Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the r...Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely reported.To fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/S-MCC.The chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and CPL.The emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV region.Notably,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV CPL.Our work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral OIHMH.The RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.展开更多
Rare-earth(RE)halide solid electrolytes(HSEs)have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries(ASSBs).However,only very limited types...Rare-earth(RE)halide solid electrolytes(HSEs)have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries(ASSBs).However,only very limited types of HSEs have been reported with high performance.In this work,tens of grams of RE-HSE Li_(3)TbBr_(6)(LTbB)was synthesized by a vacuum evaporationassisted method.The as-prepared LTbB displays a high ionic conductivity of 1.7 mS·cm^(-1),a wide electrochemical window,and good formability.Accordingly,the assembled solid lithium-tellurium(Li-Te)battery based on the LTbB HSE exhibits excellent cycling stability up to 600 cycles,which is superior to most previous reports.The processes and the chemicals during the discharge/charge of Li-Te batteries have been studied by various in situ and ex situ characterizations.Theoretical calculations have demonstrated the dominant conductivity contributions of the direct[octahedral]-[octahedral]([Oct]-[Oct])pathway for Li ion migrations in the electrolyte.The Tb sites guarantee efficient electron transfer while the Li 2s orbitals are not affected during migration,leading to a low activation barrier.Therefore,this successful fabrication and application of LTbB have offered a highly competitive solution for solid electrolytes in ASSBs,indicating the great potential of RE-based HSEs in energy devices.展开更多
IrOx-based catalysts are considered the most promising candidates for oxygen evolution reaction(OER)due to their high efficiency.However,improving their intrinsic catalytic activity is essential for practical applicat...IrOx-based catalysts are considered the most promising candidates for oxygen evolution reaction(OER)due to their high efficiency.However,improving their intrinsic catalytic activity is essential for practical application.In this work,CeO_(2)with three different morphologies(rod,cube,octahedron)and supported IrOx nanoparticles were fabricated,and they display morphology-dependent OER activity.The IrOx/CeO_(2)-rod shows the highest activity;the catalysts have a catalytic activity sequence of rod>cube>octahedron.A plausible mechanism was proposed:the CeO_(2)support with different morphologies modulates the electronic structure of IrOx by the synergistic interaction promoted by oxygen vacancies between the active component and the support,thereby altering the catalytic activity of the IrOx/CeO_(2)catalyst.展开更多
The behavior of antibiotics and the corresponding resistance genes in aerobic granular reactors for treating biogas slurry under different hydraulic retention times (10.7 h, Rl;8 h, R2) was investigated in this study....The behavior of antibiotics and the corresponding resistance genes in aerobic granular reactors for treating biogas slurry under different hydraulic retention times (10.7 h, Rl;8 h, R2) was investigated in this study. The results indicated that the hydraulic retention time could affect the effluent concentrations and removal efficiencies of sulfonamides. The average removal rates of tetracyclines, fluoroquinolones, and sulfonamides were 63%, 46%, and 90% in Rl, and 62%, 46%, and 86% in R2, respectively. Although the removal efficiencies of tetracyclines and fluoroquinolones were similar in both reactors, the respective accumulated concentrations of tetracyclines and fluoroquinolones in R1 were 7.00 and 11.15μg/g SS, which were lower than those in R2 (8.92 and 13.37μg/g SS, respectively). The difference in the relative abundance of target antibiotic resistance genes between both reactors was not significant, yet the average relative abundances of all target resistance genes in R1 were higher than those in R2 after 45 days of operation. The results of this study suggested that a longer hydraulic retention time could enhance the antibiotic removal ability of aerobic granular sludge, yet it may also increase the risk of surplus sludge utilization from a resistance genes point of view.展开更多
基金supported by the National Natural Science Foundation of China(92256202,12261131500,22305129,22371131,52103218)the Fundamental Research Funds for the Central Universities,Nankai University(023-63223021)+3 种基金Tianjin Key Lab for Rare Earth Materials and Applications(ZB19500202)the Outstanding Youth Project of Tianjin Natural Science Foundation(20JCJQJC00130)China Postdoctoral Science Foundation(BX20220157,2022M721698)the 111 Project(B12015,B18030)。
文摘Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting diodes.However,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely reported.To fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/S-MCC.The chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and CPL.The emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV region.Notably,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV CPL.Our work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral OIHMH.The RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.
基金This work was supported by the National Key R&D Program of China(No.2021YFA1501101)the Natural Science Foundation of China(No.21971117)+11 种基金Functional Research Funds for the Central Universities,Nankai University(No.63186005)Tianjin Key Lab for Rare Earth Materials and Applications(No.ZB19500202)the National Natural Science Foundation of China/Research Grant Council Joint Research Scheme(No.N_PolyU502/21)111 Project(No.B18030)from ChinaOutstanding Youth Project of Tianjin Natural Science Foundation(No.20JCJQJC00130)Key Project of Tianjin Natural Science Foundation(No.20JCZDJC00650)the Projects of Strategic Importance of The Hong Kong Polytechnic University(No.1-ZE2V)Shenzhen Fundamental Research Scheme-General Program(No.JCYJ20220531090807017)National Postdoctoral Program for Innovative Talents(No.BX20220157)Open Foundation of State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures(No.2022GXYSOF07)Haihe Laboratory of Sustainable Chemical Transformations.B.L.H.also thanks the support from Research Centre for Carbon-Strategic Catalysis(RCCSC),Research Institute for Smart Energy(RISE)Research Institute for Intelligent Wearable Systems(RI-IWEAR)of the Hong Kong Polytechnic University.
文摘Rare-earth(RE)halide solid electrolytes(HSEs)have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries(ASSBs).However,only very limited types of HSEs have been reported with high performance.In this work,tens of grams of RE-HSE Li_(3)TbBr_(6)(LTbB)was synthesized by a vacuum evaporationassisted method.The as-prepared LTbB displays a high ionic conductivity of 1.7 mS·cm^(-1),a wide electrochemical window,and good formability.Accordingly,the assembled solid lithium-tellurium(Li-Te)battery based on the LTbB HSE exhibits excellent cycling stability up to 600 cycles,which is superior to most previous reports.The processes and the chemicals during the discharge/charge of Li-Te batteries have been studied by various in situ and ex situ characterizations.Theoretical calculations have demonstrated the dominant conductivity contributions of the direct[octahedral]-[octahedral]([Oct]-[Oct])pathway for Li ion migrations in the electrolyte.The Tb sites guarantee efficient electron transfer while the Li 2s orbitals are not affected during migration,leading to a low activation barrier.Therefore,this successful fabrication and application of LTbB have offered a highly competitive solution for solid electrolytes in ASSBs,indicating the great potential of RE-based HSEs in energy devices.
基金Project supported by the National Natural Science Foundation of China(21522106.21971117)111 Project(B18030)from China+2 种基金the Open Fund of the State Key Laboratory of Rare Earth Resource Utilization(RERU2019001)the Functional Research Fund for the Central Universities,Nankai University(ZB19500202)Beijing-Tianjin-Hebei Collaborative Innovation Project(63201058).
文摘IrOx-based catalysts are considered the most promising candidates for oxygen evolution reaction(OER)due to their high efficiency.However,improving their intrinsic catalytic activity is essential for practical application.In this work,CeO_(2)with three different morphologies(rod,cube,octahedron)and supported IrOx nanoparticles were fabricated,and they display morphology-dependent OER activity.The IrOx/CeO_(2)-rod shows the highest activity;the catalysts have a catalytic activity sequence of rod>cube>octahedron.A plausible mechanism was proposed:the CeO_(2)support with different morphologies modulates the electronic structure of IrOx by the synergistic interaction promoted by oxygen vacancies between the active component and the support,thereby altering the catalytic activity of the IrOx/CeO_(2)catalyst.
基金Science and Technology Project of Fujian Province (No. 2018Y0083)Research fund of Key Laboratory of Environmental Biotechnology, Fiyian Province University (No. EBL2018008)+1 种基金National Natural Science Foundation of China (Grant No. 51878582)and STS Project ofFujian-CAS (No. 2016T3006).
文摘The behavior of antibiotics and the corresponding resistance genes in aerobic granular reactors for treating biogas slurry under different hydraulic retention times (10.7 h, Rl;8 h, R2) was investigated in this study. The results indicated that the hydraulic retention time could affect the effluent concentrations and removal efficiencies of sulfonamides. The average removal rates of tetracyclines, fluoroquinolones, and sulfonamides were 63%, 46%, and 90% in Rl, and 62%, 46%, and 86% in R2, respectively. Although the removal efficiencies of tetracyclines and fluoroquinolones were similar in both reactors, the respective accumulated concentrations of tetracyclines and fluoroquinolones in R1 were 7.00 and 11.15μg/g SS, which were lower than those in R2 (8.92 and 13.37μg/g SS, respectively). The difference in the relative abundance of target antibiotic resistance genes between both reactors was not significant, yet the average relative abundances of all target resistance genes in R1 were higher than those in R2 after 45 days of operation. The results of this study suggested that a longer hydraulic retention time could enhance the antibiotic removal ability of aerobic granular sludge, yet it may also increase the risk of surplus sludge utilization from a resistance genes point of view.