Cr^(3+)-activated near-infrared(NIR)phosphors are key for NIR phosphor-converted light emitting diodes(NIR pc-LED).While,the site occupancy of Cr^(3+)is one of the debates that have plagued researchers.Herein,Y2Mg2Al2...Cr^(3+)-activated near-infrared(NIR)phosphors are key for NIR phosphor-converted light emitting diodes(NIR pc-LED).While,the site occupancy of Cr^(3+)is one of the debates that have plagued researchers.Herein,Y2Mg2Al2-Si_(2)O1_(2)(YMAS)with multiple cationic sites is chosen as host of Cr^(3+)to synthesize YMAS:xCr^(3+)phosphors.In YMAS,Cr^(3+)ions occupy simultaneously Al/SiO4 tetrahedral,Mg/AlO6 octahedral,and Y/MgO8 dodecahedral sites which form three luminescent centers named as Cr1,Cr2,and Cr3,respectively.Cr1 and Cr2 relate to an intermediate crystal field,with transitions of^(2)E→^(4)A_(2)and^(4)T_(2)→^(4)A_(2)occurring simultaneously.As Cr^(3+)concentration increases,the^(4)T_(2)→^(4)A_(2)transition becomes more pronounced in Cr1 and Cr2,resulting in a red-shift and broadband emission.Cr3 consistently behaves a weak crystal field and exhibits the broad and long-wavelength emission.Wide-range NIR emission centering at 745 nm is realized in YMAS:0.03Cr^(3+)phosphor.This phosphor has high internal quantum efficiency(IQE?86%)and satisfying luminescence thermal stability(I423 K?70.2%).Using this phosphor,NIR pc-LEDs with 56.6 mW@320 mA optical output power is packaged and applied.Present study not only demonstrates the Cr^(3+)multi-site occupancy in a certain oxide but also provides a reliable approach via choosing a host with diverse cationic sites and local environments for Cr^(3+)to achieve broadband NIR phosphors.展开更多
Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction ...Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.展开更多
Taking the sociopetal space with high using rate and welcomed by visitors in Jingxiu Park of Baoding as the study object,human demands on spatial characteristics and space factors were evaluated by the method of POE,a...Taking the sociopetal space with high using rate and welcomed by visitors in Jingxiu Park of Baoding as the study object,human demands on spatial characteristics and space factors were evaluated by the method of POE,and modification measures of the sociopetal space in city opening park were put forward,which provided evidence for solving regional problems of city park and creating urban open space.展开更多
Based on an available parking space occupancy （APSO） survey conducted in Nanjing, China, an APSO forecasting model is proposed. The APSO survey results indicate that the time series of APSO with different time-secti...Based on an available parking space occupancy （APSO） survey conducted in Nanjing, China, an APSO forecasting model is proposed. The APSO survey results indicate that the time series of APSO with different time-sections are periodical and self-similar, and the fluctuation of the APSO increases with the decrease in time-sections. Taking the short-time change behavior into account, an APSO forecasting model combined wavelet analysis and a weighted Markov chain is presented. In this model, an original APSO time series is first decomposed by wavelet analysis, and the results include low frequency signals representing the basic trends of APSO and several high frequency signals representing disturbances of the APSO. Then different Markov models are used to forecast the changes of low and high frequency signals, respectively. Finally, integrating the predicted results induces the final forecasted APSO. A case study verifies the applicability of the proposed model. The comparisons between measured and forecasted results show that the model is a competent model and its accuracy relies on real-time update of the APSO database.展开更多
基金supported by the National Natural Science Foundation of China(No.51772330)the Fundamental Research Funds for the Central Universities of Central South University(No.506021713)the National MCF Energy R&D Program of China(No.2018YFE0306100).
文摘Cr^(3+)-activated near-infrared(NIR)phosphors are key for NIR phosphor-converted light emitting diodes(NIR pc-LED).While,the site occupancy of Cr^(3+)is one of the debates that have plagued researchers.Herein,Y2Mg2Al2-Si_(2)O1_(2)(YMAS)with multiple cationic sites is chosen as host of Cr^(3+)to synthesize YMAS:xCr^(3+)phosphors.In YMAS,Cr^(3+)ions occupy simultaneously Al/SiO4 tetrahedral,Mg/AlO6 octahedral,and Y/MgO8 dodecahedral sites which form three luminescent centers named as Cr1,Cr2,and Cr3,respectively.Cr1 and Cr2 relate to an intermediate crystal field,with transitions of^(2)E→^(4)A_(2)and^(4)T_(2)→^(4)A_(2)occurring simultaneously.As Cr^(3+)concentration increases,the^(4)T_(2)→^(4)A_(2)transition becomes more pronounced in Cr1 and Cr2,resulting in a red-shift and broadband emission.Cr3 consistently behaves a weak crystal field and exhibits the broad and long-wavelength emission.Wide-range NIR emission centering at 745 nm is realized in YMAS:0.03Cr^(3+)phosphor.This phosphor has high internal quantum efficiency(IQE?86%)and satisfying luminescence thermal stability(I423 K?70.2%).Using this phosphor,NIR pc-LEDs with 56.6 mW@320 mA optical output power is packaged and applied.Present study not only demonstrates the Cr^(3+)multi-site occupancy in a certain oxide but also provides a reliable approach via choosing a host with diverse cationic sites and local environments for Cr^(3+)to achieve broadband NIR phosphors.
基金financially supported by the Scientific and Technological Development Program of Jilin Province(20220201138GX)the support of the National Key R&D Program of China(No.2022YFA1503801)+1 种基金CAS Project for Young Scientists in Basic Research(No.YSBR-022)the Young Cross Team Project of CAS(No.JCTD-2021-14)。
文摘Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.
文摘Taking the sociopetal space with high using rate and welcomed by visitors in Jingxiu Park of Baoding as the study object,human demands on spatial characteristics and space factors were evaluated by the method of POE,and modification measures of the sociopetal space in city opening park were put forward,which provided evidence for solving regional problems of city park and creating urban open space.
基金The National Natural Science Foundation of China(No50738001)the National Basic Research Program of China (973Program) (No2006CB705501)
文摘Based on an available parking space occupancy （APSO） survey conducted in Nanjing, China, an APSO forecasting model is proposed. The APSO survey results indicate that the time series of APSO with different time-sections are periodical and self-similar, and the fluctuation of the APSO increases with the decrease in time-sections. Taking the short-time change behavior into account, an APSO forecasting model combined wavelet analysis and a weighted Markov chain is presented. In this model, an original APSO time series is first decomposed by wavelet analysis, and the results include low frequency signals representing the basic trends of APSO and several high frequency signals representing disturbances of the APSO. Then different Markov models are used to forecast the changes of low and high frequency signals, respectively. Finally, integrating the predicted results induces the final forecasted APSO. A case study verifies the applicability of the proposed model. The comparisons between measured and forecasted results show that the model is a competent model and its accuracy relies on real-time update of the APSO database.
