Structural reconstruction of electrocatalysts plays a pivotal role in catalytic performances for CO_(2)reduction reaction(CO_(2)RR),whereas the behavior is by far superficially understood.Here,we report that CO_(2)acc...Structural reconstruction of electrocatalysts plays a pivotal role in catalytic performances for CO_(2)reduction reaction(CO_(2)RR),whereas the behavior is by far superficially understood.Here,we report that CO_(2)accessibility results in a universal self-adaptive structural reconstruction from Cu_(2)O to Cu@CuxO composites,ending with feeding gas-dependent microstructures and catalytic performances.The CO_(2)-rich atmosphere favors reconstruction for CO_(2)RR,whereas the CO_(2)-deficient one prefers that for hydrogen evolution reaction.With the assistance of spectroscopic analysis and theoretical calculations,we uncover a CO_(2)-induced passivation behavior by identifying a reductionresistant but catalytic active Cu(I)-rich amorphous layer stabilized by*CO intermediates.Additionally,we find extra CO production is indispensable for the robust production of C2H4.An inverse correlation between durability and FECO/FEC2H4 is disclosed,suggesting that the selfstabilization process involving the absorption of*CO intermediates on Cu(I)sites is essential for durable electrolysis.Guided by this insight,we design hollow Cu_(2)O nanospheres for durable and selective CO_(2)RR electrolysis in producing C2H4.Our work recognizes the previously overlooked passivation reconstruction and self-stabilizing behavior and highlights the critical role of the local atmosphere in modulating reconstruction and catalytic processes.展开更多
CsPbX_(3)-based(X=I,Br,Cl)inorganic perovskite solar cells(PSCs)prepared by low-temperature process have attracted much attention because of their low cost and excellent thermal stability.However,the high trap state d...CsPbX_(3)-based(X=I,Br,Cl)inorganic perovskite solar cells(PSCs)prepared by low-temperature process have attracted much attention because of their low cost and excellent thermal stability.However,the high trap state density and serious charge recombination between low-temperature processed TiO_(2)film and inorganic perovskite layer interface seriously restrict the performance of all-inorganic PSCs.Here a thin polyethylene oxide(PEO)layer is employed to modify TiO_(2)film to passivate traps and promote carrier collection.The impacts of PEO layer on microstructure and photoelectric characteristics of TiO_(2)film and related devices are systematically studied.Characterization results suggest that PEO modification can reduce the surface roughness of TiO_(2)film,decrease its average surface potential,and passivate trap states.At optimal conditions,the champion efficiency of CsPbI_(2)Br PSCs with PEO-modified TiO_(2)(PEO-PSCs)has been improved to 11.24%from 9.03%of reference PSCs.Moreover,the hysteresis behavior and charge recombination have been suppressed in PEO-PSCs.展开更多
CsPbI_(2)Br perovskite solar cell has been extensively studied due to its exceptional thermal stability and relatively stable perovskite phase structure.However,the presence of bromine leads to a rapid crystallization...CsPbI_(2)Br perovskite solar cell has been extensively studied due to its exceptional thermal stability and relatively stable perovskite phase structure.However,the presence of bromine leads to a rapid crystallization rate of CsPbI_(2)Br films,resulting in small grain size and high defect density.Additionally,CsPbI_(2)Br demonstrates poor light absorption due to its wide bandgap.Therefore,it is crucial to control the crystallization rate and increase the film thickness to reduce defect density,enhance light absorption,and improve photovoltaic performance.In this study,we utilized a PbAc_(2)-incorporated twice spincoating(PTS) process to address these issues.Initially,PbAc_(2) was added to the CsPbI_(2)Br precursor solution to form a CsPbI_(2)Br film,which was then coated with the CsPbI_(2)Br precursor solution to produce the PTS film,Ac^(-)can delay the perovskite crystallization,leading to the formation of thicker and denser CsPbI_(2)Br films.Moreover,lone-pair electrons of the oxygen atom provided by Ac^(-)formed coordination bonds with under-coordinated Pb~(2+) ions to fill halogen ion vacancies,thereby reducing the defect density.Ultimately,the PTS CsPbI_(2)Br device achieved a peak power conversion efficiency(PCE) of 16.19% and maintained 96.7% of its initial PCE over 1500 h at room temperature under 25% relative humidity without any encapsulation.展开更多
Offshore carbon dioxide(CO_(2)) geological storage(OCGS) represents a significant strategy for addressing climate change by curtailing greenhouse gas emissions. Nonetheless, the risk of CO_(2) leakage poses a substant...Offshore carbon dioxide(CO_(2)) geological storage(OCGS) represents a significant strategy for addressing climate change by curtailing greenhouse gas emissions. Nonetheless, the risk of CO_(2) leakage poses a substantial concern associated with this technology. This study introduces an innovative approach for establishing OCGS leakage scenarios, involving four pivotal stages, namely, interactive matrix establishment, risk matrix evaluation, cause–effect analysis, and scenario development, which has been implemented in the Pearl River Estuary Basin in China. The initial phase encompassed the establishment of an interaction matrix for OCGS systems based on features, events, and processes. Subsequent risk matrix evaluation and cause–effect analysis identified key system components, specifically CO_(2) injection and faults/features. Building upon this analysis, two leakage risk scenarios were successfully developed, accompanied by the corresponding mitigation measures. In addition, this study introduces the application of scenario development to risk assessment, including scenario numerical simulation and quantitative assessment. Overall, this research positively contributes to the sustainable development and safe operation of OCGS projects and holds potential for further refinement and broader application to diverse geographical environments and project requirements. This comprehensive study provides valuable insights into the establishment of OCGS leakage scenarios and demonstrates their practical application to risk assessment, laying the foundation for promoting the sustainable development and safe operation of ocean CO_(2) geological storage projects while proposing possibilities for future improvements and broader applications to different contexts.展开更多
Geomagnetic storm events have a strong influence on the ionosphere–thermosphere(I-T)coupling system.Analyzing the regional response process of the I-T system and its differences across the northern and southern hemis...Geomagnetic storm events have a strong influence on the ionosphere–thermosphere(I-T)coupling system.Analyzing the regional response process of the I-T system and its differences across the northern and southern hemispheres is an important but challenging task.In this study,we used a combination of multiple observations and a model simulation to examine the north–south hemispheric difference in the I-T coupling system in the American and Asian sectors during the geomagnetic superstorm that occurred in May 2024.Observations of the total electron content(TEC)showed that the Asian sector had negative storms in the northern hemisphere and positive storms in the southern hemisphere,a process that exacerbated the hemispheric differences in the TEC.However,both hemispheres of the American sector showed negative storms.The thermospheric composition changes also differed between the two sectors,and their variation could partially explain the hemispheric differences caused by positive and negative storms.Moreover,the influence of the thermospheric density change was less than that of the thermospheric composition.Finally,the dynamic effect of the thermospheric wind and the plasma transport processes strongly modulated the north–south differences in the TEC at nighttime in the American and Asian sectors,respectively,during this superstorm.展开更多
L2 reading is not only an important channel for people to obtain information and knowledge,but also the main way for people to learn a foreign language.Reading information processing can be divided into controlled pro...L2 reading is not only an important channel for people to obtain information and knowledge,but also the main way for people to learn a foreign language.Reading information processing can be divided into controlled processing and automatic processing.Controlled information processing is a conscious and resource-intensive processing model,while automatic information processing is an unconscious and automatic processing model.This study investigates the characteristics and interactivity of controlled and automatic information processing in L2 reading,and explores the roles of controlled and automatic information processing strategies in improving L2 reading ability.The findings are as follows:(a)controlled and automatic information processing is interactive in L2 reading;and(b)the uses of controlled and automatic information processing strategies are beneficial to the improvement of the reading ability of L2 learners.This study has important theoretical and practical value in improving the efficiency of L2 reading teaching and learning.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.22479097)the Shanghai Science and Technology Committee(Grant No.23ZR1433000)the National High-Level Talent Program for Young Scholars,the Start-up Fund(F.S.)from Shanghai Jiao Tong University.
文摘Structural reconstruction of electrocatalysts plays a pivotal role in catalytic performances for CO_(2)reduction reaction(CO_(2)RR),whereas the behavior is by far superficially understood.Here,we report that CO_(2)accessibility results in a universal self-adaptive structural reconstruction from Cu_(2)O to Cu@CuxO composites,ending with feeding gas-dependent microstructures and catalytic performances.The CO_(2)-rich atmosphere favors reconstruction for CO_(2)RR,whereas the CO_(2)-deficient one prefers that for hydrogen evolution reaction.With the assistance of spectroscopic analysis and theoretical calculations,we uncover a CO_(2)-induced passivation behavior by identifying a reductionresistant but catalytic active Cu(I)-rich amorphous layer stabilized by*CO intermediates.Additionally,we find extra CO production is indispensable for the robust production of C2H4.An inverse correlation between durability and FECO/FEC2H4 is disclosed,suggesting that the selfstabilization process involving the absorption of*CO intermediates on Cu(I)sites is essential for durable electrolysis.Guided by this insight,we design hollow Cu_(2)O nanospheres for durable and selective CO_(2)RR electrolysis in producing C2H4.Our work recognizes the previously overlooked passivation reconstruction and self-stabilizing behavior and highlights the critical role of the local atmosphere in modulating reconstruction and catalytic processes.
基金financially supported by the Guangzhou Basic and Applied Basic Research Foundation,China(No.303523)。
文摘CsPbX_(3)-based(X=I,Br,Cl)inorganic perovskite solar cells(PSCs)prepared by low-temperature process have attracted much attention because of their low cost and excellent thermal stability.However,the high trap state density and serious charge recombination between low-temperature processed TiO_(2)film and inorganic perovskite layer interface seriously restrict the performance of all-inorganic PSCs.Here a thin polyethylene oxide(PEO)layer is employed to modify TiO_(2)film to passivate traps and promote carrier collection.The impacts of PEO layer on microstructure and photoelectric characteristics of TiO_(2)film and related devices are systematically studied.Characterization results suggest that PEO modification can reduce the surface roughness of TiO_(2)film,decrease its average surface potential,and passivate trap states.At optimal conditions,the champion efficiency of CsPbI_(2)Br PSCs with PEO-modified TiO_(2)(PEO-PSCs)has been improved to 11.24%from 9.03%of reference PSCs.Moreover,the hysteresis behavior and charge recombination have been suppressed in PEO-PSCs.
基金supported by the National Natural Science Foundation of China (U22A20142)the Fundamental Research Funds for the Central Universities (2023JC007)。
文摘CsPbI_(2)Br perovskite solar cell has been extensively studied due to its exceptional thermal stability and relatively stable perovskite phase structure.However,the presence of bromine leads to a rapid crystallization rate of CsPbI_(2)Br films,resulting in small grain size and high defect density.Additionally,CsPbI_(2)Br demonstrates poor light absorption due to its wide bandgap.Therefore,it is crucial to control the crystallization rate and increase the film thickness to reduce defect density,enhance light absorption,and improve photovoltaic performance.In this study,we utilized a PbAc_(2)-incorporated twice spincoating(PTS) process to address these issues.Initially,PbAc_(2) was added to the CsPbI_(2)Br precursor solution to form a CsPbI_(2)Br film,which was then coated with the CsPbI_(2)Br precursor solution to produce the PTS film,Ac^(-)can delay the perovskite crystallization,leading to the formation of thicker and denser CsPbI_(2)Br films.Moreover,lone-pair electrons of the oxygen atom provided by Ac^(-)formed coordination bonds with under-coordinated Pb~(2+) ions to fill halogen ion vacancies,thereby reducing the defect density.Ultimately,the PTS CsPbI_(2)Br device achieved a peak power conversion efficiency(PCE) of 16.19% and maintained 96.7% of its initial PCE over 1500 h at room temperature under 25% relative humidity without any encapsulation.
文摘Offshore carbon dioxide(CO_(2)) geological storage(OCGS) represents a significant strategy for addressing climate change by curtailing greenhouse gas emissions. Nonetheless, the risk of CO_(2) leakage poses a substantial concern associated with this technology. This study introduces an innovative approach for establishing OCGS leakage scenarios, involving four pivotal stages, namely, interactive matrix establishment, risk matrix evaluation, cause–effect analysis, and scenario development, which has been implemented in the Pearl River Estuary Basin in China. The initial phase encompassed the establishment of an interaction matrix for OCGS systems based on features, events, and processes. Subsequent risk matrix evaluation and cause–effect analysis identified key system components, specifically CO_(2) injection and faults/features. Building upon this analysis, two leakage risk scenarios were successfully developed, accompanied by the corresponding mitigation measures. In addition, this study introduces the application of scenario development to risk assessment, including scenario numerical simulation and quantitative assessment. Overall, this research positively contributes to the sustainable development and safe operation of OCGS projects and holds potential for further refinement and broader application to diverse geographical environments and project requirements. This comprehensive study provides valuable insights into the establishment of OCGS leakage scenarios and demonstrates their practical application to risk assessment, laying the foundation for promoting the sustainable development and safe operation of ocean CO_(2) geological storage projects while proposing possibilities for future improvements and broader applications to different contexts.
基金supported by the National Natural Science Foundation of China (Grant Nos. 42030202, 42241115, and 42174204)the China Postdoctoral Science Foundation (Grant No. 2023M743467)+2 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences (Grant No. Y202021)the National Key R&D Program of China (Grant No. 2022YFF0504400)the Opening Funding of the Chinese Academy of Sciences dedicated to the Chinese Meridian Project
文摘Geomagnetic storm events have a strong influence on the ionosphere–thermosphere(I-T)coupling system.Analyzing the regional response process of the I-T system and its differences across the northern and southern hemispheres is an important but challenging task.In this study,we used a combination of multiple observations and a model simulation to examine the north–south hemispheric difference in the I-T coupling system in the American and Asian sectors during the geomagnetic superstorm that occurred in May 2024.Observations of the total electron content(TEC)showed that the Asian sector had negative storms in the northern hemisphere and positive storms in the southern hemisphere,a process that exacerbated the hemispheric differences in the TEC.However,both hemispheres of the American sector showed negative storms.The thermospheric composition changes also differed between the two sectors,and their variation could partially explain the hemispheric differences caused by positive and negative storms.Moreover,the influence of the thermospheric density change was less than that of the thermospheric composition.Finally,the dynamic effect of the thermospheric wind and the plasma transport processes strongly modulated the north–south differences in the TEC at nighttime in the American and Asian sectors,respectively,during this superstorm.
文摘L2 reading is not only an important channel for people to obtain information and knowledge,but also the main way for people to learn a foreign language.Reading information processing can be divided into controlled processing and automatic processing.Controlled information processing is a conscious and resource-intensive processing model,while automatic information processing is an unconscious and automatic processing model.This study investigates the characteristics and interactivity of controlled and automatic information processing in L2 reading,and explores the roles of controlled and automatic information processing strategies in improving L2 reading ability.The findings are as follows:(a)controlled and automatic information processing is interactive in L2 reading;and(b)the uses of controlled and automatic information processing strategies are beneficial to the improvement of the reading ability of L2 learners.This study has important theoretical and practical value in improving the efficiency of L2 reading teaching and learning.
