Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen production.In this study,a Schottky heterojunction has been successfully cons...Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen production.In this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine PtNPs onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small PtNPs while maximizing the utilization of the Pt active sites.The fabricated PtNPs@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%Pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine CTF-1.Theoretical calculations revealed that the strong electron transfer(Q(Pt)=−0.726 qe,in the analysis of Bader charge,Q(Pt)is the charge quantity transferred from Pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between PtNPs and CTF-1 triggers a strong interaction,which makes PtNPs being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production efficiency.Importantly,the hydrogen binding free energy(ΔGH*)of PtNPs@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic performance.The overall findings of this work provide a new platform to incorporate metallic NPs into COFs for the design and fabrication of highly efficient photocatalysts.展开更多
Polyoxometalates(POMs)are classified as solid superacids which can exhibit notable proton conductivity,making them a promising functional inorganic filler for enhancing the proton conductivity of proton exchange membr...Polyoxometalates(POMs)are classified as solid superacids which can exhibit notable proton conductivity,making them a promising functional inorganic filler for enhancing the proton conductivity of proton exchange membranes(PEMs).In this study,a series of hybrid membranes were obtained by molecular-level hybridization of Weakley-type POM Na_(7)H_(2)LaW_(10)O_(36)(LaW_(10))clusters into sulfonated poly(aryl ether ketone sulfone)(SPAEKS).All hybrid membranes exhibited greater proton conductivity than the pristine membrane in the 30–80℃temperature range.When the doping amount of LaW 10 reached 7 wt.%,the proton conductivity of M-LaW 10^(-7)achieved 64 mS·cm^(−1)at 80℃.Lanthanide ions'high coordination number property and variable coordination environment can aid to attract more water molecules from the environment.LaW 10 and these bound water can construct denser hydrogen bonds with–SO_(3)H of SPAEKS.These intensive hydrogen bonds will facilitate the constitution of more continuous proton transport channels,and improve the proton conductivity of the hybrid membrane.This work off ers a fresh approach to using POMs containing rare-earth components in PEMs.展开更多
Background:The incidence of brucellosis,which is caused by the Brucella species of bacteria,is rapidly rising worldwide;however,few studies have investigated the immune response to this pathogen and clinical biochemic...Background:The incidence of brucellosis,which is caused by the Brucella species of bacteria,is rapidly rising worldwide;however,few studies have investigated the immune response to this pathogen and clinical biochemical features.In this paper,we examined the levels of various cytokines and inflammatory factors as well as clinical course characteristics in patients with brucellosis,in order to provide evidence for the diagnosis,assessment,and prognosis of this infectious disease.Methods:A total of 191 brucellosis inpatients(50 acute cases and 141 chronic cases),as well as 60 healthy control subjects,were included in the analysis.We investigated changes in the levels of six cytokines(IL-4,IL-6,IL-10,IL-17,TNF-α,INF-γ)and related clinical biochemical markers in patients with acute and chronic brucellosis in Xinjiang,China.Possible factors were statistically analyzed using the t test,χ2 test,z test and a multivariate logistic stepwise regression test.Results:We found that IL-4,IL-6,IL-10,IL-17,IFN-γ,and TNF-αlevels were higher in those with brucellosis than in controls(P<0.05).With regard to disease progression,procalcitonin(PCT)and C-reactive protein(CRP)levels were significantly higher in those with an acute infection compared to chronic cases(P<0.05).We found that the expression of all six cytokines tested was closely related to the degree of brucellosis using univariate logistic regression;however,only IL-6 and INF-γlevels were independent factors associated with the severity of brucellosis.Conclusions:Assessing cytokine levels in patients with acute and chronic brucellosis is not only useful for detecting the immune response,but can also be indicative of the severity of brucellosis.In particular,we propose IL-6 and INF-γlevels may be useful independent predictive factors in the clinical evaluation and diagnosis of brucellosis.展开更多
In the field of proton exchange membranes(PEMs),it is still a great challenge to explore new Nafion alternatives,maintaining the high proton conductivity and lowering the cost of practical application.In this work,a s...In the field of proton exchange membranes(PEMs),it is still a great challenge to explore new Nafion alternatives,maintaining the high proton conductivity and lowering the cost of practical application.In this work,a series of low sulfonated poly(aryl ether ketone sulfone)(SPAEKS)membranes hybridized by[Bi_(6)O_(5)(OH)_(3)]_(2)(NO_(3))10⋅6H_(2)O(H_(6)Bi_(12)O_(16))have been successfully fabricated.When the doping amount of H6Bi12O16 reaches 5 wt%,the DS15-Bi12-5 showing the best proton conductive ability and mechanical properties.The proton conductivity can achieve 72.8 mS⋅cm−1 at 80℃ and the tensile strength can reach 43.57 MPa.Confirmed by experimental data and activation energy(Ea)calculations,the existence of Bi cluster makes more hydrogen bonds,providing additional proton hopping sites and offers more proton transport vehicles,leading to a high proton conduction performance.This work proved that polyoxometalates(POMs)can replace the role of sulfonate groups in SPAEKS to a certain extent and work out the defects of high sulfonation,making a remarkable contribution to the practical application of low sulfonated SPAEKS.展开更多
基金the National Natural Science Foundation of China(Nos.22271022 and 21701016)the Science and Technology Development Planning of Jilin Province(No.YDZJ202201ZYTS342)+1 种基金the China Scholarship Council(CSC No.201802335014)Partial support from the Robert A.Welch Foundation(B-0027)(S.M.)and Researchers Supporting Program(No.RSP-2024R55)at King Saud University,Riyadh,Saudi Arabia is also acknowledged.
文摘Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen production.In this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine PtNPs onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small PtNPs while maximizing the utilization of the Pt active sites.The fabricated PtNPs@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%Pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine CTF-1.Theoretical calculations revealed that the strong electron transfer(Q(Pt)=−0.726 qe,in the analysis of Bader charge,Q(Pt)is the charge quantity transferred from Pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between PtNPs and CTF-1 triggers a strong interaction,which makes PtNPs being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production efficiency.Importantly,the hydrogen binding free energy(ΔGH*)of PtNPs@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic performance.The overall findings of this work provide a new platform to incorporate metallic NPs into COFs for the design and fabrication of highly efficient photocatalysts.
基金financially supported by the National Natural Science Foundation of China(No.22271022)the Natural Science Foundation of Jilin Province(No.YDZJ202201ZYTS342)supported by the China Scholarship Council(CSC No.201802335014).
文摘Polyoxometalates(POMs)are classified as solid superacids which can exhibit notable proton conductivity,making them a promising functional inorganic filler for enhancing the proton conductivity of proton exchange membranes(PEMs).In this study,a series of hybrid membranes were obtained by molecular-level hybridization of Weakley-type POM Na_(7)H_(2)LaW_(10)O_(36)(LaW_(10))clusters into sulfonated poly(aryl ether ketone sulfone)(SPAEKS).All hybrid membranes exhibited greater proton conductivity than the pristine membrane in the 30–80℃temperature range.When the doping amount of LaW 10 reached 7 wt.%,the proton conductivity of M-LaW 10^(-7)achieved 64 mS·cm^(−1)at 80℃.Lanthanide ions'high coordination number property and variable coordination environment can aid to attract more water molecules from the environment.LaW 10 and these bound water can construct denser hydrogen bonds with–SO_(3)H of SPAEKS.These intensive hydrogen bonds will facilitate the constitution of more continuous proton transport channels,and improve the proton conductivity of the hybrid membrane.This work off ers a fresh approach to using POMs containing rare-earth components in PEMs.
基金This study was funded by grants from Major Infectious Diseases such as AIDS and Viral Hepatitis Prevention and Control technology major projects(2018ZX10101002 and 2018ZX10201002).
文摘Background:The incidence of brucellosis,which is caused by the Brucella species of bacteria,is rapidly rising worldwide;however,few studies have investigated the immune response to this pathogen and clinical biochemical features.In this paper,we examined the levels of various cytokines and inflammatory factors as well as clinical course characteristics in patients with brucellosis,in order to provide evidence for the diagnosis,assessment,and prognosis of this infectious disease.Methods:A total of 191 brucellosis inpatients(50 acute cases and 141 chronic cases),as well as 60 healthy control subjects,were included in the analysis.We investigated changes in the levels of six cytokines(IL-4,IL-6,IL-10,IL-17,TNF-α,INF-γ)and related clinical biochemical markers in patients with acute and chronic brucellosis in Xinjiang,China.Possible factors were statistically analyzed using the t test,χ2 test,z test and a multivariate logistic stepwise regression test.Results:We found that IL-4,IL-6,IL-10,IL-17,IFN-γ,and TNF-αlevels were higher in those with brucellosis than in controls(P<0.05).With regard to disease progression,procalcitonin(PCT)and C-reactive protein(CRP)levels were significantly higher in those with an acute infection compared to chronic cases(P<0.05).We found that the expression of all six cytokines tested was closely related to the degree of brucellosis using univariate logistic regression;however,only IL-6 and INF-γlevels were independent factors associated with the severity of brucellosis.Conclusions:Assessing cytokine levels in patients with acute and chronic brucellosis is not only useful for detecting the immune response,but can also be indicative of the severity of brucellosis.In particular,we propose IL-6 and INF-γlevels may be useful independent predictive factors in the clinical evaluation and diagnosis of brucellosis.
基金NationalNatural Science Foundation of China,Grant/Award Numbers:21701016,51803011Science and Technology Development Planning of Jilin Province,Grant/Award Number:20190103129JH+2 种基金Education Department of Jilin Province,Grant/Award Number:JJKH20200666KJChina Scholarship Council,Grant/Award Number:201802335014Welch Foundation,Grant/Award Number:B-0027。
文摘In the field of proton exchange membranes(PEMs),it is still a great challenge to explore new Nafion alternatives,maintaining the high proton conductivity and lowering the cost of practical application.In this work,a series of low sulfonated poly(aryl ether ketone sulfone)(SPAEKS)membranes hybridized by[Bi_(6)O_(5)(OH)_(3)]_(2)(NO_(3))10⋅6H_(2)O(H_(6)Bi_(12)O_(16))have been successfully fabricated.When the doping amount of H6Bi12O16 reaches 5 wt%,the DS15-Bi12-5 showing the best proton conductive ability and mechanical properties.The proton conductivity can achieve 72.8 mS⋅cm−1 at 80℃ and the tensile strength can reach 43.57 MPa.Confirmed by experimental data and activation energy(Ea)calculations,the existence of Bi cluster makes more hydrogen bonds,providing additional proton hopping sites and offers more proton transport vehicles,leading to a high proton conduction performance.This work proved that polyoxometalates(POMs)can replace the role of sulfonate groups in SPAEKS to a certain extent and work out the defects of high sulfonation,making a remarkable contribution to the practical application of low sulfonated SPAEKS.
