Fluctuation in overlying water quality across multiple habitats and the reservoir conditions of different sediment pollutants significantly influence the“source-sink”effect of endogenous nutrients in shallow-water w...Fluctuation in overlying water quality across multiple habitats and the reservoir conditions of different sediment pollutants significantly influence the“source-sink”effect of endogenous nutrients in shallow-water wetlands.This study investigated the sediment nutrient composition in four habitats(i.e.open-water area,ditch,pond,and reed marsh)within Baiyangdian wetland(BYDW),combined with the simulated release experiment to estimate the nutrient exchange flux under the different overlying water qualities.The findings indicate that the nutrient contents of ditch sediments were significantly higher than those in the other habitats.The ditch overlying water exhibited significantly higher concentrations of soluble reactive phosphorus(SRP),total phosphorus(TP),and ammonia nitrogen(NH4+-N),and the maximum contents were 0.009 mg/L,0.0443 mg/L,and 0.4057 mg/L,respectively.Sediment horizon depth significantly influenced the composition of different P fractions.While residual phosphorus(Res-P)and calcium-bound phosphorus(Ca-P)comprised a substantial portion of TP,about 60.53%-79.46%.Sediments in ditch,pond,and reed marsh areas acted as TP sources under the raw water quality condition,and the releasing rate was 4.68,1.80,and 0.18 mg/(m2・day).The overlying water quality,sediment pH,organic matter(OM)content,as well as phosphorus speciation significantly influenced the exchange of phosphorus-containing substances.Both Chloroflexi and Proteobacteria significantly contributed to the degradation of sediment nutrients in open-water and reed areas.Ditch exhibited the highest TP release,with the release amount W(TP)varied from 64.15–72.17 t/yr.The ditch and pond areas exhibited relatively strong“source”potential,highlighting the need for effective management of endogenous pollution.展开更多
Nonlinear optical(NLO)materials play an increasingly important role in laser technology.Birefringence is one of the most important parameters for NLO materials to realize angle phase-matching conditions.In comparison ...Nonlinear optical(NLO)materials play an increasingly important role in laser technology.Birefringence is one of the most important parameters for NLO materials to realize angle phase-matching conditions.In comparison with other desirable optical properties,the availability of birefringence and refractive index dispersion is especially problematic owing to the strict requirements for single crystals.In this review,we described how to obtain the refractive index and birefringence of NLO materials from crystals sub-millimeters to centimeters in size.Espe-cially,recently developed methods including the minimum deflection angle method,auto-collimation method,prism coupling method,oil immersion technique,interference color method,and theoretical calculation(DFT)for rapid assessment of birefringence are summarized,the contents of which are mainly focused on the principles and typical applications,together with the advantages and drawbacks.In addition,representative examples of bire-fringent measurements were presented.The purpose of this work is to provide a useful perspective on the characterization of birefringence for NLO materials.It is hoped that this review can give a clear description of the birefringence measurements and accelerate the discovery of new NLO crystals.展开更多
novel visible-light induced phosphorylation cyclization to indole-fused medium-sized diazepines was established under room temperature.Broad substrate scope,good functional group compatibility,large-scale synthesis an...novel visible-light induced phosphorylation cyclization to indole-fused medium-sized diazepines was established under room temperature.Broad substrate scope,good functional group compatibility,large-scale synthesis and derivatization via nitration,chlorination and cyanation demonstrate the utility of this protocol.P-centered radical involed energy transfer(EnT)process was proposed based on radical inhibition experiments,visible-light irradiation on-off test,apparent quantum efficiency(AQE)calculation,UV-vis absorption spectroscopic studies and cyclic voltammetry experiments.展开更多
MicroRNA(miRNA),a crucial regulatory factor for maintaining homeostasis,is closely linked to the pathogenesis of numerous diseases.However,traditional miRNA detection technologies exhibit limitations,including low sel...MicroRNA(miRNA),a crucial regulatory factor for maintaining homeostasis,is closely linked to the pathogenesis of numerous diseases.However,traditional miRNA detection technologies exhibit limitations,including low selectivity and sensitivity.In this study,a dual-mode self-calibrated nanopore sensing system based on rolling circle amplification(RCA)and hydrophobic modification is proposed for the highly sensitive detection of miRNA-21.Binding of miRNA-21 activates the DNAzyme catalytic activity,which triggers the stepwise release of a fluorescent group.Concurrently,residual sequences on the nanopore surface catalyze the RCA reaction,increasing the density of negative charges and amplifying the current signal,with enhancements reaching up to 384%.Fitting the ratio of electrical and fluorescence signals to the Hill equation enables self-calibrated detection of miRNA-21,thereby effectively eliminating systematic errors.This system achieves a linear detection range for miRNA-21 from 1 pM to 100 nM in fluorescence assays and from 1 fM to 1 nM in electrochemical assays,with detection limits of 0.16 pM and 0.28 fM,respectively.Furthermore,this innovative approach enables sensitive detection of clinical serum samples with elevated miRNA-21 expression levels.The system holds potential applications in the field of biomedicine,particularly in advancing disease diagnosis.展开更多
This study focused on the pollution characteristics, influencing factors, and source apportionment of organophosphate triesters (tri-OPEs) and diesters (di-OPEs) in the plastic greenhouses soils with cultivation perio...This study focused on the pollution characteristics, influencing factors, and source apportionment of organophosphate triesters (tri-OPEs) and diesters (di-OPEs) in the plastic greenhouses soils with cultivation periods ranging from 6 to 32 years. The concentrations of Σ13tri-OPEs and Σ5di-OPEs in soil samples ranged from 39.60 to 730.52 ng/g dw and 2.25–6.94 ng/g dw, respectively. Tris (chloroethyl) phosphate was the predominant tri-OPE, while dibutyl phosphate was the most abundant di-OPE. The levels of OPEs pollution increased with the age of mulch film, highlighting the impact of the duration of mulch film usage on OPE accumulation. The type of fertilizer significantly impacted OPE levels. Soil samples treated with compound fertilizers showed the highest concentration of tri-OPEs, reaching up to 205.32 ng/g dry weight. In contrast, the highest concentration of di-OPEs was found in soil samples treated with water-soluble fertilizers, with a peak of 3.89 ng/g dry weight. Total organic carbon, pH, total nitrogen, and total phosphorus had minimal effect on OPEs levels. According to the Positive Matrix Factorization Model, the primary sources of OPEs included the use of pesticides, food packaging materials, and small-scale machinery (48.39 %), water and reclaimed water irrigation (17.68 %), the utilization of agricultural films (17.39 %), and atmospheric deposition and degradation processes (16.54 %). Compared to the moderate risks associated with compounds such as tri-2-ethyl phosphate, 2-ethylhexyl diphenyl phosphate, and tris(1-chloro-2-propyl) phosphate, tris(chloroethyl) phosphate exhibited a higher risk level in soil samples. This study offers insights into the potential risks linked to OPE contamination in agricultural soils.展开更多
TS-1 zeolite,celebrated for its superior catalytic performance in selective oxidation reactions,presents a significant challenge in optimizing the microstructure of its titanium active sites to maximize the efficiency...TS-1 zeolite,celebrated for its superior catalytic performance in selective oxidation reactions,presents a significant challenge in optimizing the microstructure of its titanium active sites to maximize the efficiency for specific applications.In this study,we successfully manipulated the microstructure of titanium species within TS-1 by kinetically controlling the crystallization process,thereby achieving the formation of poly-hexacoordinated Ti species in the initial amorphous titanosilicate phase and the construction of framework TiO4 species in fully crystallized TS-1 zeolite.Notably,the amorphous titanosilicate catalyst exhibited high efficiency in the oxidative desulfurization of dibenzothiophene,while showing negligible activity in 1-hexene epoxidation.Conversely,the crystalline TS-1 catalyst demonstrated outstanding performance in alkene epoxidation but limited efficacy in oxidative desulfurization.This study outlines a controlled crystallization process that allows precise tuning of zeolite active sites,thereby enhancing their catalytic effectiveness for targeted applications.展开更多
Comprehensive Summary The 21st century has witnessed a continuous evolution in the development of boron-stereogenic chemistry.Since the 1990s,various innovations for the synthesis of tetracoordinate boron-stereogenic ...Comprehensive Summary The 21st century has witnessed a continuous evolution in the development of boron-stereogenic chemistry.Since the 1990s,various innovations for the synthesis of tetracoordinate boron-stereogenic compounds,which exhibited great potential applications,have been demonstrated by synthetic chemists.This paper reviews the significant progress and recent advances towards the assembly of enantioenriched boron-stereogenic compounds,and hopes to shed light on new perspectives and inspire further research in this emerging field.展开更多
The poor temperature stability of the BaTiO3 ceramic has always been the main problem limiting their application.This situation has been improved but sacrifices the intrinsic polarization,which significantly reduce...The poor temperature stability of the BaTiO3 ceramic has always been the main problem limiting their application.This situation has been improved but sacrifices the intrinsic polarization,which significantly reduces the dielectric constant.In this work,the mechanism of multiple polarization was creatively introduced,and the temperature stability and dielectric properties of BaTiO3-based ceramics are simultaneously enhanced.In particular,the Ba0.9925Bi0.005Ti0.995Ca0.005O2.995(BBTC0.5)ceramic sample achieved excellent temperature stability(-14.8%to 8.85%)over an ultra-wide temperature range(-47 to 400℃)and exhibited colossal permittivity(27,125,25℃,1 kHz)and low dielectric loss(0.07,25℃,1 kHz).The dielectric properties,complex impedance spectra combined with XPS results indicate that the defective dipole clusters(Ti3+-VO-Ti3+,BiBa and Ca″Ti-VO)along with surface effects lead to colossal permittivity effect.More importantly,SEM images show the presence of the second phase at grain boundaries,which prevent the carriers within the grains from accumulating at the grain boundaries.As a result,the dielectric loss was reduced and the temperature stability was further extended.This strategy breaks the traditional limitation of singleoncomprehensive enhancement by singlepolarization mechanism,and is of great theoretical and practical significance to promote the research and application of high-performance BaTiO3-based ceramic materials.展开更多
The discovery of new infrared nonlinear optical(IR NLO)materials with a large second harmonic generation(SHG)effect and broad optical bandgap is still a challenging task.Based on this,we propose a rational strategy fo...The discovery of new infrared nonlinear optical(IR NLO)materials with a large second harmonic generation(SHG)effect and broad optical bandgap is still a challenging task.Based on this,we propose a rational strategy for the design of new NLO materials:(i)the coupling of stereochemically active lone-pair(SCALP)Sn(Ⅱ)cations and typical PS4units into a structure enhances the SHG response.展开更多
基金supported by the Core Talent Project under the Yanzhao Gold Terrace Attracting Talent Plan(Education Platform)of Hebei Province(No.HJZD202507)Hebei University 2025 youth talent support program,the Key Project of National Natural Science Foundation of China(No.42330705)Collaborative Innovation Center for Baiyangdian Basin Ecological Protection and Beijing-Tianjin-Hebei Sustainable Development.
摘要Fluctuation in overlying water quality across multiple habitats and the reservoir conditions of different sediment pollutants significantly influence the“source-sink”effect of endogenous nutrients in shallow-water wetlands.This study investigated the sediment nutrient composition in four habitats(i.e.open-water area,ditch,pond,and reed marsh)within Baiyangdian wetland(BYDW),combined with the simulated release experiment to estimate the nutrient exchange flux under the different overlying water qualities.The findings indicate that the nutrient contents of ditch sediments were significantly higher than those in the other habitats.The ditch overlying water exhibited significantly higher concentrations of soluble reactive phosphorus(SRP),total phosphorus(TP),and ammonia nitrogen(NH4+-N),and the maximum contents were 0.009 mg/L,0.0443 mg/L,and 0.4057 mg/L,respectively.Sediment horizon depth significantly influenced the composition of different P fractions.While residual phosphorus(Res-P)and calcium-bound phosphorus(Ca-P)comprised a substantial portion of TP,about 60.53%-79.46%.Sediments in ditch,pond,and reed marsh areas acted as TP sources under the raw water quality condition,and the releasing rate was 4.68,1.80,and 0.18 mg/(m2・day).The overlying water quality,sediment pH,organic matter(OM)content,as well as phosphorus speciation significantly influenced the exchange of phosphorus-containing substances.Both Chloroflexi and Proteobacteria significantly contributed to the degradation of sediment nutrients in open-water and reed areas.Ditch exhibited the highest TP release,with the release amount W(TP)varied from 64.15–72.17 t/yr.The ditch and pond areas exhibited relatively strong“source”potential,highlighting the need for effective management of endogenous pollution.
基金supported by the National Natural Science Foundation of China(Grant No.21975062)Hebei Province Outstanding Youth Fund(Grant No.E2020201003)+1 种基金Science and Technology Project of Hebei Education Department(Grant Nos.ZD2022156,BJ2020020)Key Projects of Scientific Research and Cultivation Fund of Baoding University(Grant No.2022Z01).
摘要Nonlinear optical(NLO)materials play an increasingly important role in laser technology.Birefringence is one of the most important parameters for NLO materials to realize angle phase-matching conditions.In comparison with other desirable optical properties,the availability of birefringence and refractive index dispersion is especially problematic owing to the strict requirements for single crystals.In this review,we described how to obtain the refractive index and birefringence of NLO materials from crystals sub-millimeters to centimeters in size.Espe-cially,recently developed methods including the minimum deflection angle method,auto-collimation method,prism coupling method,oil immersion technique,interference color method,and theoretical calculation(DFT)for rapid assessment of birefringence are summarized,the contents of which are mainly focused on the principles and typical applications,together with the advantages and drawbacks.In addition,representative examples of bire-fringent measurements were presented.The purpose of this work is to provide a useful perspective on the characterization of birefringence for NLO materials.It is hoped that this review can give a clear description of the birefringence measurements and accelerate the discovery of new NLO crystals.
摘要novel visible-light induced phosphorylation cyclization to indole-fused medium-sized diazepines was established under room temperature.Broad substrate scope,good functional group compatibility,large-scale synthesis and derivatization via nitration,chlorination and cyanation demonstrate the utility of this protocol.P-centered radical involed energy transfer(EnT)process was proposed based on radical inhibition experiments,visible-light irradiation on-off test,apparent quantum efficiency(AQE)calculation,UV-vis absorption spectroscopic studies and cyclic voltammetry experiments.
基金financially supported by the National Natural Science Foundation of China(22176080 and 32401191)Natural Science Foundation of Shandong Province(ZR2023YQ015)+5 种基金Natural Science Foundation of Hebei Province(B2024201050)Hebei Province Innovation Capability Enhancement Plan Project(22567620H)Research and Innovation Team of Hebei University(IT2023A03)Natural Science Interdisciplinary Research Program of Hebei University(DXK202307)Taishan Scholar Project of Shandong Province(tsqn202312216)the Foundation of Hebei University(050001-513300201004)。
摘要MicroRNA(miRNA),a crucial regulatory factor for maintaining homeostasis,is closely linked to the pathogenesis of numerous diseases.However,traditional miRNA detection technologies exhibit limitations,including low selectivity and sensitivity.In this study,a dual-mode self-calibrated nanopore sensing system based on rolling circle amplification(RCA)and hydrophobic modification is proposed for the highly sensitive detection of miRNA-21.Binding of miRNA-21 activates the DNAzyme catalytic activity,which triggers the stepwise release of a fluorescent group.Concurrently,residual sequences on the nanopore surface catalyze the RCA reaction,increasing the density of negative charges and amplifying the current signal,with enhancements reaching up to 384%.Fitting the ratio of electrical and fluorescence signals to the Hill equation enables self-calibrated detection of miRNA-21,thereby effectively eliminating systematic errors.This system achieves a linear detection range for miRNA-21 from 1 pM to 100 nM in fluorescence assays and from 1 fM to 1 nM in electrochemical assays,with detection limits of 0.16 pM and 0.28 fM,respectively.Furthermore,this innovative approach enables sensitive detection of clinical serum samples with elevated miRNA-21 expression levels.The system holds potential applications in the field of biomedicine,particularly in advancing disease diagnosis.
基金supported by Natural Science Foundation of Hebei Province(No.B2024201033)Natural Science Interdisciplinary Research Program of Hebei University(DXK202302)National Natural Science Foundation of China(Nos.42077369,42477444).
摘要This study focused on the pollution characteristics, influencing factors, and source apportionment of organophosphate triesters (tri-OPEs) and diesters (di-OPEs) in the plastic greenhouses soils with cultivation periods ranging from 6 to 32 years. The concentrations of Σ13tri-OPEs and Σ5di-OPEs in soil samples ranged from 39.60 to 730.52 ng/g dw and 2.25–6.94 ng/g dw, respectively. Tris (chloroethyl) phosphate was the predominant tri-OPE, while dibutyl phosphate was the most abundant di-OPE. The levels of OPEs pollution increased with the age of mulch film, highlighting the impact of the duration of mulch film usage on OPE accumulation. The type of fertilizer significantly impacted OPE levels. Soil samples treated with compound fertilizers showed the highest concentration of tri-OPEs, reaching up to 205.32 ng/g dry weight. In contrast, the highest concentration of di-OPEs was found in soil samples treated with water-soluble fertilizers, with a peak of 3.89 ng/g dry weight. Total organic carbon, pH, total nitrogen, and total phosphorus had minimal effect on OPEs levels. According to the Positive Matrix Factorization Model, the primary sources of OPEs included the use of pesticides, food packaging materials, and small-scale machinery (48.39 %), water and reclaimed water irrigation (17.68 %), the utilization of agricultural films (17.39 %), and atmospheric deposition and degradation processes (16.54 %). Compared to the moderate risks associated with compounds such as tri-2-ethyl phosphate, 2-ethylhexyl diphenyl phosphate, and tris(1-chloro-2-propyl) phosphate, tris(chloroethyl) phosphate exhibited a higher risk level in soil samples. This study offers insights into the potential risks linked to OPE contamination in agricultural soils.
基金the National Natural Science Foundation of China(Grant No.22201094)the Jilin Youth Growth Science and Technology Plan Project(Grant No.20230508189RC).
摘要TS-1 zeolite,celebrated for its superior catalytic performance in selective oxidation reactions,presents a significant challenge in optimizing the microstructure of its titanium active sites to maximize the efficiency for specific applications.In this study,we successfully manipulated the microstructure of titanium species within TS-1 by kinetically controlling the crystallization process,thereby achieving the formation of poly-hexacoordinated Ti species in the initial amorphous titanosilicate phase and the construction of framework TiO4 species in fully crystallized TS-1 zeolite.Notably,the amorphous titanosilicate catalyst exhibited high efficiency in the oxidative desulfurization of dibenzothiophene,while showing negligible activity in 1-hexene epoxidation.Conversely,the crystalline TS-1 catalyst demonstrated outstanding performance in alkene epoxidation but limited efficacy in oxidative desulfurization.This study outlines a controlled crystallization process that allows precise tuning of zeolite active sites,thereby enhancing their catalytic effectiveness for targeted applications.
基金the National Natural Science Foundation of China(22122102,22271134)Guangdong Provincial Key Laboratory of Catalysis(2020B121201002)+2 种基金Guangdong Pearl River Talent Program(2019QN01Y628)Shenzhen Scienceand TechnologyyInnovationCommittee(RCJC20221008092723013,JCYJ20230807093104009)Hebei ProvinceInnovationCapability Enhancement Plan Project(22567632H).
摘要Comprehensive Summary The 21st century has witnessed a continuous evolution in the development of boron-stereogenic chemistry.Since the 1990s,various innovations for the synthesis of tetracoordinate boron-stereogenic compounds,which exhibited great potential applications,have been demonstrated by synthetic chemists.This paper reviews the significant progress and recent advances towards the assembly of enantioenriched boron-stereogenic compounds,and hopes to shed light on new perspectives and inspire further research in this emerging field.
基金supported by the Natural Science Foundation of Hebei province(E2020201021 and E2023201019)Hebei Province Innovation Capability Enhancement Plan Project(22567620H)+2 种基金Industry-University-Research Cooperation Project of Colleges and Universities in Hebei Province(CXZX2025016)Industry-University-Research Cooperation Major Projects of Shijiazhuang City(241130477A)Research Innovation Team of College of Chemistry and Environmental Science of Hebei University(hxkytd2102).
摘要The poor temperature stability of the BaTiO3 ceramic has always been the main problem limiting their application.This situation has been improved but sacrifices the intrinsic polarization,which significantly reduces the dielectric constant.In this work,the mechanism of multiple polarization was creatively introduced,and the temperature stability and dielectric properties of BaTiO3-based ceramics are simultaneously enhanced.In particular,the Ba0.9925Bi0.005Ti0.995Ca0.005O2.995(BBTC0.5)ceramic sample achieved excellent temperature stability(-14.8%to 8.85%)over an ultra-wide temperature range(-47 to 400℃)and exhibited colossal permittivity(27,125,25℃,1 kHz)and low dielectric loss(0.07,25℃,1 kHz).The dielectric properties,complex impedance spectra combined with XPS results indicate that the defective dipole clusters(Ti3+-VO-Ti3+,BiBa and Ca″Ti-VO)along with surface effects lead to colossal permittivity effect.More importantly,SEM images show the presence of the second phase at grain boundaries,which prevent the carriers within the grains from accumulating at the grain boundaries.As a result,the dielectric loss was reduced and the temperature stability was further extended.This strategy breaks the traditional limitation of singleoncomprehensive enhancement by singlepolarization mechanism,and is of great theoretical and practical significance to promote the research and application of high-performance BaTiO3-based ceramic materials.
基金supported by the National Natural Science Foundation of China(Grant Nos.52372009,51872324)the Natural Science Foundation of Hebei Province(Grant No.E2020201005)+1 种基金the Science Foundation for Distinguished Young Scholars of Hebei Province(B2021201045)the Central Guidance on Local Science and Technology Development Fund of Hebei Province(226Z2402G).
摘要The discovery of new infrared nonlinear optical(IR NLO)materials with a large second harmonic generation(SHG)effect and broad optical bandgap is still a challenging task.Based on this,we propose a rational strategy for the design of new NLO materials:(i)the coupling of stereochemically active lone-pair(SCALP)Sn(Ⅱ)cations and typical PS4units into a structure enhances the SHG response.