Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-excha...Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline transform.Interatomic forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport channels,In addition,the partially freed Cs~+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation process.The In-aip(Cs)modified perovskite films have a flat morphology,large grains and excellent optoelectronic properties.Benefiting from the high-quality perovskite films and faster charge extraction,the In-aip(Cs)-modified PSCs achieved a champion PCE of 23.03%,superior to the In-aip-modified(22.29%)and control device(21.13%),More importantly,the unencapsulated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal stability.Over a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85%of its initial PCE after storing in a glove box at 85℃,and retained 87%of the primary PCE upon storage in ambient condition at 25℃under a humidity of 40%.展开更多
Heat accumulation inside perovskite solar cells causes the decomposition of the perovskite layer and hole transport materials(HTMs)under working conditions,yielding a decrease in long-term stability.Here,we present a ...Heat accumulation inside perovskite solar cells causes the decomposition of the perovskite layer and hole transport materials(HTMs)under working conditions,yielding a decrease in long-term stability.Here,we present a zeolite-assisted heat conduction strategy by introducing economic zeolite crystals(e.g.,NaX,NaY,and ZSM-5)as a cooling filter to induce heat diffusion.The fitted thermal diffusion kinetic equation from real-time infrared thermal imaging technology reveals the zeolite skeleton assisted thermal co nduction mechanism of internal lattice vibration.Additionally,the nearly twofold improved conductivity of the modified HTM film is benefited from Na^(+)hopping on the supercages of the zeolite,therefore,the best-performed device with a rapid heat diffusion and defect inhibition obtains a remarkable power conversion efficiency of 23.42%.Both of NaX modified sprio-OMeTAD and PTAA based devices exhibit excellent operational stability after heating 1000 h at 85℃under N_(2)condition.This work demonstrates the potential application of economical porous zeolite materials in improving the thermal stability of PSCs.展开更多
Mesoporous Ti O2/Carbon beads have been prepared via a facile impregnation-carbonization approach, in which a porous anion-exchange resin and K2 Ti O(C2O4)2were used as hard carbon and titanium source, respectively.Ch...Mesoporous Ti O2/Carbon beads have been prepared via a facile impregnation-carbonization approach, in which a porous anion-exchange resin and K2 Ti O(C2O4)2were used as hard carbon and titanium source, respectively.Characterization results reveal that the self-assembled composites have disordered mesostructure, uniform mesopores,large pore volumes, and high surface areas. The mesopore walls are composed of amorphous carbon, well-dispersed and confined anatase or rutile nanoparticles. Some anatase phase of Ti O2 was transformed to rutile phase via an increase of carbonization temperature or repeated impregnation of the resin with Ti O(C2O4)22-species. X-ray photoelectron spectroscopy, carbon, hydrogen, and nitrogen element analysis, and thermal gravity analysis results indicate the doping of carbon into the Ti O2 lattice and strong interaction between carbon and Ti O2 nanoparticles. A synergy effect by carbon and Ti O2 in the composites has been discussed herein on the degradation of methyl orange under visible light. The dye removal process involves adsorption of the dye from water by the mesopores in the composites, followed by photodegradation on the separated dye-loaded catalysts. Mesopores allow full access of the dye molecules to the surface of Ti O2 nanoparticles.Importantly, the bead format of such composite enables their straightforward separation from the reaction mixture in their application as a liquid-phase heterogeneous photodegradation catalyst.展开更多
A novel photocatalyst of mesoporous graphitic carbon nitride(g-C_3N_4) co-doped with Co and Mo(Co/Mo-MCN) has been one-pot synthesized via a simple template-free method; cobalt chloride and molybdenum disulfide were u...A novel photocatalyst of mesoporous graphitic carbon nitride(g-C_3N_4) co-doped with Co and Mo(Co/Mo-MCN) has been one-pot synthesized via a simple template-free method; cobalt chloride and molybdenum disulfide were used as the Co and Mo sources, respectively. The characterization results evidently indicate that molybdenum disulfide functions as Mo sources to incorporate Mo atoms in the framework of g-C_3N_4 and as a catalyst for promoting the decomposition of g-C_3N_4, resulting in the creation of mesopores. The obtained Co/Mo-MCN exhibited a significant enhancement of the photocatalytic activity in H_2 evolution(8.6 times) and Rhodamine B degradation(10.1 times) under visible light irradiation compared to pristine g-C_3N_4. Furthermore, density functional theory calculations were applied to further understand the photocatalytic enhancement mechanism of the optical absorption properties at the atomic level after Co-or Mo-doping. Finite-di erence time-domain simulations were performed to evaluate the e ect of the mesopore structures on the light absorption capability. The results revealed that both the bimetal doping and the mesoporous architectures resulted in an enhanced optical absorption; this phenomenon was considered to have played a critical role in the improvement in the photocatalytic performance of Co/Mo-MCN.展开更多
A novel air-stable n-type benzothiaphene endcapped azaarene(BTPQ) and its sulfonated derivative(BSPQ) were prepared via two pathways and characterized by NMR, UV–vis, fluorescence and cyclic voltammetry spectroscopy....A novel air-stable n-type benzothiaphene endcapped azaarene(BTPQ) and its sulfonated derivative(BSPQ) were prepared via two pathways and characterized by NMR, UV–vis, fluorescence and cyclic voltammetry spectroscopy. Symmetrically introducing four nitrogen atoms into acenes, the semiconductor properties could be changed from p-type to n-type detected through the space charge limited current(SCLC) method. After sulfonation of BTPQ, BSPQ is with deeper frontier orbital energy levels and enhanced the electron mobility.展开更多
基金supported by National Natural Science Foundation of China(Grant No.22001050,22072034)the China Postdoctoral Science Foundation(Grant No.2020T130147,2020M681084)+1 种基金the Postdoctoral Foundation of Heilongjiang Province(Grant No.LBH-Z19059)the Natural Science Foundation of Heilongjiang Youth Fund(Grant No.YQ2021B002)。
文摘Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline transform.Interatomic forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport channels,In addition,the partially freed Cs~+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation process.The In-aip(Cs)modified perovskite films have a flat morphology,large grains and excellent optoelectronic properties.Benefiting from the high-quality perovskite films and faster charge extraction,the In-aip(Cs)-modified PSCs achieved a champion PCE of 23.03%,superior to the In-aip-modified(22.29%)and control device(21.13%),More importantly,the unencapsulated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal stability.Over a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85%of its initial PCE after storing in a glove box at 85℃,and retained 87%of the primary PCE upon storage in ambient condition at 25℃under a humidity of 40%.
基金supported by the National Natural Science Foundation of China(22001050,22072034,21873025)the China Postdoctoral Science Foundation(2020T130147,2020M681084)+1 种基金the Postdoctoral Foundation of Heilongjiang Province(LBH-Z19059)the Natural Science Foundation of Heilongjiang Youth Fund(YQ2021B002)。
文摘Heat accumulation inside perovskite solar cells causes the decomposition of the perovskite layer and hole transport materials(HTMs)under working conditions,yielding a decrease in long-term stability.Here,we present a zeolite-assisted heat conduction strategy by introducing economic zeolite crystals(e.g.,NaX,NaY,and ZSM-5)as a cooling filter to induce heat diffusion.The fitted thermal diffusion kinetic equation from real-time infrared thermal imaging technology reveals the zeolite skeleton assisted thermal co nduction mechanism of internal lattice vibration.Additionally,the nearly twofold improved conductivity of the modified HTM film is benefited from Na^(+)hopping on the supercages of the zeolite,therefore,the best-performed device with a rapid heat diffusion and defect inhibition obtains a remarkable power conversion efficiency of 23.42%.Both of NaX modified sprio-OMeTAD and PTAA based devices exhibit excellent operational stability after heating 1000 h at 85℃under N_(2)condition.This work demonstrates the potential application of economical porous zeolite materials in improving the thermal stability of PSCs.
基金supported by Natural Science Foundation of China(21303031,21353004,51472062)Natural Science Foundation of Heilongjiang Province of China(B201010)+2 种基金Fundamental Research Funds for the Central Universities(HIT.IBRSEM.201326)Program for Science&Technology Innovation Talent in Harbin(2013RFQXJ004,2007RFXXG018)China Postdoctoral Science Foundation(2012T50334,20100480991)
文摘Mesoporous Ti O2/Carbon beads have been prepared via a facile impregnation-carbonization approach, in which a porous anion-exchange resin and K2 Ti O(C2O4)2were used as hard carbon and titanium source, respectively.Characterization results reveal that the self-assembled composites have disordered mesostructure, uniform mesopores,large pore volumes, and high surface areas. The mesopore walls are composed of amorphous carbon, well-dispersed and confined anatase or rutile nanoparticles. Some anatase phase of Ti O2 was transformed to rutile phase via an increase of carbonization temperature or repeated impregnation of the resin with Ti O(C2O4)22-species. X-ray photoelectron spectroscopy, carbon, hydrogen, and nitrogen element analysis, and thermal gravity analysis results indicate the doping of carbon into the Ti O2 lattice and strong interaction between carbon and Ti O2 nanoparticles. A synergy effect by carbon and Ti O2 in the composites has been discussed herein on the degradation of methyl orange under visible light. The dye removal process involves adsorption of the dye from water by the mesopores in the composites, followed by photodegradation on the separated dye-loaded catalysts. Mesopores allow full access of the dye molecules to the surface of Ti O2 nanoparticles.Importantly, the bead format of such composite enables their straightforward separation from the reaction mixture in their application as a liquid-phase heterogeneous photodegradation catalyst.
基金the financial support from National Natural Science Foundation of China (51472062)
文摘A novel photocatalyst of mesoporous graphitic carbon nitride(g-C_3N_4) co-doped with Co and Mo(Co/Mo-MCN) has been one-pot synthesized via a simple template-free method; cobalt chloride and molybdenum disulfide were used as the Co and Mo sources, respectively. The characterization results evidently indicate that molybdenum disulfide functions as Mo sources to incorporate Mo atoms in the framework of g-C_3N_4 and as a catalyst for promoting the decomposition of g-C_3N_4, resulting in the creation of mesopores. The obtained Co/Mo-MCN exhibited a significant enhancement of the photocatalytic activity in H_2 evolution(8.6 times) and Rhodamine B degradation(10.1 times) under visible light irradiation compared to pristine g-C_3N_4. Furthermore, density functional theory calculations were applied to further understand the photocatalytic enhancement mechanism of the optical absorption properties at the atomic level after Co-or Mo-doping. Finite-di erence time-domain simulations were performed to evaluate the e ect of the mesopore structures on the light absorption capability. The results revealed that both the bimetal doping and the mesoporous architectures resulted in an enhanced optical absorption; this phenomenon was considered to have played a critical role in the improvement in the photocatalytic performance of Co/Mo-MCN.
基金supported by Natural Science Foundation of Heilongjiang Youth Fund (No. YQ2021B002)Heilongjiang Postdoctoral Scientific Research Developmental Fund (No. LBH-Q20018)State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology)。
文摘A novel air-stable n-type benzothiaphene endcapped azaarene(BTPQ) and its sulfonated derivative(BSPQ) were prepared via two pathways and characterized by NMR, UV–vis, fluorescence and cyclic voltammetry spectroscopy. Symmetrically introducing four nitrogen atoms into acenes, the semiconductor properties could be changed from p-type to n-type detected through the space charge limited current(SCLC) method. After sulfonation of BTPQ, BSPQ is with deeper frontier orbital energy levels and enhanced the electron mobility.