Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impa...Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule passivation.In this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to devices.These sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated counterparts.Consequently,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect states.Perovskite solar cells (PSCs) fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency (PCE) of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun illumination.Moreover,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10(9H)-yl)butyl)p hosphonic acid (DMAcPA),the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.展开更多
Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we d...Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.展开更多
Nickel oxide/copper oxide composites are prepared. Then the composites were transferred into autoclave and thermal sinter under different temperature and different time. As-prepared composites were analyzed by XRD, an...Nickel oxide/copper oxide composites are prepared. Then the composites were transferred into autoclave and thermal sinter under different temperature and different time. As-prepared composites were analyzed by XRD, and it was concluded that with the increase of hydrothermal time, content of NiO and Ni<sub>0.75</sub>Cu<sub>0.25</sub>O increases, but particles become smaller;it would improve the electrochemical activity. By SEM images directed lower crystallinity of composites, deeper porosity and rougher surface would have better electrochemical activity. The electrochemical performance was investigated by cyclic voltametry, AC impedance and galvanostatic charge-discharge. All results show that under the condition of 150°C 30 h, the electrochemical performance is the best. The specific capacitance was 225.67 F·g<sup>-1</sup> at the charge-discharge current of 1 A·g<sup>-1</sup>.展开更多
基金National Natural Science Foundation of China (NSFC)(52273266, U2001216)Shenzhen Science and Technology Innovation Committee (20231121102401001)+2 种基金Shenzhen Key Laboratory Project (ZDSYS201602261933302)GuangdongHong Kong-Macao Joint Laboratory on Micro-Nano Manufacturing Technology (2021LSYS004)SUSTech high level special funds (G03050K002)。
文摘Widely used spin-coated nickle oxide (NiOx) based perovskite solar cells often suffer from severe interfacial reactions between the NiOxand adjacent perovskite layers due to surface defect states,which inherently impair device performance in a long-term view,even with surface molecule passivation.In this study,we developed high-quality magnetron-sputtered NiOxthin films through detailed process optimization,and compared systematically sputtered and spin-coated NiOxthin film surfaces from materials to devices.These sputtered NiOxfilms exhibit improved crystallinity,smoother surfaces,and significantly reduced Ni3+or Ni vacancies compared to their spin-coated counterparts.Consequently,the interface between the perovskite and sputtered NiOxfilm shows a substantially reduced density of defect states.Perovskite solar cells (PSCs) fabricated with our optimally sputtered NiOxfilms achieved a high power conversion efficiency (PCE) of up to 19.93%and demonstrated enhanced stability,maintaining 86.2% efficiency during 500 h of maximum power point tracking under one standard sun illumination.Moreover,with the surface modification using (4-(2,7-dibromo-9,9-dimethylacridin-10(9H)-yl)butyl)p hosphonic acid (DMAcPA),the device PCE was further promoted to 23.07%,which is the highest value reported for sputtered NiOxbased PSCs so far.
基金supported by the National Nature Science Foundation of China(62504130)National Key Research and Development Program of China(2018YFB0704100)+1 种基金the Key university laboratory of highly efficient utilization of solar energy and sustainable development of Guangdong(Y01256331)the Technology Development Project of Henan Province(252102240047).
文摘Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.
文摘Nickel oxide/copper oxide composites are prepared. Then the composites were transferred into autoclave and thermal sinter under different temperature and different time. As-prepared composites were analyzed by XRD, and it was concluded that with the increase of hydrothermal time, content of NiO and Ni<sub>0.75</sub>Cu<sub>0.25</sub>O increases, but particles become smaller;it would improve the electrochemical activity. By SEM images directed lower crystallinity of composites, deeper porosity and rougher surface would have better electrochemical activity. The electrochemical performance was investigated by cyclic voltametry, AC impedance and galvanostatic charge-discharge. All results show that under the condition of 150°C 30 h, the electrochemical performance is the best. The specific capacitance was 225.67 F·g<sup>-1</sup> at the charge-discharge current of 1 A·g<sup>-1</sup>.
