Conjugated covalent organic frameworks(COFs)hold great promise in photocatalytic hydrogen evolution owing to their high crystallinity,large surface area,and distinct structure.However,COFs exhibit poor charge separati...Conjugated covalent organic frameworks(COFs)hold great promise in photocatalytic hydrogen evolution owing to their high crystallinity,large surface area,and distinct structure.However,COFs exhibit poor charge separation.Therefore,investigating highly effective COF-based photocatalysts is crucial.For the first time,conjugated COF/perylene diimide urea polymer(PUP)all-organic heterostructure with S-scheme interfacial charge-transfer channels was successfully developed and manufactured via in situ coupling of the two-dimensional triazine-based imine-linked COF(denoted as TATF-COF)with PUP.The optimal photocatalytic hydrogen-evolution rate of 94.5 mmol h^(-1) g^(-1) for TATF-COF/PUP is 3.5 times that of pure TATF-COF and is comparable to or even higher than that of the previously reported COF-based photocatalysts,resulting in an apparent quantum efficiency of up to 19.7%at 420 nm.The improved directional S-scheme charge transfer driven by the tuned built-in electric field and enhanced oxidation and reduction reaction rates of the photogenerated carriers contribute synergistically to the boosted photocatalytic H_(2) evolution.Experiments and theoretical studies reveal plausible H_(2) evolution and spatial S-scheme charge-separation mechanisms under visible-light irradiation.This study provides advanced methods for constructing all-organic S-scheme high-efficiency photocatalysts by the modulation of band structures.展开更多
We report the plasmon-enhanced polymer bulk-heterojunction solar cells with Ag nanoparticles (AgNPs) obtained via chemical method. Here, the AgNPs films with different particle densities are introduced between the pol...We report the plasmon-enhanced polymer bulk-heterojunction solar cells with Ag nanoparticles (AgNPs) obtained via chemical method. Here, the AgNPs films with different particle densities are introduced between the poly (3,4-ethylene dioxythiophene) poly (styrenesulfonate) (PEDOT: PSS) buffer layer and the poly (3-hexythiophene):[6,6]-phenyl-c61 butyric acid methyl ester (P3HT: PCBM) layer. By improving the optical absorption of the active layer owing to the localized surface plasmons, the power conversion efficiency of the solar cells is increased compared with the control device. It is shown that the efficiency of the device increases with the density of AgNPs. For the device employing higher density, the resulted power conversion efficiency is found to increase from 2.89% to 3.38%, enhanced by 16.96%.展开更多
High interfacial energy Li^(0)-electrolyte interface contributes to larger Li^(0) nucleation embryos and a more stable interface,so the interfacial energy is essential for highly reversible Li^(0) deposition/stripping...High interfacial energy Li^(0)-electrolyte interface contributes to larger Li^(0) nucleation embryos and a more stable interface,so the interfacial energy is essential for highly reversible Li^(0) deposition/stripping.Herein,a high interfacial-energy artificial solid electrolyte interphase(SEI)with rich LiF embedded in lithiated poly-2-acrylamido-2-methylpropane sulfonic acid(PAMPS-Li)network is designed to realize favorable Li^(0) nucleation and rapid desolvation of Li+simultaneously.The Li-F bonds in LiF(001)exhibit stronger ion-dipole interactions with Li atoms,offering higher interfacial energies.When the growth surface energy and total interfacial energy of Li^(0) are balanced,the high interfacial energy SEI with abundant LiF can promote the formation of larger Li^(0) nucleation embryos.In addition,the PAMPS-Li with immobilized anions presents weaker interaction with Li^(0) and possesses higher polymer-Li interfacial energy,and its amide and sulfonic acid groups exhibit higher binding energies with Li^(+).Therefore,PAMPS-Li can easily promote the Li+to escape from the solvent sheath and weaken the desolvation energy barrier.The highly reversible Li^(0) deposition behavior with restricted side reactions is achieved based on the synergistic modification of high interfacial energy SEI with heterostructure.Most importantly,lifespan of multi-layered Li^(0) pouch cell(330 Wh kg-1)with a low N/P ratio(1.67)is over 100 cycles,verifying its potential practical application.展开更多
The surface plasmonic effect and scattering effect of gold nanorods(AuNRs) on the performance of bulk heterojunction photovoltaic devices based on the blend of polythiophene and fullerene are investigated.AuNRs enhanc...The surface plasmonic effect and scattering effect of gold nanorods(AuNRs) on the performance of bulk heterojunction photovoltaic devices based on the blend of polythiophene and fullerene are investigated.AuNRs enhance the excitation since the plasmonic effect increases the electric field,mainly in the area near the interface between the active layer and AuNRs.The results show that the incident photo-to-electron conversion efficiency(IPCE) obviously increases for the device with a layer of gold nanorods,resulting from the plasmonic effect of AuNRs in the range of 500-670 nm and the scattering effect in the range of 370-410 nm.The power conversion efficiency(PCE) is increased by 7.6% due to the near field effect of the localized surface plasmons(LSP) of AuNRs and the scattering effect.The short circuit current density is also increased by 9.1% owing to the introduction of AuNRs.However,AuNRs can cause a little deterioration in open circuit voltage.展开更多
文摘Conjugated covalent organic frameworks(COFs)hold great promise in photocatalytic hydrogen evolution owing to their high crystallinity,large surface area,and distinct structure.However,COFs exhibit poor charge separation.Therefore,investigating highly effective COF-based photocatalysts is crucial.For the first time,conjugated COF/perylene diimide urea polymer(PUP)all-organic heterostructure with S-scheme interfacial charge-transfer channels was successfully developed and manufactured via in situ coupling of the two-dimensional triazine-based imine-linked COF(denoted as TATF-COF)with PUP.The optimal photocatalytic hydrogen-evolution rate of 94.5 mmol h^(-1) g^(-1) for TATF-COF/PUP is 3.5 times that of pure TATF-COF and is comparable to or even higher than that of the previously reported COF-based photocatalysts,resulting in an apparent quantum efficiency of up to 19.7%at 420 nm.The improved directional S-scheme charge transfer driven by the tuned built-in electric field and enhanced oxidation and reduction reaction rates of the photogenerated carriers contribute synergistically to the boosted photocatalytic H_(2) evolution.Experiments and theoretical studies reveal plausible H_(2) evolution and spatial S-scheme charge-separation mechanisms under visible-light irradiation.This study provides advanced methods for constructing all-organic S-scheme high-efficiency photocatalysts by the modulation of band structures.
基金supported by the Project of Tianjin Ministry of Education (No. 20100723)the National Natural Science Foundation of China (No. 60876046)
文摘We report the plasmon-enhanced polymer bulk-heterojunction solar cells with Ag nanoparticles (AgNPs) obtained via chemical method. Here, the AgNPs films with different particle densities are introduced between the poly (3,4-ethylene dioxythiophene) poly (styrenesulfonate) (PEDOT: PSS) buffer layer and the poly (3-hexythiophene):[6,6]-phenyl-c61 butyric acid methyl ester (P3HT: PCBM) layer. By improving the optical absorption of the active layer owing to the localized surface plasmons, the power conversion efficiency of the solar cells is increased compared with the control device. It is shown that the efficiency of the device increases with the density of AgNPs. For the device employing higher density, the resulted power conversion efficiency is found to increase from 2.89% to 3.38%, enhanced by 16.96%.
基金supported by the National Natural Science Foundation of China(22109030 and 21875195)Guangdong Basic and Applied Basic Research Foundation(2019A1515111069 and 2021A1515010177)the Key Research and Development Program of Yunnan Province(202103AA080019)。
文摘High interfacial energy Li^(0)-electrolyte interface contributes to larger Li^(0) nucleation embryos and a more stable interface,so the interfacial energy is essential for highly reversible Li^(0) deposition/stripping.Herein,a high interfacial-energy artificial solid electrolyte interphase(SEI)with rich LiF embedded in lithiated poly-2-acrylamido-2-methylpropane sulfonic acid(PAMPS-Li)network is designed to realize favorable Li^(0) nucleation and rapid desolvation of Li+simultaneously.The Li-F bonds in LiF(001)exhibit stronger ion-dipole interactions with Li atoms,offering higher interfacial energies.When the growth surface energy and total interfacial energy of Li^(0) are balanced,the high interfacial energy SEI with abundant LiF can promote the formation of larger Li^(0) nucleation embryos.In addition,the PAMPS-Li with immobilized anions presents weaker interaction with Li^(0) and possesses higher polymer-Li interfacial energy,and its amide and sulfonic acid groups exhibit higher binding energies with Li^(+).Therefore,PAMPS-Li can easily promote the Li+to escape from the solvent sheath and weaken the desolvation energy barrier.The highly reversible Li^(0) deposition behavior with restricted side reactions is achieved based on the synergistic modification of high interfacial energy SEI with heterostructure.Most importantly,lifespan of multi-layered Li^(0) pouch cell(330 Wh kg-1)with a low N/P ratio(1.67)is over 100 cycles,verifying its potential practical application.
基金supported by the National Natural Science Foundation of China (Grant Nos. 61275175,61036007,61125505 and 60978061)Program for New Century Excellent Talents in University (Grant No.NCET-08-0717)+1 种基金National Science Foundation for Distinguished Young Scholars of China (Grant No. 61125505)the 111 Project of China(Grant No. B08002)
文摘The surface plasmonic effect and scattering effect of gold nanorods(AuNRs) on the performance of bulk heterojunction photovoltaic devices based on the blend of polythiophene and fullerene are investigated.AuNRs enhance the excitation since the plasmonic effect increases the electric field,mainly in the area near the interface between the active layer and AuNRs.The results show that the incident photo-to-electron conversion efficiency(IPCE) obviously increases for the device with a layer of gold nanorods,resulting from the plasmonic effect of AuNRs in the range of 500-670 nm and the scattering effect in the range of 370-410 nm.The power conversion efficiency(PCE) is increased by 7.6% due to the near field effect of the localized surface plasmons(LSP) of AuNRs and the scattering effect.The short circuit current density is also increased by 9.1% owing to the introduction of AuNRs.However,AuNRs can cause a little deterioration in open circuit voltage.