As one of the pentlandites,Fe5Ni4S8(FNS) based materials have attracted increasing attention due to their excellent catalytic properties and promising applicability.The control over the catalyst surface structure ofte...As one of the pentlandites,Fe5Ni4S8(FNS) based materials have attracted increasing attention due to their excellent catalytic properties and promising applicability.The control over the catalyst surface structure often benefits its heterogeneous catalytic activity.However,this has not been investigated for FNS materials at the nanoscale regarding the catalytic activity related to high-index facets.Herein,FNS nanoparticles(FNSNPs) with enclosed continuous tunable high-index facets were prepared and studied to clarify the relationship between the structure and catalytic functionality.The results suggested strong dependence between exposed facets of FNSNPs and their sizes.The decline in the average size to5.8 nm led to enclosing by high-index facets(422) and(511) to yield optimal electrocatalytic activities toward the hydrogen evolution reaction.The catalytic activity of FNSNPs was closely related to the surface energy of the main exposed facets.These findings clarified the relationship between high-index-facet and high-surface-energy FNSNPs,as promising approaches in crystal surface control engineering.展开更多
During oxygen evolution reaction(OER),complex changes have been reported on surfaces of bimetallic Fe-Ni-based catalysts,and regulating the dynamic evolution could improve their electrocatalytic performances.Herein,a ...During oxygen evolution reaction(OER),complex changes have been reported on surfaces of bimetallic Fe-Ni-based catalysts,and regulating the dynamic evolution could improve their electrocatalytic performances.Herein,a pyrrolidone-promoted reconstruction of pentlandite was investigated to uncover the correlation between the reconstructed surface and the OER performance.The theoretical calculations indicated the preferential implantation of pyrrolidone at Fe atoms,useful for regulating the electronic structures of pentlandite.The vale nce state of Ni increased,suggesting the promotion of the in-situ reconstruction of pentlandite via strengthening hydroxyl adsorption to generate highly active NiOOH.The electron-rich pentlandite was also found conducive to charge transfer under applied voltages.The Operando Raman and various quasi-in-situ characterizations confirmed the realization of more delocalized electronic structures of pentlandite by introducing pyrrolidone.This,in turn,promoted the accumulation of hydroxyl groups on the pentlandite surface,thereby boosting the formation of highly active NiOOH at lower OER potentials.Consequently,the adsorption energies of intermediates were optimized,conducive to enhanced OER reaction kinetics.As a proof of concept,the pentlandite decorated by pyrrolidone exhibited an overpotential as low as 265 mV at 10 mA cm^(-2) coupled with stable catalysis for 1000 hours at a high current density of 100 mA cm^(-2).In sum,new insights into unlocking the high catalytic activity of bimetallic Fe-Ni-based catalysts were provided,promising for future synthesis of advanced catalysts.展开更多
[Objectives]This study was conducted to develop an enzyme-linked immunoassay kit that can detect the residual amount of pentachloronitrobenzene in Penaeus vannamei.[Methods]This study was conducted to develop an enzym...[Objectives]This study was conducted to develop an enzyme-linked immunoassay kit that can detect the residual amount of pentachloronitrobenzene in Penaeus vannamei.[Methods]This study was conducted to develop an enzyme-linked immunoassay kit that can detect the residual amount of pentachloronitrobenzene in P.vannamei.[Results]The standard curve range of the kit was 0-8.1μg/L;the detection limit for P.vannamei was 0.912μg/kg;the recovery was 80.6%-103.5%;and the relative standard deviation range within batches was 5.3%-10.1%,and the relative standard deviation range between batches was 6.7%-8.1%.The specificity of the pentachloronitrobenzene monoclonal antibody was relatively good,and the cross-reaction rates with pentachlorophenol,hexachlorobenzene,tetrachlorophthalide,and chlorothalonil were low,all of which did not exceed 30%.The ELISA kit could be stored at 4℃for 12 months,showing good stability.[Conclusions]The detection kit has low cost,short time and small deviation,and is an ideal preliminary screening method.展开更多
Background:The Global Initiative for Chronic Obstructive Lung Disease(GOLD)2017 proposed a new classification that reclassified many chronic obstructive pulmonary disease(COPD)patients from group D to B.However,there ...Background:The Global Initiative for Chronic Obstructive Lung Disease(GOLD)2017 proposed a new classification that reclassified many chronic obstructive pulmonary disease(COPD)patients from group D to B.However,there is a paucity of data related to the comparison between reclassified and non-reclassified COPD patients in terms of long-term prognosis.This study aimed to investigate long-term outcomes of them and determine whether the GOLD 2017 revision improved the assessment of COPD patients.Methods:This observational,multicenter,prospective study recruited outpatients at 12 tertiary hospitals in China from November 2016 to February 2018 and followed them up until February 2022.All enrolled patients were classified into groups A toDbased on GOLD 2017,and the subjects in group B included patients reclassified from group D to B(group DB)and those remaining in group B(group BB).Incidence rates and hazard ratios(HRs)were calculated for the exacerbation of COPD and hospitalization in each group.Results:We included and followed up 845 patients.During the first year of follow-up,the GOLD 2017 classification had a better discrimination ability for different risks of COPD exacerbation and hospitalization than GOLD 2013.Group DB was associated with a higher risk of moderate-to-severe exacerbation(HR=1.88,95%confidence interval[CI]=1.37-2.59,P<0.001)and hospitalization for COPD exacerbation(HR=2.23,95%CI=1.29-3.85,P=0.004)than group BB.However,during the last year of follow-up,the differences in the risks of frequent exacerbations and hospitalizations between group DB and BB were not statistically significant(frequent exacerbations:HR=1.02,95%CI=0.51-2.03,P=0.955;frequent hospitalizations:HR=1.66,95%CI=0.58-4.78,P=0.348).The mortality rates of the two groups were both approximately 9.0%during the entire follow-up period.Conclusions:The long-term prognosis of patients reclassified into group B and of those remaining in group B was similar,although patients reclassified from group D to group B had worse short-term outcomes.The GOLD 2017 revision could improve the assessment of Chinese COPD patients in terms of long-term prognosis.展开更多
The well completion process in oil and gas industry,aiming to build effective exploitation,is divided into acidizing and formation water production process.Oxide scale(OS)formed on the inner wall of the HP-13Cr stainl...The well completion process in oil and gas industry,aiming to build effective exploitation,is divided into acidizing and formation water production process.Oxide scale(OS)formed on the inner wall of the HP-13Cr stainless steel tubes during the hot extrusion process changes the surface roughness.The effects of OS on the corrosion of HP-13Cr stainless steel during well completion process were studied by corrosion measurement,spectra analysis,microscopic observation and numerical simulation.The results indicate that the OS make no change of phase distribution and element composition of corrosion scale,while the increasing OS roughness is the dominant factor for accelerating corrosion rate during the well completion process.In acidizing process,the greater surface roughness OS of HP-13Cr stainless steel increases the corrosion rate obviously due to a larger interfacial area in contact with the aggressive environment.During subsequent formation water production process,the turbulence eddy,formed at locations characterized with greater surface roughness OS,can deteriorate the corrosion scale and accelerate the mass transfer of the corrosive species,resulting in more serious corrosion.展开更多
Three imidazole-modified Ag-polyoxovanadates frameworks(APFs)with a controllable molar ratio of Ag+to polyoxovanadates(POVs)[Ag(IM)_(2)]_(2)V_(4)O_(12)·2Ag(IM)_(2)(APF-1),[Ag_(2)(1-eIM)_(4)]_(2)[Ag(1-eIM)_(2)]_(3...Three imidazole-modified Ag-polyoxovanadates frameworks(APFs)with a controllable molar ratio of Ag+to polyoxovanadates(POVs)[Ag(IM)_(2)]_(2)V_(4)O_(12)·2Ag(IM)_(2)(APF-1),[Ag_(2)(1-eIM)_(4)]_(2)[Ag(1-eIM)_(2)]_(3)·2Ag(1-eIM)_(2)·3(1-HeIM)[V_(10)O_(28)]_(2)(APF-2)and[Ag(1-pIM)_(2)]_(3)[HV_(10)O_(28)]·2Ag(1-pIM)_(2)·2H_(2)O(APF-3)(IM=imida-zole;1-eIM=1-ethylimidazole and 1-pIM=1-propylimidazole)have been successfully achieved by self-assembly of POVs,Ag+cations,and three different imidazole derivatives.Interestingly,the molar ratios of Ag+to POVs vary from 4:1,4.5:1 to 5:1 by changing the vanadium resources and imidazole deriva-tives.Notably,the coordination environment of Ag+cations and the structure of POVs in the APFs are also different.Specifically,for APF-1,the four Ag atoms adopt three-coordinated and four-coordinated geometries,respectively,and Ag-imidazole complexes and[V_(4)O 1_(2)]_(4)−cluster form the one-dimensional polymeric chains.While Ag atoms in APF-2 and APF-3 exhibit two-,four-and five-coordinated geome-tries for APF-2,four-,five-and six-coordinated geometries for APF-3,respectively.These Ag+cations and decavanadate clusters are assembled into the 2D supramolecular structure through the Ag-O bonds and Ag…Ag argentophilic interaction.Remarkably,thus-obtained APF-2 can serve as powerful efficient hetero-geneous catalyst for construction of C–N bond and detoxification of simulant sulfur mustard(yields up to 99%),which enable successful recycling for three cycles with remained catalytic activities and structure stability.展开更多
基金financially supported by the Scientific and Technological Development Program of Jilin Province(Grant No.20220201138GX)the Project for Self-innovation Ability Construction of Jilin Province Development and Reform Commission(Grant No.2021C026)the Project Supported by Graduate Innovation Fund of Jilin University。
文摘As one of the pentlandites,Fe5Ni4S8(FNS) based materials have attracted increasing attention due to their excellent catalytic properties and promising applicability.The control over the catalyst surface structure often benefits its heterogeneous catalytic activity.However,this has not been investigated for FNS materials at the nanoscale regarding the catalytic activity related to high-index facets.Herein,FNS nanoparticles(FNSNPs) with enclosed continuous tunable high-index facets were prepared and studied to clarify the relationship between the structure and catalytic functionality.The results suggested strong dependence between exposed facets of FNSNPs and their sizes.The decline in the average size to5.8 nm led to enclosing by high-index facets(422) and(511) to yield optimal electrocatalytic activities toward the hydrogen evolution reaction.The catalytic activity of FNSNPs was closely related to the surface energy of the main exposed facets.These findings clarified the relationship between high-index-facet and high-surface-energy FNSNPs,as promising approaches in crystal surface control engineering.
基金financially supported by the Scientific and Technological Development Program of Jilin Province (20220201138GX)。
文摘During oxygen evolution reaction(OER),complex changes have been reported on surfaces of bimetallic Fe-Ni-based catalysts,and regulating the dynamic evolution could improve their electrocatalytic performances.Herein,a pyrrolidone-promoted reconstruction of pentlandite was investigated to uncover the correlation between the reconstructed surface and the OER performance.The theoretical calculations indicated the preferential implantation of pyrrolidone at Fe atoms,useful for regulating the electronic structures of pentlandite.The vale nce state of Ni increased,suggesting the promotion of the in-situ reconstruction of pentlandite via strengthening hydroxyl adsorption to generate highly active NiOOH.The electron-rich pentlandite was also found conducive to charge transfer under applied voltages.The Operando Raman and various quasi-in-situ characterizations confirmed the realization of more delocalized electronic structures of pentlandite by introducing pyrrolidone.This,in turn,promoted the accumulation of hydroxyl groups on the pentlandite surface,thereby boosting the formation of highly active NiOOH at lower OER potentials.Consequently,the adsorption energies of intermediates were optimized,conducive to enhanced OER reaction kinetics.As a proof of concept,the pentlandite decorated by pyrrolidone exhibited an overpotential as low as 265 mV at 10 mA cm^(-2) coupled with stable catalysis for 1000 hours at a high current density of 100 mA cm^(-2).In sum,new insights into unlocking the high catalytic activity of bimetallic Fe-Ni-based catalysts were provided,promising for future synthesis of advanced catalysts.
基金Key R&D Program of Hebei Province:Special Project on Key Common Technologies for High-quality Agricultural Development(20327505D).
文摘[Objectives]This study was conducted to develop an enzyme-linked immunoassay kit that can detect the residual amount of pentachloronitrobenzene in Penaeus vannamei.[Methods]This study was conducted to develop an enzyme-linked immunoassay kit that can detect the residual amount of pentachloronitrobenzene in P.vannamei.[Results]The standard curve range of the kit was 0-8.1μg/L;the detection limit for P.vannamei was 0.912μg/kg;the recovery was 80.6%-103.5%;and the relative standard deviation range within batches was 5.3%-10.1%,and the relative standard deviation range between batches was 6.7%-8.1%.The specificity of the pentachloronitrobenzene monoclonal antibody was relatively good,and the cross-reaction rates with pentachlorophenol,hexachlorobenzene,tetrachlorophthalide,and chlorothalonil were low,all of which did not exceed 30%.The ELISA kit could be stored at 4℃for 12 months,showing good stability.[Conclusions]The detection kit has low cost,short time and small deviation,and is an ideal preliminary screening method.
基金supported by grants from the National Natural Science Foundation of China(Nos.81873410,81800043,and 82070049)the National Key R&D Program of China(No.2016YFC1304700)+1 种基金the Natural Science Foundation of Hunan Province(No.2020JJ5818)the Fundamental Research Funds for the Central Universities of Central South University(No.2021zzts0389).
文摘Background:The Global Initiative for Chronic Obstructive Lung Disease(GOLD)2017 proposed a new classification that reclassified many chronic obstructive pulmonary disease(COPD)patients from group D to B.However,there is a paucity of data related to the comparison between reclassified and non-reclassified COPD patients in terms of long-term prognosis.This study aimed to investigate long-term outcomes of them and determine whether the GOLD 2017 revision improved the assessment of COPD patients.Methods:This observational,multicenter,prospective study recruited outpatients at 12 tertiary hospitals in China from November 2016 to February 2018 and followed them up until February 2022.All enrolled patients were classified into groups A toDbased on GOLD 2017,and the subjects in group B included patients reclassified from group D to B(group DB)and those remaining in group B(group BB).Incidence rates and hazard ratios(HRs)were calculated for the exacerbation of COPD and hospitalization in each group.Results:We included and followed up 845 patients.During the first year of follow-up,the GOLD 2017 classification had a better discrimination ability for different risks of COPD exacerbation and hospitalization than GOLD 2013.Group DB was associated with a higher risk of moderate-to-severe exacerbation(HR=1.88,95%confidence interval[CI]=1.37-2.59,P<0.001)and hospitalization for COPD exacerbation(HR=2.23,95%CI=1.29-3.85,P=0.004)than group BB.However,during the last year of follow-up,the differences in the risks of frequent exacerbations and hospitalizations between group DB and BB were not statistically significant(frequent exacerbations:HR=1.02,95%CI=0.51-2.03,P=0.955;frequent hospitalizations:HR=1.66,95%CI=0.58-4.78,P=0.348).The mortality rates of the two groups were both approximately 9.0%during the entire follow-up period.Conclusions:The long-term prognosis of patients reclassified into group B and of those remaining in group B was similar,although patients reclassified from group D to group B had worse short-term outcomes.The GOLD 2017 revision could improve the assessment of Chinese COPD patients in terms of long-term prognosis.
基金financially supported by the National Natural Science Foundation of China(No.U1460202)the National program for the Young Top-notch Professionals+2 种基金the Fundamental Research Funds for the Central Universities(No.N170205002)the National Key Research and Development Program of China(No.2017YFB0702203)the Chinese Postdoctoral Science Foundation(No.01270012810066)。
文摘The well completion process in oil and gas industry,aiming to build effective exploitation,is divided into acidizing and formation water production process.Oxide scale(OS)formed on the inner wall of the HP-13Cr stainless steel tubes during the hot extrusion process changes the surface roughness.The effects of OS on the corrosion of HP-13Cr stainless steel during well completion process were studied by corrosion measurement,spectra analysis,microscopic observation and numerical simulation.The results indicate that the OS make no change of phase distribution and element composition of corrosion scale,while the increasing OS roughness is the dominant factor for accelerating corrosion rate during the well completion process.In acidizing process,the greater surface roughness OS of HP-13Cr stainless steel increases the corrosion rate obviously due to a larger interfacial area in contact with the aggressive environment.During subsequent formation water production process,the turbulence eddy,formed at locations characterized with greater surface roughness OS,can deteriorate the corrosion scale and accelerate the mass transfer of the corrosive species,resulting in more serious corrosion.
基金supported by the National Natu-ral Science Foundation of China(Nos.21871125,21871026 and 22001034)the Natural Science Foundation of Shandong Province,China(Nos.ZR2019MB043 and ZR2019QB022)the Construction Project of Quality Curriculum for Postgraduate Education of Shandong Province(No.SDYKC19057).
文摘Three imidazole-modified Ag-polyoxovanadates frameworks(APFs)with a controllable molar ratio of Ag+to polyoxovanadates(POVs)[Ag(IM)_(2)]_(2)V_(4)O_(12)·2Ag(IM)_(2)(APF-1),[Ag_(2)(1-eIM)_(4)]_(2)[Ag(1-eIM)_(2)]_(3)·2Ag(1-eIM)_(2)·3(1-HeIM)[V_(10)O_(28)]_(2)(APF-2)and[Ag(1-pIM)_(2)]_(3)[HV_(10)O_(28)]·2Ag(1-pIM)_(2)·2H_(2)O(APF-3)(IM=imida-zole;1-eIM=1-ethylimidazole and 1-pIM=1-propylimidazole)have been successfully achieved by self-assembly of POVs,Ag+cations,and three different imidazole derivatives.Interestingly,the molar ratios of Ag+to POVs vary from 4:1,4.5:1 to 5:1 by changing the vanadium resources and imidazole deriva-tives.Notably,the coordination environment of Ag+cations and the structure of POVs in the APFs are also different.Specifically,for APF-1,the four Ag atoms adopt three-coordinated and four-coordinated geometries,respectively,and Ag-imidazole complexes and[V_(4)O 1_(2)]_(4)−cluster form the one-dimensional polymeric chains.While Ag atoms in APF-2 and APF-3 exhibit two-,four-and five-coordinated geome-tries for APF-2,four-,five-and six-coordinated geometries for APF-3,respectively.These Ag+cations and decavanadate clusters are assembled into the 2D supramolecular structure through the Ag-O bonds and Ag…Ag argentophilic interaction.Remarkably,thus-obtained APF-2 can serve as powerful efficient hetero-geneous catalyst for construction of C–N bond and detoxification of simulant sulfur mustard(yields up to 99%),which enable successful recycling for three cycles with remained catalytic activities and structure stability.