The pyrolysis under inert atmosphere has been widely used for the synthesis of metal containing heteroatoms doped carbon materials, versatile catalysts for various reactions. However, it is difficult to prevent metal ...The pyrolysis under inert atmosphere has been widely used for the synthesis of metal containing heteroatoms doped carbon materials, versatile catalysts for various reactions. However, it is difficult to prevent metal nanoparticles aggregation during pyrolysis process. Herein, we reported the efficient synthesis of nitrogen doped carbon hollow nanospheres with cobalt nanoparticles （Co NP, ca. 10nm in size） distributed uniformly in the shell via pyrolysis of yolk-shell structured Zn-Co-ZIFs@polydopamine （PDA）. PDA acted as both protection layer and carbon source, which successfully prevented the aggregation of cobalt nanoparticles during high-temperature pyrolysis process. The Co NP and N containing carbon （Co NP/NC） hollow nanospheres were active for both oxygen evolution reaction （OER） and oxygen reduction reaction （ORR）, affording overpotential of 430 mV at 10 mA/cm2 for OER in 1 M KOH and comparable half-wave potential to that of Pt/C （0.80V vs RHE） for ORR in 0.1 M KOH. The superior performance of carbon hollow nanospheres for both OER and ORR was mainly attributed to its small metal nanoparticles, N-doping and hollow nanostructure. The protection and confinement effect that originated from PDA coating strategy could be extended to the synthesis of other hollow structured carbon materials, especially the ones with small metal nanoparticles.展开更多
The practical application of energetic materials, particularly 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20), is frequently impeded by phase transition challenges. In this study, we propose a novel...The practical application of energetic materials, particularly 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20), is frequently impeded by phase transition challenges. In this study, we propose a novel strategy to enhance the stability of CL-20 by employing a thermo-sensitive polymer,poly(N-isopropylacrylamide)(PNIPAM), to modulate its phase transitions. Our approach involves the use of an in-situ polymerized polydopamine(PDA) shell as a platform for surface grafting through atom transfer radical polymerization, yielding a core-shell structured CL-20@PDA-PNIPAM. Through comprehensive characterization, the successful grafting of PNIPAM is confirmed, significantly enhanced the phase stability of CL-20. Notably, our core-shell structure exhibits a 13℃ increase in phase transition temperature compared to raw CL-20, thereby delaying the ε→a phase transition by over 80 min under combined thermal and solvent conditions. The enhanced stability is attributed to the hydrophobic nature of PNIPAM above its low critical solution temperature in water, which effectively shields the CL-20 crystal. These findings provide new insights into enhancing the stability and safety of energetic materials in complex environments, highlighting the potential of our molecular switch mechanism.展开更多
As a renewable and environment-friendly technology for seawater desalination and wastewater purification,solar energy triggered steam generation is attractive to address the long-standing global water scarcity issues....As a renewable and environment-friendly technology for seawater desalination and wastewater purification,solar energy triggered steam generation is attractive to address the long-standing global water scarcity issues.However,practical utilization of solar energy for steam generation is severely restricted by the complex synthesis,low energy conversion efficiency,insufficient solar spectrum absorption and water extraction capability of state-of-the-art technologies.Here,for the first time,we report a facile strategy to realize hydrogen bond induced self-assembly of a polydopamine(PDA)@MXene microsphere photothermal layer for synergistically achieving wide-spectrum and highly efficient solar absorption capability(≈96%in a wide solar spectrum range of 250–1,500 nm wavelength).Moreover,such a system renders fast water transport and vapor escaping due to the intrinsically hydrophilic nature of both MXene and PDA,as well as the interspacing between core-shell microspheres.The solar-to-vapor conversion efficiencies under the solar illumination of 1 sun and 4 sun are as high as 85.2%and 93.6%,respectively.Besides,the PDA@MXene photothermal layer renders the system durable mechanical properties,allowing producing clean water from seawater with the salt rejection rate beyond 99%.Furthermore,stable light absorption performance can be achieved and well maintained due to the formation of ternary TiO2/C/MXene complex caused by oxidative degradation of MXene.Therefore,this work proposes an attractive MXene-assisted strategy for fabricating high performance photothermal composites for advanced solar-driven seawater desalination applications.展开更多
文摘The pyrolysis under inert atmosphere has been widely used for the synthesis of metal containing heteroatoms doped carbon materials, versatile catalysts for various reactions. However, it is difficult to prevent metal nanoparticles aggregation during pyrolysis process. Herein, we reported the efficient synthesis of nitrogen doped carbon hollow nanospheres with cobalt nanoparticles （Co NP, ca. 10nm in size） distributed uniformly in the shell via pyrolysis of yolk-shell structured Zn-Co-ZIFs@polydopamine （PDA）. PDA acted as both protection layer and carbon source, which successfully prevented the aggregation of cobalt nanoparticles during high-temperature pyrolysis process. The Co NP and N containing carbon （Co NP/NC） hollow nanospheres were active for both oxygen evolution reaction （OER） and oxygen reduction reaction （ORR）, affording overpotential of 430 mV at 10 mA/cm2 for OER in 1 M KOH and comparable half-wave potential to that of Pt/C （0.80V vs RHE） for ORR in 0.1 M KOH. The superior performance of carbon hollow nanospheres for both OER and ORR was mainly attributed to its small metal nanoparticles, N-doping and hollow nanostructure. The protection and confinement effect that originated from PDA coating strategy could be extended to the synthesis of other hollow structured carbon materials, especially the ones with small metal nanoparticles.
基金supported by National Natural Science Foundation of China(Grant Nos.U2130207,21875232,12372342)Foundation of President of China Academy of Engineering Physics(Grant Nos.YZJJZQ2023008,YZJJZQ2022006)the Foundation of China Academy of Engineering Physics(Grant Nos.CX20210015,CX20210027)。
文摘The practical application of energetic materials, particularly 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane(CL-20), is frequently impeded by phase transition challenges. In this study, we propose a novel strategy to enhance the stability of CL-20 by employing a thermo-sensitive polymer,poly(N-isopropylacrylamide)(PNIPAM), to modulate its phase transitions. Our approach involves the use of an in-situ polymerized polydopamine(PDA) shell as a platform for surface grafting through atom transfer radical polymerization, yielding a core-shell structured CL-20@PDA-PNIPAM. Through comprehensive characterization, the successful grafting of PNIPAM is confirmed, significantly enhanced the phase stability of CL-20. Notably, our core-shell structure exhibits a 13℃ increase in phase transition temperature compared to raw CL-20, thereby delaying the ε→a phase transition by over 80 min under combined thermal and solvent conditions. The enhanced stability is attributed to the hydrophobic nature of PNIPAM above its low critical solution temperature in water, which effectively shields the CL-20 crystal. These findings provide new insights into enhancing the stability and safety of energetic materials in complex environments, highlighting the potential of our molecular switch mechanism.
基金supported by the National Natural Science Foundation of China(Nos.51873126,51422305,and 51721091)。
文摘As a renewable and environment-friendly technology for seawater desalination and wastewater purification,solar energy triggered steam generation is attractive to address the long-standing global water scarcity issues.However,practical utilization of solar energy for steam generation is severely restricted by the complex synthesis,low energy conversion efficiency,insufficient solar spectrum absorption and water extraction capability of state-of-the-art technologies.Here,for the first time,we report a facile strategy to realize hydrogen bond induced self-assembly of a polydopamine(PDA)@MXene microsphere photothermal layer for synergistically achieving wide-spectrum and highly efficient solar absorption capability(≈96%in a wide solar spectrum range of 250–1,500 nm wavelength).Moreover,such a system renders fast water transport and vapor escaping due to the intrinsically hydrophilic nature of both MXene and PDA,as well as the interspacing between core-shell microspheres.The solar-to-vapor conversion efficiencies under the solar illumination of 1 sun and 4 sun are as high as 85.2%and 93.6%,respectively.Besides,the PDA@MXene photothermal layer renders the system durable mechanical properties,allowing producing clean water from seawater with the salt rejection rate beyond 99%.Furthermore,stable light absorption performance can be achieved and well maintained due to the formation of ternary TiO2/C/MXene complex caused by oxidative degradation of MXene.Therefore,this work proposes an attractive MXene-assisted strategy for fabricating high performance photothermal composites for advanced solar-driven seawater desalination applications.
