Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.L...Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.展开更多
Powdery mildew negatively impacts wheat yield and quality.Emmer wheat(Triticum dicoccum),an ancestral species of common wheat,is a gene donor for wheat improvement.Cultivated emmer accession H1-707 exhibited all-stage...Powdery mildew negatively impacts wheat yield and quality.Emmer wheat(Triticum dicoccum),an ancestral species of common wheat,is a gene donor for wheat improvement.Cultivated emmer accession H1-707 exhibited all-stage resistance to powdery mildew over consecutive years.Genetic analysis of H1-707 at the seedling stage revealed a dominant monogenic inheritance pattern,and the underlying gene was designated Pm71.By employing bulked segregant exome sequencing(BSE-Seq)and using 2000 F2:3 families,Pm71 was fine mapped to a 336-kb interval on chromosome arm 6AS by referencing to the durum cv.Svevo RefSeq 1.0.Collinearity analysis revealed high homology in the candidate interval between Svevo and six Triticum species.Among six high-confidence genes annotated within this interval,TRITD6Av1G005050 encoding a GDSL esterase/lipase was identified as a key candidate for Pm71.展开更多
Defect engineering in metal organic frameworks(MOFs)has captured significant attention in the field of photocatalysis.A series of UiO-66(Ce)(UiO=University of Oslo)MOFs with different contents of missing-linker defect...Defect engineering in metal organic frameworks(MOFs)has captured significant attention in the field of photocatalysis.A series of UiO-66(Ce)(UiO=University of Oslo)MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine(BA)and thioanisole(TA)under visible light.The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce3+content.It also generates a high concentration of oxygen vacancies.In situ Fourier transform infrared spectroscopy(FTIR)results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H-N…Ce and the C-S…Ce interactions,respectively.Simulated in situ electron paramagnetic resonance(EPR)data indicate that O_(2) activation and reduction occur at coordinatively unsaturated Ce^(3+)sites to form·O_(2)^(-).This is accelerated by the Ce^(3+)/Ce^(4+)redox cycle associated with the photogenerated electrons.The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA.The most active sample exhibits 98.4%and 95.5%conversion rates for BA and TA oxidation.Mechanisms for the molecular activation are proposed at the molecular level.展开更多
This study focuses on the spatiotemporal distribution,urban-rural variations,and driving factors of ammonia Vertical Column Densities(VCDs)in China’s Yangtze River Delta region(YRD)from 2008 to 2020.Utilizing data fr...This study focuses on the spatiotemporal distribution,urban-rural variations,and driving factors of ammonia Vertical Column Densities(VCDs)in China’s Yangtze River Delta region(YRD)from 2008 to 2020.Utilizing data from the Infrared Atmospheric Sounding Interfer-ometer(IASI),Generalized Additive Models(GAM),and the GEOS-Chem chemical transport model,we observed a significant increase of NH_(3)VCDs in the YRD between 2014 and 2020.The spatial distribution analysis revealed higher NH_(3)concentrations in the northern part of the YRD region,primarily due to lower precipitation,alkaline soil,and intensive agricul-tural activities.NH_(3)VCDs in the YRD region increased significantly(65.18%)from 2008 to 2020.The highest growth rate occurs in the summer,with an annual average growth rate of 7.2%during the period from 2014 to 2020.Agricultural emissions dominated NH_(3)VCDs during spring and summer,with high concentrations primarily located in the agricultural areas adjacent to densely populated urban zones.Regions within several large urban areas have been discovered to exhibit relatively stable variations in NH_(3)VCDs.The rise in NH_(3)VCDs within the YRD region was primarily driven by the reduction of acidic gases like SO_(2),as emphasized by GAM modeling and sensitivity tests using the GEOS-Chem model.The concentration changes of acidic gases contribute to over 80%of the interannual variations in NH_(3)VCDs.This emphasizes the crucial role of environmental policies targeting the reduction of these acidic gases.Effective emission control is urgent tomitigate environmental hazards and secondary particulate matter,especially in the northern YRD.展开更多
We present systematic identifications of supergiants in M31/M33 based on the Large Sky Area Multi-Object Fiber Spectroscopic Telescope(LAMOST)spectroscopic survey.Radial velocities of nearly 5000 photometrically selec...We present systematic identifications of supergiants in M31/M33 based on the Large Sky Area Multi-Object Fiber Spectroscopic Telescope(LAMOST)spectroscopic survey.Radial velocities of nearly 5000 photometrically selected M31/M33 supergiant candidates have been properly derived from the qualified spectra released in LAMOST DR10.By comparing their radial velocities with those predicted from the rotation curve of M31,as well as utilizing Gaia astrometric measurements to exclude foreground contaminations,199 supergiant members in M31,including 168“Rank1”and 31“Rank2,”have been successfully identified.This sample contains 62 blue supergiants(BSGs,all“Rank1”),134 yellow supergiants(YSGs,103“Rank1”and 31“Rank2”)and three red supergiants(RSGs,all“Rank1”).For M33,we identify 84 supergiant members(56“Rank1”and 28“Rank2”),which include 28 BSGs(all“Rank1”),53 YSGs(25“Rank1”and 28“Rank2”)and three RSGs(all“Rank1”).So far,this is one of the largest supergiant samples of M31/M33 with full optical wavelength coverage(3700<λ<9100Å).This sample is valuable for understanding star formation and stellar evolution under different environments.展开更多
China is the largest emitter of anthropogenic CO_(2) globally,with its cities recognized as significant emission hotspots.Consequently,evaluating anthropogenic CO_(2) emissions and the carbon neutral capability(CNC)of...China is the largest emitter of anthropogenic CO_(2) globally,with its cities recognized as significant emission hotspots.Consequently,evaluating anthropogenic CO_(2) emissions and the carbon neutral capability(CNC)of Chinese cities is critical for climate change mitigation.Despite this importance,no studies to date have assessed recent and future city-scale CNCs using the top-down atmospheric inversion approach,revealing substantial knowledge gaps regarding regional CO_(2) budgets.To address these issues,this research focused on Hangzhou,a megacity known for having the highest forest cover among China’s provincial capitals,as study region.Year-round atmospheric CO_(2) concentration measurements were conducted from December 2020 to November 2021 at two sites:one urban and one suburban.These observations,along with their difference,were utilized to derive city-scale posterior anthropogenic CO_(2) emissions and to evaluate recent and future CNCs.Our key findings are as follows:(1)The manufacturing industry,energy industry and oil refineries/transformation industry were identified as the largest contributors to urban-suburban CO_(2) difference,accounting for 36.5%,21.3%,and 16.6%,respectively.Additionally,82.5%,65.2%,81.2%and 86.3%of total anthropogenic CO_(2) enhancements were attributed to emissions within Hangzhou city in winter,spring,summer and autumn,respectively.(2)The posterior annual anthropogenic CO_(2) emission for Hangzhouwas estimated at 4.65(±0.72)×10^(10) kg/a,indicating significant biases among different prior CO_(2) emission inventories.The annual biological CO_(2) sink,derived from multiple products,was estimated at-0.48(±0.16)×10^(10) kg.(3)The calculated CNC for 2021was 10.3%±3.4%,highlighting a substantial gap towards achieving full carbon neutrality.Considering potential increases in ecosystem carbon sinks due to forest age and uncertainties from climate change,it was predicted that at least 65.2%-82.6%of anthropogenic CO_(2) emissions must be reduced to achieve the goal of full carbon neutrality by year of 2060.展开更多
基金financially supported by Shenzhen Science and Technology Program(JCYJ20240813142900001)Guangdong Provincial Key Laboratory of New Energy Materials Service Safety。
文摘Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.
基金financially supported by National Natural Science Foundation of China(32301800,32301923 and 32072053)Wheat Industrial Technology System of Shandong Province(SDAIT-01-01)Key Research and Development Project of Shandong Province(2022LZG002-4,2023LZGC009-4-4).
文摘Powdery mildew negatively impacts wheat yield and quality.Emmer wheat(Triticum dicoccum),an ancestral species of common wheat,is a gene donor for wheat improvement.Cultivated emmer accession H1-707 exhibited all-stage resistance to powdery mildew over consecutive years.Genetic analysis of H1-707 at the seedling stage revealed a dominant monogenic inheritance pattern,and the underlying gene was designated Pm71.By employing bulked segregant exome sequencing(BSE-Seq)and using 2000 F2:3 families,Pm71 was fine mapped to a 336-kb interval on chromosome arm 6AS by referencing to the durum cv.Svevo RefSeq 1.0.Collinearity analysis revealed high homology in the candidate interval between Svevo and six Triticum species.Among six high-confidence genes annotated within this interval,TRITD6Av1G005050 encoding a GDSL esterase/lipase was identified as a key candidate for Pm71.
基金supported by the National Natural Science Foundation of China(Nos.22272026 and 22272028)the 111 Project(No.D16008)Jinhong Bi thanks the Youth Talent Support Program of Fujian Province(No.00387077).
文摘Defect engineering in metal organic frameworks(MOFs)has captured significant attention in the field of photocatalysis.A series of UiO-66(Ce)(UiO=University of Oslo)MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine(BA)and thioanisole(TA)under visible light.The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce3+content.It also generates a high concentration of oxygen vacancies.In situ Fourier transform infrared spectroscopy(FTIR)results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H-N…Ce and the C-S…Ce interactions,respectively.Simulated in situ electron paramagnetic resonance(EPR)data indicate that O_(2) activation and reduction occur at coordinatively unsaturated Ce^(3+)sites to form·O_(2)^(-).This is accelerated by the Ce^(3+)/Ce^(4+)redox cycle associated with the photogenerated electrons.The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA.The most active sample exhibits 98.4%and 95.5%conversion rates for BA and TA oxidation.Mechanisms for the molecular activation are proposed at the molecular level.
基金supported by the Joint Funds of the National Natural Science Foundation of China(No.U21A2027)the New Cornerstone Science Foundation through the XPLORER PRIZE(2023-1033).
文摘This study focuses on the spatiotemporal distribution,urban-rural variations,and driving factors of ammonia Vertical Column Densities(VCDs)in China’s Yangtze River Delta region(YRD)from 2008 to 2020.Utilizing data from the Infrared Atmospheric Sounding Interfer-ometer(IASI),Generalized Additive Models(GAM),and the GEOS-Chem chemical transport model,we observed a significant increase of NH_(3)VCDs in the YRD between 2014 and 2020.The spatial distribution analysis revealed higher NH_(3)concentrations in the northern part of the YRD region,primarily due to lower precipitation,alkaline soil,and intensive agricul-tural activities.NH_(3)VCDs in the YRD region increased significantly(65.18%)from 2008 to 2020.The highest growth rate occurs in the summer,with an annual average growth rate of 7.2%during the period from 2014 to 2020.Agricultural emissions dominated NH_(3)VCDs during spring and summer,with high concentrations primarily located in the agricultural areas adjacent to densely populated urban zones.Regions within several large urban areas have been discovered to exhibit relatively stable variations in NH_(3)VCDs.The rise in NH_(3)VCDs within the YRD region was primarily driven by the reduction of acidic gases like SO_(2),as emphasized by GAM modeling and sensitivity tests using the GEOS-Chem model.The concentration changes of acidic gases contribute to over 80%of the interannual variations in NH_(3)VCDs.This emphasizes the crucial role of environmental policies targeting the reduction of these acidic gases.Effective emission control is urgent tomitigate environmental hazards and secondary particulate matter,especially in the northern YRD.
基金funded by the National Natural Science Foundation of China(NSFC,grant Nos.12090040,12090044,12133001,and 12422303)Beijing Natural Science Foundation(no.1242016)+2 种基金the science research grants from the China Manned Space Projectsupported by the Talents Program(24CE-YS-08)the Popular Science Project(24CD012)of the Beijing Academy of Science and Technology.
文摘We present systematic identifications of supergiants in M31/M33 based on the Large Sky Area Multi-Object Fiber Spectroscopic Telescope(LAMOST)spectroscopic survey.Radial velocities of nearly 5000 photometrically selected M31/M33 supergiant candidates have been properly derived from the qualified spectra released in LAMOST DR10.By comparing their radial velocities with those predicted from the rotation curve of M31,as well as utilizing Gaia astrometric measurements to exclude foreground contaminations,199 supergiant members in M31,including 168“Rank1”and 31“Rank2,”have been successfully identified.This sample contains 62 blue supergiants(BSGs,all“Rank1”),134 yellow supergiants(YSGs,103“Rank1”and 31“Rank2”)and three red supergiants(RSGs,all“Rank1”).For M33,we identify 84 supergiant members(56“Rank1”and 28“Rank2”),which include 28 BSGs(all“Rank1”),53 YSGs(25“Rank1”and 28“Rank2”)and three RSGs(all“Rank1”).So far,this is one of the largest supergiant samples of M31/M33 with full optical wavelength coverage(3700<λ<9100Å).This sample is valuable for understanding star formation and stellar evolution under different environments.
基金supported by the National Natural Science Foundation of China(Nos.42475125,42105117,42021004 and 41975143)the National Key R&D Program of China(Nos.2019YFA0607202 and 2020YFA0607501)+4 种基金Jiangsu Science Foundation for Distinguished Young Scholar(No.BK20220055)the 333 Project of Jiangsu Province(No.BRA2017402)the R&D Foundation of Jiangsu Province,China(No.BK20220020)Zhejiang Provincial Basic Public Welfare Research Project(No.LGF22D050004)the Key Laboratory of Ecosystem Carbon Source and Sink,China Meteorological Administration(ECSSCMA).
文摘China is the largest emitter of anthropogenic CO_(2) globally,with its cities recognized as significant emission hotspots.Consequently,evaluating anthropogenic CO_(2) emissions and the carbon neutral capability(CNC)of Chinese cities is critical for climate change mitigation.Despite this importance,no studies to date have assessed recent and future city-scale CNCs using the top-down atmospheric inversion approach,revealing substantial knowledge gaps regarding regional CO_(2) budgets.To address these issues,this research focused on Hangzhou,a megacity known for having the highest forest cover among China’s provincial capitals,as study region.Year-round atmospheric CO_(2) concentration measurements were conducted from December 2020 to November 2021 at two sites:one urban and one suburban.These observations,along with their difference,were utilized to derive city-scale posterior anthropogenic CO_(2) emissions and to evaluate recent and future CNCs.Our key findings are as follows:(1)The manufacturing industry,energy industry and oil refineries/transformation industry were identified as the largest contributors to urban-suburban CO_(2) difference,accounting for 36.5%,21.3%,and 16.6%,respectively.Additionally,82.5%,65.2%,81.2%and 86.3%of total anthropogenic CO_(2) enhancements were attributed to emissions within Hangzhou city in winter,spring,summer and autumn,respectively.(2)The posterior annual anthropogenic CO_(2) emission for Hangzhouwas estimated at 4.65(±0.72)×10^(10) kg/a,indicating significant biases among different prior CO_(2) emission inventories.The annual biological CO_(2) sink,derived from multiple products,was estimated at-0.48(±0.16)×10^(10) kg.(3)The calculated CNC for 2021was 10.3%±3.4%,highlighting a substantial gap towards achieving full carbon neutrality.Considering potential increases in ecosystem carbon sinks due to forest age and uncertainties from climate change,it was predicted that at least 65.2%-82.6%of anthropogenic CO_(2) emissions must be reduced to achieve the goal of full carbon neutrality by year of 2060.
