Pt-based catalysts are widely used in propane dehydrogenation reaction for the production of propylene.Suppressing irreversible deactivation caused by the sintering of Pt particles under harsh conditions and regenerat...Pt-based catalysts are widely used in propane dehydrogenation reaction for the production of propylene.Suppressing irreversible deactivation caused by the sintering of Pt particles under harsh conditions and regeneration process is a significant challenge in this catalyst.Herein,a series of highly ordered mesoporous Al_(2)O_(3) supports with different levels of Al3+penta sites,are fabricated and used as the support to disperse Pt-Sn_(2) clusters.Characterizations of Pt-Sn_(2)/meso-Al_(2)O_(3) with XRD,NMR,CO-IR,STEM,TG,and Raman techniques along with propane dehydrogenation-regeneration cycles test reveal the structure-stability-re generability relationship.The coordinatively unsaturated pentacoordinate Al_(Al3+penta)^(3+)can strongly anchor Pt atoms via a formation of Al-O-Pt bond,and thus stabilize the Pt-based particles at the surface of Al_(2)O_(3).The stability and regenerability of Pt-Sn2/meso-Al_(2)O_(3) are strongly dependent on the content of Al3+penta sites in the Al_(2)O_(3) structure,and a high level of Al3+penta sites can effectively prevent the agglomeration of Pt-Sn2 clusters into large Pt nanoparticles in the consecutive dehydrogenation-regeneration cycles.The Pt-Sn2/meso-Al_(2)O_(3)-600 with the highest level of Al_(penta)^(3+) (50.8%)delivers the best performance in propane dehydrogenation,which exhibits propane conversion of 40%and propylene selectivity above 98%at 570℃ with 10 vol%C_(3)H_(8) and 10 vol% H_(2) feed.A slow deactivation in this catalyst is ascribed to the formation of coke,and the catalytic performance can be fully restored in the consecutive dehydrogenation-regeneration cycles via a simple calcination treatment.展开更多
A series of PtSn/hierarchical ZSM-5 catalysts were developed for propane dehydrogenation,in which the PtSn bimetallic particles are confined in the mesopores of hierarchical ZSM-5 zeolite.The synthesis of PtSn/hierarc...A series of PtSn/hierarchical ZSM-5 catalysts were developed for propane dehydrogenation,in which the PtSn bimetallic particles are confined in the mesopores of hierarchical ZSM-5 zeolite.The synthesis of PtSn/hierarchical ZSM-5 catalysts was achieved via the loading of Pt and Sn species onto the hierarchical ZSM-5 catalysts that are obtained through a desilication of conventional ZSM-5.The PtSn/hierarchical ZSM-5 catalysts were fully characterized by XRD,N_(2) adsorption,STEM,XPS,and CO-IR techniques,which reveals that highly dispersed PtSn bimetallic nanoparticles are enclosed into mesopores of hierarchical ZSM-5.The catalytic performance of PtSn/hierarchical ZSM-5 is greatly affected by the concentrations of alkali solution in the desilication process and Sn/Pt ratios in PtSn bimetallic particles.The PtSn1.00/ZSM-5(0.8)catalyst shows the highest efficiency in propane dehydrogenation,which gives an initial conversion of 46%and selectivity of 98%at 570℃.The high efficiency in these PtSn/hierarchical ZSM-5 catalysts for propane dehydrogenation is mainly ascribed to the confinement of PtSn particles in the mesopores of hierarchical ZSM-5 zeolite.展开更多
Morphology is of great significance to the performance of organic solar cells(OSCs),since appropriate morphology could not only promote the exciton dissociation,but also reduce the charge recombination.In this work,we...Morphology is of great significance to the performance of organic solar cells(OSCs),since appropriate morphology could not only promote the exciton dissociation,but also reduce the charge recombination.In this work,we have developed a solid additive-assisted layer-by-layer(SAA-LBL)processing to fabricate high-efficiency OSCs.By adding the solid additive of fatty acid(FA)into polymer donor PM6 solution,controllable pre-phase separation forms between PM6 and FA.This intermixed morphology facilitates the diffusion of acceptor Y6 into the donor PM6 during the LBL processing,due to the good miscibility and fast-solvation of the FA with chloroform solution dripping.Interestingly,this results in the desired morphology with refined phase-separated domain and vertical phase-separation structure to better balance the charge transport/collection and exciton dissociation.Consequently,the binary single junction OSCs based on PM6:Y6 blend reach champion power conversion efficiency(PCE)of 18.16%with SAA-LBL processing,which can be generally applicable to diverse systems,e.g.,the PM6:L8-BO-based devices and thick-film devices.The efficacy of SAA-LBL is confirmed in binary OSCs based on PM6:L8-BO,where record PCEs of 19.02%and 16.44%are realized for devices with 100 and 250 nm active layers,respectively.The work provides a simple but effective way to control the morphology for high-efficiency OSCs and demonstrates the SAA-LBL processing a promising methodology for boosting the industrial manufacturing of OSCs.展开更多
Using poly(amic acid)(PAA)as a precursor followed by thermal imidization,the polyimide/barium titanate composite films were successfully prepared by a direct mixing method and in situ process.The influence of processi...Using poly(amic acid)(PAA)as a precursor followed by thermal imidization,the polyimide/barium titanate composite films were successfully prepared by a direct mixing method and in situ process.The influence of processing factors,such as particle size,distribution mode and polymerization method on dielectric prop-erties was studied.Results revealed that the dielectric constant(ε)of the composite film increased by using bigger fillers or employing in situ polymerization and bimodal distribution.When the composite film contain-ing 50 Vol-%of BaTiO3 with size in 100 nm was pre-pared via in situ process,its dielectric constant reached 45 at 10 kHz.展开更多
基金Financial supports of the National Natural Science Foundation of China(21878050,91934301)the State Key Laboratory of Coal Conversion(J21-22-620)the 111 Project(D17005)。
文摘Pt-based catalysts are widely used in propane dehydrogenation reaction for the production of propylene.Suppressing irreversible deactivation caused by the sintering of Pt particles under harsh conditions and regeneration process is a significant challenge in this catalyst.Herein,a series of highly ordered mesoporous Al_(2)O_(3) supports with different levels of Al3+penta sites,are fabricated and used as the support to disperse Pt-Sn_(2) clusters.Characterizations of Pt-Sn_(2)/meso-Al_(2)O_(3) with XRD,NMR,CO-IR,STEM,TG,and Raman techniques along with propane dehydrogenation-regeneration cycles test reveal the structure-stability-re generability relationship.The coordinatively unsaturated pentacoordinate Al_(Al3+penta)^(3+)can strongly anchor Pt atoms via a formation of Al-O-Pt bond,and thus stabilize the Pt-based particles at the surface of Al_(2)O_(3).The stability and regenerability of Pt-Sn2/meso-Al_(2)O_(3) are strongly dependent on the content of Al3+penta sites in the Al_(2)O_(3) structure,and a high level of Al3+penta sites can effectively prevent the agglomeration of Pt-Sn2 clusters into large Pt nanoparticles in the consecutive dehydrogenation-regeneration cycles.The Pt-Sn2/meso-Al_(2)O_(3)-600 with the highest level of Al_(penta)^(3+) (50.8%)delivers the best performance in propane dehydrogenation,which exhibits propane conversion of 40%and propylene selectivity above 98%at 570℃ with 10 vol%C_(3)H_(8) and 10 vol% H_(2) feed.A slow deactivation in this catalyst is ascribed to the formation of coke,and the catalytic performance can be fully restored in the consecutive dehydrogenation-regeneration cycles via a simple calcination treatment.
基金supports of the National Natural Science Foundation of China(21878050,22178062)Foundation of State Key Labora-tory of Coal Conversion(J21-22-620)Green Petrochemical Engineering Base of Intelligence Introduction for Innovation(111 Project D17005)are gratefully acknowledged.
文摘A series of PtSn/hierarchical ZSM-5 catalysts were developed for propane dehydrogenation,in which the PtSn bimetallic particles are confined in the mesopores of hierarchical ZSM-5 zeolite.The synthesis of PtSn/hierarchical ZSM-5 catalysts was achieved via the loading of Pt and Sn species onto the hierarchical ZSM-5 catalysts that are obtained through a desilication of conventional ZSM-5.The PtSn/hierarchical ZSM-5 catalysts were fully characterized by XRD,N_(2) adsorption,STEM,XPS,and CO-IR techniques,which reveals that highly dispersed PtSn bimetallic nanoparticles are enclosed into mesopores of hierarchical ZSM-5.The catalytic performance of PtSn/hierarchical ZSM-5 is greatly affected by the concentrations of alkali solution in the desilication process and Sn/Pt ratios in PtSn bimetallic particles.The PtSn1.00/ZSM-5(0.8)catalyst shows the highest efficiency in propane dehydrogenation,which gives an initial conversion of 46%and selectivity of 98%at 570℃.The high efficiency in these PtSn/hierarchical ZSM-5 catalysts for propane dehydrogenation is mainly ascribed to the confinement of PtSn particles in the mesopores of hierarchical ZSM-5 zeolite.
基金supported by the National Key Research and Development Program of China(No.2019YFA0705900)the National Natural Science Foundation of China(Nos.52127806,52173185,21734008,and 61721005)+1 种基金the Fundamental Research Funds for the Central Universities(No.226-2022-00133 and No.226-2022-00209)research start up fund from Zhejiang University。
文摘Morphology is of great significance to the performance of organic solar cells(OSCs),since appropriate morphology could not only promote the exciton dissociation,but also reduce the charge recombination.In this work,we have developed a solid additive-assisted layer-by-layer(SAA-LBL)processing to fabricate high-efficiency OSCs.By adding the solid additive of fatty acid(FA)into polymer donor PM6 solution,controllable pre-phase separation forms between PM6 and FA.This intermixed morphology facilitates the diffusion of acceptor Y6 into the donor PM6 during the LBL processing,due to the good miscibility and fast-solvation of the FA with chloroform solution dripping.Interestingly,this results in the desired morphology with refined phase-separated domain and vertical phase-separation structure to better balance the charge transport/collection and exciton dissociation.Consequently,the binary single junction OSCs based on PM6:Y6 blend reach champion power conversion efficiency(PCE)of 18.16%with SAA-LBL processing,which can be generally applicable to diverse systems,e.g.,the PM6:L8-BO-based devices and thick-film devices.The efficacy of SAA-LBL is confirmed in binary OSCs based on PM6:L8-BO,where record PCEs of 19.02%and 16.44%are realized for devices with 100 and 250 nm active layers,respectively.The work provides a simple but effective way to control the morphology for high-efficiency OSCs and demonstrates the SAA-LBL processing a promising methodology for boosting the industrial manufacturing of OSCs.
基金the National Natural Science Foundation of China(Grant No.50103010)the Education Department of Zhejiang Province(No.20071157)for supporting this work.
文摘Using poly(amic acid)(PAA)as a precursor followed by thermal imidization,the polyimide/barium titanate composite films were successfully prepared by a direct mixing method and in situ process.The influence of processing factors,such as particle size,distribution mode and polymerization method on dielectric prop-erties was studied.Results revealed that the dielectric constant(ε)of the composite film increased by using bigger fillers or employing in situ polymerization and bimodal distribution.When the composite film contain-ing 50 Vol-%of BaTiO3 with size in 100 nm was pre-pared via in situ process,its dielectric constant reached 45 at 10 kHz.