significant role in modifying the optoelectronic device properties of 2D materials.展开更多
基金supported by the National Key Research and Development Program of China(2022YFB4101800)National Natural Science Foundation of China(22278077,22108040)+2 种基金Key Program of Qingyuan Innovation Laboratory(00221004)Research Program of Qingyuan Innovation Laboratory(00523006)Natural Science Foundation of Fujian Province(2022J02019)。
文摘Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.
基金supported by the National Natural Science Foundation of China(22378065,22278077)the Fujian Province Department of Science&Technology,China(2019YZ017001)。
文摘The ultra-deep desulfurization of oil needs to be solved urgently due to various problems,including environmental pollution and environmental protection requirements.Oxidative desulfurization(ODS)was considered to be the most promising technology.The facile synthesis of highly efficient and stable HPW-based heterogeneous catalysts for oxidative desulfurization is still a challenging task.In this paper,pentamethylene hexamine(PEHA)and phosphotungstic acid(HPW)were combined by a simple one-step method to prepare a heterogeneous catalyst of PEHA-HPW for the production of ultra-deep desulfurization fuel oil.The composite material exhibited excellent catalytic activity and high recyclability,which could reach a 100% dibenzothiophene(DBT)removal rate in 30 min and be recycled at least 5 times.Experiments and DFT simulations were used to better examine the ODS mechanism of PEHA-HPW.It was proved that the rich amino groups on the surface of PEHA-HPW play a crucial role.This work provides a simple and feasible way for the manufacture of efficient HPW-based catalysts.
基金financially supported by the National Key R&D Program of China(Grant No.2022YFB3808000/2022YFB3808001,Grant No.2021YFC2400600/2021 YFC2400604)the Medical Innovation Project of Science and Technology Program of Fujian Provincial Health Commission(Grant No.2021CXA006)+1 种基金the Project for High-Level Talent Innovation and Entrepreneurship of Quanzhou(Grant No.2022C016R)the Key Program of Qingyuan Innovation Laboratory(Grant No.00221002).
文摘Nanovaccines have gathered significant attention for their potential to elicit tumor-specific immunological responses.Despite notable progress in tumor immunotherapy,nanovaccines still encounter considerable challenges such as low delivery efficiency,limited targeting ability,and suboptimal efficacy.With an aim of addressing these issues,engineering customized nanovaccines through modification or functionalization has emerged as a promising approach.These tailored nanovaccines not only enhance antigen presentation,but also effectively modulate immunosuppression within the tumor microenvironment.Specifically,they are distinguished by their diverse sizes,shapes,charges,structures,and unique physicochemical properties,along with targeting ligands.These features of nanovaccines facilitate lymph node accumulation and activation/regulation of immune cells.This overview of bespoke nanovaccines underscores their potential in both prophylactic and therapeutic applications,offering insights into their future development and role in cancer immunotherapy.
基金the National Natural Science Foundation of China (Nos.51525202, 51772084, 61574054, 61635001, and 51802089)Innovation platform and talent plan of Hunan Province (No.2017RS3027)+1 种基金the Program for Youth Leading Talent and Science and Technology Innovation of Ministry of Science and Technology of Chinathe Foundation for Innovative Research Groups of NSFC (No.21521063).
文摘Lead halide perovskites have received tremendous attentions recently for their excellent properties such as high light absorption coefficient and long charge carrier diffusion length. However, the stability issues and the existence of toxic lead cations have largely limited their applications in optoelectronic area. Herein, we report the synthesis and investigation of highly stable and lead-free Cs3Bi2I9 perovskite nanoplates for visible light photodetection applications. The Cs3Bi2I9 nanoplates were synthesized through a facile solution-processed method, which is also applicable to various substrates. The achieved nanoplates present very good crystal quality and exhibit excellent long-term stability even exposed in moist air for several months. Photodetectors were constructed based on these high-quality perovskite nanoplates for the first time, and display a maximum photoresponsivity of 33.1 mA/W under the illumination of 450 nm laser, which is six times higher than the solution-synthesized CH3NH3PbI3 nanowire photodetectors. The specific detectivity of these devices can reach up to 10^10 Jones. Additionally, the devices exhibit fast rise and decay time of 10.2 and 37.2 ms, respectively, and highly stable photoswitching behavior with their photoresponse well retaining under alternating light and darkness. This work opens up a new opportunity for stable and low-toxic perovskite-based optoelectronic applications.
基金This work is supported by the National Natural Science Foundation of China(Nos.51525202,51902098,51772084,61574054,51972105,11904098,)the Hunan Provincial N atural Science F oundation of C hina(No.2018RS3051)+1 种基金the Joint Funds of the National N atural Science Foundation of China(No.U19A2090)H unan Provincial(China)Natural Science Foundation for Excellent Young Scholars(No.2019JJ30004).
文摘Monolayer MoS2 is a direct band gap semiconductor with large exciton binding energy,which is a promising candidate for the application of ultrathin optoelectronic devices.However,the optoelectronic performance of monolayer M0S2 is seriously limited to its growth quality and carrier mobility.In this work,we report the direct vapor growth and the optoelectronic device of verticallystacked MoS2/MoSe2 heterostructure,and further discuss the mechanism of improved device performance.The optical and high-resolution atomic characterizations demonstrate that the heterostructure interface is of high-quality without atomic alloying.Electrical transport measurements indicate that the heterostructure transistor exhibits a high mobility of 28.5 cm^2/(V·s)and a high on/off ratio of 10^7.The optoelectronic characterizations prove that the heterostructure device presents an enhanced photoresponsivity of 36 A/W and a remarkable detectivity of 4.8×10^11 Jones,which benefited from the interface induced built-in electric field and carrier dependent Coulomb screening effect.This work demonstrates that the construction of two-dimensional(2D)semiconductor heterostructures plays a significant role in modifying the optoelectronic device properties of 2D materials.