Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging,primarily due to the limitations in charge transfer kinetics.Herein,a fascinating p...Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging,primarily due to the limitations in charge transfer kinetics.Herein,a fascinating plasmonic tandem heterojunction with the hc-CdS/Mo_(2)C@C heterostructure is aimfully prepared for effectively promoting the charge separation kinetics of the CdS photocatalyst via the synergistic strategy of phase junction,Schottky junction,and photothermal effect.The difference in atomic configuration between cubic-CdS (c-CdS) and hexagonal-CdS (h-CdS) leads to effective charge separation through a typical Ⅱ charge transfer mechanism,and plasmonic Schottky junction further extracts the electrons in the hc-CdS phase junction to realize gradient charge transfer.Besides,the photothermal effect of Mo_(2)C@C helps to expand the light absorption,accelerate charge transfer kinetics,and reduce the hydrogen evolution energy barrier.The carbon layer provides a fast channel for charge transfer and protects the photocatalyst from photocorrosion.As a result,the optimized hc-CMC photocatalyst exhibits a significantly high photocatalytic H_(2)production activity of 28.63 mmol/g/h and apparent quantum efficiency of 61.8%,surpassing most of the reported photocatalysts.This study provides a feasible strategy to enhance the charge transfer kinetics and photocatalytic activity of CdS by constructing plasmonic tandem heterogeneous junctions.展开更多
The metal oxide promoter decisively influences the overall performance of Fe catalysts in the direct hydrogenation of CO_(2)to C_(5+)hydrocarbons.However,the roles of metal oxide promoter for Fe catalysts,particularly...The metal oxide promoter decisively influences the overall performance of Fe catalysts in the direct hydrogenation of CO_(2)to C_(5+)hydrocarbons.However,the roles of metal oxide promoter for Fe catalysts,particularly ZrO_(2),have rarely been investigated.To plug this knowledge gap,a new Fe catalyst promoted with Na and partially reduced ZrO_(x)(Na-FeZrO_(x-9))was developed in this study;the catalyst helped produce C_(5+)hydrocarbons in remarkably high yield(26.3%at 360℃).In contrast to ZrO_(x)-free Fe-oxide,NaFeZrO_(x)-9 exhibited long-term stability for CO_(2)hydrogenation(750 h on-stream).The findings revealed multiple roles of ZrO_(x).Notably,ZrO_(x)decorated the Fe-oxide particles after calcination,thereby suppressing excess particle aggregation during the reaction,and acted as a"coke remover"to eliminate the carbon deposited on the catalyst surface.Additionally,oxygen vacancy(O_(v))sites in ZrO_(x)and electron transfer from ZrO_(x)to Fe sites facilitated the adsorption of CO_(2)at the Zr-Fe interface.展开更多
Pd/Co_(2)MnSi(CMS)/Co/Pd multilayer films were designed based on the idea of combining highly spin-polarized materials with strong perpendicular magnetic anisotropy(PMA)films.The PMA of Pd/CMS/Co/Pd multilayer films w...Pd/Co_(2)MnSi(CMS)/Co/Pd multilayer films were designed based on the idea of combining highly spin-polarized materials with strong perpendicular magnetic anisotropy(PMA)films.The PMA of Pd/CMS/Co/Pd multilayer films was studied by optimizing the growth conditions and thickness of each film layer.The optimal structure of the multilayer films was Pd(6 nm)/CMS(5 nm)/Co(2 nm)/Pd(1 nm).Its abnormal Hall resistance(R_(Hall)),coercivity(H_(c))and effective magnetic anisotropy constant(Keff)are 0.08Ω,284 Oe and 1.36 Merg/cm^(3),respectively,which are 100%,492%,and 183%higher than the corresponding values(0.04Ω,48 Oe,and 0.48 Merg/cm^(3))of the Pd(6 nm)/Co(1 nm)/Pd(3 nm)trilayer films.The analysis shows that the increases of the above values are the result of the Pd/CMS interface effect and CMS/Co interface ferromagnetic(FM)coupling,and that it is closely related to the thickness of each film layer in the multilayer films and the growth conditions of the multilayer films.展开更多
Two-terminal(2-T)perovskite(PVK)/CuIn(Ga)Se_(2)(CIGS)tandem solar cells(TSCs)have been considered as an ideal tandem cell because of their best bandgap matching regarding to Shockley–Queisser(S–Q)limits.However,the ...Two-terminal(2-T)perovskite(PVK)/CuIn(Ga)Se_(2)(CIGS)tandem solar cells(TSCs)have been considered as an ideal tandem cell because of their best bandgap matching regarding to Shockley–Queisser(S–Q)limits.However,the nature of the irregular rough morphology of commercial CIGS prevents people from improving tandem device performances.In this paper,D-homoserine lactone hydrochloride is proven to improve coverage of PVK materials on irregular rough CIGS surfaces and also passivate bulk defects by modulating the growth of PVK crystals.In addition,the minority carriers near the PVK/C60 interface and the incompletely passivated trap states caused interface recombination.A surface reconstruction with 2-thiopheneethylammonium iodide and N,N-dimethylformamide assisted passivates the defect sites located at the surface and grain boundaries.Meanwhile,LiF is used to create this field effect,repelling hole carriers away from the PVK and C60 interface and thus reducing recombination.As a result,a 2-T PVK/CIGS tandem yielded a power conversion efficiency of 24.6%(0.16 cm^(2)),one of the highest results for 2-T PVK/CIGS TSCs to our knowledge.This validation underscores the potential of our methodology in achieving superior performance in PVK/CIGS tandem solar cells.展开更多
Food allergy has become a global concern.Spleen tyrosine kinase(SYK)inhibitors are promising therapeutics against allergic disorders.In this study,a total of 300 natural phenolic compounds were firstly subjected to vi...Food allergy has become a global concern.Spleen tyrosine kinase(SYK)inhibitors are promising therapeutics against allergic disorders.In this study,a total of 300 natural phenolic compounds were firstly subjected to virtual screening.Sesamin and its metabolites,sesamin monocatechol(SC-1)and sesamin dicatechol(SC-2),were identified as potential SYK inhibitors,showing high binding affinity and inhibition efficiency towards SYK.Compared with R406(a traditional SYK inhibitor),sesamin,SC-1,and SC-2 had lower binding energy and inhibition constant(Ki)during molecular docking,exhibited higher bioavailability,safety,metabolism/clearance rate,and distribution uniformity ADMET predictions,and showed high stability in occupying the ATP-binding pocket of SYK during molecular dynamics simulations.In anti-dinitrophenyl-immunoglobulin E(Anti-DNP-Ig E)/dinitrophenyl-human serum albumin(DNP-HSA)-stimulated rat basophilic leukemia(RBL-2H3)cells,sesamin in the concentration range of 5-80μmol/L influenced significantly the degranulation and cytokine release,with 54.00%inhibition againstβ-hexosaminidase release and 58.45%decrease in histamine.In BALB/c mice,sesamin could ameliorate Anti-DNP-Ig E/DNP-HSA-induced passive cutaneous anaphylaxis(PCA)and ovalbumin(OVA)-induced active systemic anaphylaxis(ASA)reactions,reduce the levels of allergic mediators(immunoglobulins and pro-inflammatory cytokines),partially correct the imbalance of T helper(Th)cells differentiation in the spleen,and inhibit the phosphorylation of SYK and its downstream signaling proteins,including p38 mitogen-activated protein kinases(p38 MAPK),extracellular signalregulated kinases(ERK),and p65 nuclear factor-κB(p65 NF-κB)in the spleen.Thus,sesamin may be a safe and versatile SYK inhibitor that can alleviate Ig E-mediated food allergies.展开更多
基金National Natural Science Foundation of China (Nos. 22371165, 22209098 and 21971143)111 Project (D20015)Opening Found of Hubei Three Gorges Laboratory (SC232001, SK213002)。
文摘Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging,primarily due to the limitations in charge transfer kinetics.Herein,a fascinating plasmonic tandem heterojunction with the hc-CdS/Mo_(2)C@C heterostructure is aimfully prepared for effectively promoting the charge separation kinetics of the CdS photocatalyst via the synergistic strategy of phase junction,Schottky junction,and photothermal effect.The difference in atomic configuration between cubic-CdS (c-CdS) and hexagonal-CdS (h-CdS) leads to effective charge separation through a typical Ⅱ charge transfer mechanism,and plasmonic Schottky junction further extracts the electrons in the hc-CdS phase junction to realize gradient charge transfer.Besides,the photothermal effect of Mo_(2)C@C helps to expand the light absorption,accelerate charge transfer kinetics,and reduce the hydrogen evolution energy barrier.The carbon layer provides a fast channel for charge transfer and protects the photocatalyst from photocorrosion.As a result,the optimized hc-CMC photocatalyst exhibits a significantly high photocatalytic H_(2)production activity of 28.63 mmol/g/h and apparent quantum efficiency of 61.8%,surpassing most of the reported photocatalysts.This study provides a feasible strategy to enhance the charge transfer kinetics and photocatalytic activity of CdS by constructing plasmonic tandem heterogeneous junctions.
基金financial support from the National Research Council of Science&Technology(NST)grant funded by the Ministry of Science and ICT,Republic of Korea(CAP21012-100)the Korea Institute of Energy Technology Evaluation and Planning(KETEP),under the Ministry of Trade,Industry&Energy(MOTIE),Republic of Korea(20224C10300010)the KETEP grant funded by the MOTIE(20224000000440,Sector coupling energy industry advancement manpower training program)。
文摘The metal oxide promoter decisively influences the overall performance of Fe catalysts in the direct hydrogenation of CO_(2)to C_(5+)hydrocarbons.However,the roles of metal oxide promoter for Fe catalysts,particularly ZrO_(2),have rarely been investigated.To plug this knowledge gap,a new Fe catalyst promoted with Na and partially reduced ZrO_(x)(Na-FeZrO_(x-9))was developed in this study;the catalyst helped produce C_(5+)hydrocarbons in remarkably high yield(26.3%at 360℃).In contrast to ZrO_(x)-free Fe-oxide,NaFeZrO_(x)-9 exhibited long-term stability for CO_(2)hydrogenation(750 h on-stream).The findings revealed multiple roles of ZrO_(x).Notably,ZrO_(x)decorated the Fe-oxide particles after calcination,thereby suppressing excess particle aggregation during the reaction,and acted as a"coke remover"to eliminate the carbon deposited on the catalyst surface.Additionally,oxygen vacancy(O_(v))sites in ZrO_(x)and electron transfer from ZrO_(x)to Fe sites facilitated the adsorption of CO_(2)at the Zr-Fe interface.
基金Project supported by Shandong Provincial Natural Science Foundation,China(Grant No.ZR2022ME059)。
文摘Pd/Co_(2)MnSi(CMS)/Co/Pd multilayer films were designed based on the idea of combining highly spin-polarized materials with strong perpendicular magnetic anisotropy(PMA)films.The PMA of Pd/CMS/Co/Pd multilayer films was studied by optimizing the growth conditions and thickness of each film layer.The optimal structure of the multilayer films was Pd(6 nm)/CMS(5 nm)/Co(2 nm)/Pd(1 nm).Its abnormal Hall resistance(R_(Hall)),coercivity(H_(c))and effective magnetic anisotropy constant(Keff)are 0.08Ω,284 Oe and 1.36 Merg/cm^(3),respectively,which are 100%,492%,and 183%higher than the corresponding values(0.04Ω,48 Oe,and 0.48 Merg/cm^(3))of the Pd(6 nm)/Co(1 nm)/Pd(3 nm)trilayer films.The analysis shows that the increases of the above values are the result of the Pd/CMS interface effect and CMS/Co interface ferromagnetic(FM)coupling,and that it is closely related to the thickness of each film layer in the multilayer films and the growth conditions of the multilayer films.
基金supported by“National Natural Science Foundation of China(U21A20171,U20A20245)”“Hubei Provincial Natural Science Foundation of China(2023AFA010)”+1 种基金“Independent Innovation Projects of the Hubei Longzhong Laboratory(2022ZZ-09)”“Social Public Welfare and Basic Research Special Project of Zhongshan(2020B2015).”。
文摘Two-terminal(2-T)perovskite(PVK)/CuIn(Ga)Se_(2)(CIGS)tandem solar cells(TSCs)have been considered as an ideal tandem cell because of their best bandgap matching regarding to Shockley–Queisser(S–Q)limits.However,the nature of the irregular rough morphology of commercial CIGS prevents people from improving tandem device performances.In this paper,D-homoserine lactone hydrochloride is proven to improve coverage of PVK materials on irregular rough CIGS surfaces and also passivate bulk defects by modulating the growth of PVK crystals.In addition,the minority carriers near the PVK/C60 interface and the incompletely passivated trap states caused interface recombination.A surface reconstruction with 2-thiopheneethylammonium iodide and N,N-dimethylformamide assisted passivates the defect sites located at the surface and grain boundaries.Meanwhile,LiF is used to create this field effect,repelling hole carriers away from the PVK and C60 interface and thus reducing recombination.As a result,a 2-T PVK/CIGS tandem yielded a power conversion efficiency of 24.6%(0.16 cm^(2)),one of the highest results for 2-T PVK/CIGS TSCs to our knowledge.This validation underscores the potential of our methodology in achieving superior performance in PVK/CIGS tandem solar cells.
基金Incubation Program of Youth Innovation in Shandong ProvinceKey Research and Development Program of Shandong Province(2021TZXD007)。
文摘Food allergy has become a global concern.Spleen tyrosine kinase(SYK)inhibitors are promising therapeutics against allergic disorders.In this study,a total of 300 natural phenolic compounds were firstly subjected to virtual screening.Sesamin and its metabolites,sesamin monocatechol(SC-1)and sesamin dicatechol(SC-2),were identified as potential SYK inhibitors,showing high binding affinity and inhibition efficiency towards SYK.Compared with R406(a traditional SYK inhibitor),sesamin,SC-1,and SC-2 had lower binding energy and inhibition constant(Ki)during molecular docking,exhibited higher bioavailability,safety,metabolism/clearance rate,and distribution uniformity ADMET predictions,and showed high stability in occupying the ATP-binding pocket of SYK during molecular dynamics simulations.In anti-dinitrophenyl-immunoglobulin E(Anti-DNP-Ig E)/dinitrophenyl-human serum albumin(DNP-HSA)-stimulated rat basophilic leukemia(RBL-2H3)cells,sesamin in the concentration range of 5-80μmol/L influenced significantly the degranulation and cytokine release,with 54.00%inhibition againstβ-hexosaminidase release and 58.45%decrease in histamine.In BALB/c mice,sesamin could ameliorate Anti-DNP-Ig E/DNP-HSA-induced passive cutaneous anaphylaxis(PCA)and ovalbumin(OVA)-induced active systemic anaphylaxis(ASA)reactions,reduce the levels of allergic mediators(immunoglobulins and pro-inflammatory cytokines),partially correct the imbalance of T helper(Th)cells differentiation in the spleen,and inhibit the phosphorylation of SYK and its downstream signaling proteins,including p38 mitogen-activated protein kinases(p38 MAPK),extracellular signalregulated kinases(ERK),and p65 nuclear factor-κB(p65 NF-κB)in the spleen.Thus,sesamin may be a safe and versatile SYK inhibitor that can alleviate Ig E-mediated food allergies.
文摘目的分析免疫细胞CD8~+T细胞、CD4~+T细胞及高敏C反应蛋白(high sensitivity C-reactive protein,hs-CRP)与认知功能的关系,探讨免疫、慢性炎症与阿尔茨海默病相关认知障碍的关系。方法采用观察性研究设计中的横断面研究,选取2024年6~12月在北京中医药大学东直门医院阿尔茨海默病门诊就诊的101例患者,均主诉记忆力下降。采用简易智能状态检查量表(mini-mental state examination,MMSE)和延迟故事回忆量表(delayed story recall task,DSR)进行认知评估,分为观察组(伴认知障碍)60例和对照组(不伴认知障碍)41例,比较2组外周血CD8~+T细胞、CD4~+T细胞和hs-CRP水平。结果观察组MMSE评分及各子项目、DSR评分显著低于对照组,日常生活活动能力量表评分显著高于对照组,差异有统计学意义(P<0.05,P<0.01)。观察组外周血hs-CRP水平显著高于对照组(P<0.05)。二元logistic回归分析显示,CD8~+T细胞和体质量指数是认知障碍的保护因素(OR=0.998,95%CI:0.996~1.000,P=0.038;OR=0.843,95%CI:0.719~0.990,P=0.037),外周血hs-CRP水平是认知障碍的独立危险因素(OR=2.004,95%CI:1.215~3.306,P=0.006)。Spearman秩相关分析显示,hs-CRP水平与CD4~+T细胞呈显著正相关(P=0.011),与CD8~+T细胞无相关性(P>0.05)。结论慢性炎症与免疫失衡协同驱动认知衰退,hs-CRP可作为基层认知障碍筛查指标。
