Carbazole moiety-based 2PACz([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)self-assembled monolayers(SAMs)are excellent hole-selective contact(HSC)materials with abilities to excel the charge-transferdynamics of perovski...Carbazole moiety-based 2PACz([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)self-assembled monolayers(SAMs)are excellent hole-selective contact(HSC)materials with abilities to excel the charge-transferdynamics of perovskite solar cells(PSCs).Herein,we report a facile but powerful method to functionalize the surface of 2PACz-SAM,by which reproducible,highly stable,high-efficiency wide-bandgap PSCs can be obtained.The 2PACz surface treatment with various donor number solvents improves assembly of 2PACz-SAM and leave residual surface-bound solvent molecules on 2PACz-SAM,which increases perovskite grain size,retards halide segregation,and accelerates hole extraction.The surface functionalization achieves a high power conversion efficiency(PCE)of 17.62%for a single-junction wide-bandgap(~1.77 e V)PSC.We also demonstrate a monolithic all-perovskite tandem solar cell using surfaceengineered HSC,showing high PCE of 24.66%with large open-circuit voltage of 2.008 V and high fillfactor of 81.45%.Our results suggest this simple approach can further improve the tandem device,when coupled with a high-performance narrow-bandgap sub-cell.展开更多
The conversion of methane to olefins,aromatics,and hydrogen(MTOAH)can be used to stably obtain hydrocarbons when the effect of the catalytic surface is optimized from the reaction engineering perspective.In this study...The conversion of methane to olefins,aromatics,and hydrogen(MTOAH)can be used to stably obtain hydrocarbons when the effect of the catalytic surface is optimized from the reaction engineering perspective.In this study,Fe/Si C catalysts were packed into a quartz tube reactor.The catalytic surfaces of Si C and the impregnated Fe species decreased the apparent activation energies(E_a)of methane consumption in the blank reactor between 965 and 1020℃.Consequently,the hydrocarbon yield increased by 2.4times at 1020℃.Based on the model reactions of ethane,ethylene,and acetylene mixed with hydrogen in the range of 500-1020℃,an excess amount of Fe in the reactor favored the C-C coupling reaction over the selective hydrogenation of acetylene;consequently,coke formation was favored over the hydrogenation reaction.The gas-phase reactions and catalyst properties were optimized to increase hydrocarbon yields while reducing coke selectivity.The 0.2Fe catalyst-packed reactor(0.26 wt%Fe)resulted in a hydrocarbon yield of 7.1%and a coke selectivity of<2%when the ratio of the void space of the postcatalyst zone to the catalyst space was adjusted to be≥2.Based on these findings,the facile approach of decoupling the reaction zone between the catalyst surface and the gas-phase reaction can provide insights into catalytic reactor design,thereby facilitating the scale-up from the laboratory to the commercial scale.展开更多
基金supported by the National Research Foundation of Korea (NRF)the Ministry of Science,ICT (2022M3J1A1085285,2019R1A2C1084010,and 2022R1A2C2006532)the Korea Electric Power Corporation (R20XO02-1)。
文摘Carbazole moiety-based 2PACz([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)self-assembled monolayers(SAMs)are excellent hole-selective contact(HSC)materials with abilities to excel the charge-transferdynamics of perovskite solar cells(PSCs).Herein,we report a facile but powerful method to functionalize the surface of 2PACz-SAM,by which reproducible,highly stable,high-efficiency wide-bandgap PSCs can be obtained.The 2PACz surface treatment with various donor number solvents improves assembly of 2PACz-SAM and leave residual surface-bound solvent molecules on 2PACz-SAM,which increases perovskite grain size,retards halide segregation,and accelerates hole extraction.The surface functionalization achieves a high power conversion efficiency(PCE)of 17.62%for a single-junction wide-bandgap(~1.77 e V)PSC.We also demonstrate a monolithic all-perovskite tandem solar cell using surfaceengineered HSC,showing high PCE of 24.66%with large open-circuit voltage of 2.008 V and high fillfactor of 81.45%.Our results suggest this simple approach can further improve the tandem device,when coupled with a high-performance narrow-bandgap sub-cell.
基金supported by the C1 Gas Refinery Program through the National Research Foundation of Korea (NRF)funded by the Ministry of Science,ICT&Future Planning (NRF2017M3D3A1A01037001)supported by the Ministry of Trade,Industry and Energy (MOTIE),Korea Institute for Advancement of Technology (KIAT)through the Virtual Engineering Platform Program (P0022334)。
文摘The conversion of methane to olefins,aromatics,and hydrogen(MTOAH)can be used to stably obtain hydrocarbons when the effect of the catalytic surface is optimized from the reaction engineering perspective.In this study,Fe/Si C catalysts were packed into a quartz tube reactor.The catalytic surfaces of Si C and the impregnated Fe species decreased the apparent activation energies(E_a)of methane consumption in the blank reactor between 965 and 1020℃.Consequently,the hydrocarbon yield increased by 2.4times at 1020℃.Based on the model reactions of ethane,ethylene,and acetylene mixed with hydrogen in the range of 500-1020℃,an excess amount of Fe in the reactor favored the C-C coupling reaction over the selective hydrogenation of acetylene;consequently,coke formation was favored over the hydrogenation reaction.The gas-phase reactions and catalyst properties were optimized to increase hydrocarbon yields while reducing coke selectivity.The 0.2Fe catalyst-packed reactor(0.26 wt%Fe)resulted in a hydrocarbon yield of 7.1%and a coke selectivity of<2%when the ratio of the void space of the postcatalyst zone to the catalyst space was adjusted to be≥2.Based on these findings,the facile approach of decoupling the reaction zone between the catalyst surface and the gas-phase reaction can provide insights into catalytic reactor design,thereby facilitating the scale-up from the laboratory to the commercial scale.