Available online Integrating transition metal centered MOFs with conductive materials is a feasible route to enhance electron transfer efficiency of materials.Herein,a composite porous structure CQDs_(10)@NiFe-MOF-A w...Available online Integrating transition metal centered MOFs with conductive materials is a feasible route to enhance electron transfer efficiency of materials.Herein,a composite porous structure CQDs_(10)@NiFe-MOF-A was fabricated via introducing carbon quantum dots(CQDs)into porous NiFe-MOF.The CQDs would make partial loss of lattice in MOF during its growth,leading to the composite building block with the coexistance of crystalline region and amorphous region.The calcining treatment would produce an ultrathin protective layer as well as some lattice collapse.The synergy effect between NiFe ions effectively regulated electronic structure of metal active sites,and successful grafting of CQDs to NiFe-MOF significantly improved electrical conductivity.As expected,the catalyst exhibited outstanding OER performances with high mass activity of 91.6 A/g at overpotential of 300 mV and robust durability of 10,000 cycles in 1 mol/L KOH,which outperformed that of noble catalyst IrO_(2)of 25.2 A/g.The strategy paves a feasible and effective avenue for the non-noble metal catalysts.展开更多
Mesoporous superacids S2O82–-Fe2O3/SBA-15(SFS)with active nanoparticles are prepared by ultrasonic adsorption method.This method is adopted to ensure a homo-dispersed nanoparticle active phase,large specific surface ...Mesoporous superacids S2O82–-Fe2O3/SBA-15(SFS)with active nanoparticles are prepared by ultrasonic adsorption method.This method is adopted to ensure a homo-dispersed nanoparticle active phase,large specific surface area and many acidic sites.Compared with bulk S2O82–-Fe2O3,Br?nsted acid catalysts and other reported catalysts,SFS with an Fe2O3 loading of 30%(SFS-30)exhibits an outstanding activity in the probe reaction of alcoholysis of styrene oxide by methanol with 100%yield.Moreover,SFS-30 also shows a more excellent catalytic performance than bulk S2O82–-Fe2O3 towards the alcoholysis of other ROHs(R=C2H5-C4H9).Lewis and Bronsted acid sites on the SFS-30 surfaces are confirmed by pyridine adsorbed infrared spectra.The highly efficient catalytic activity of SFS-30 may be attributed to the synergistic effect from the nano-effect of S2O82–-Fe2O3 nanoparticles and the mesostructure of SBA-15.Finally,SFS-30 shows a good catalytic reusability,providing an 84.1%yield after seven catalytic cycles.展开更多
Self‐assembled mesoporous polyoxometalate‐based ionic hybrid catalyst,[PxyDim]2.5PMoV2,was prepared by combining p‐xylene‐tethered diimidazole ionic liquid[PxyDim]Cl2with Keggin‐structured V‐substituted polyoxom...Self‐assembled mesoporous polyoxometalate‐based ionic hybrid catalyst,[PxyDim]2.5PMoV2,was prepared by combining p‐xylene‐tethered diimidazole ionic liquid[PxyDim]Cl2with Keggin‐structured V‐substituted polyoxometalate H5PMo10V2O40.The obtained hybrid was shown to be a mesostructured and hydrophobic material with good thermal stability.In the H2O2‐based hydroxylation of benzene to phenol,the hybrid showed extraordinary catalytic activity and rate,and quite stable reusability.The unique hydrophobic properties and mesoporous structure of the hybrid were responsible for its excellent catalytic performance.展开更多
The development of high-performance non-precious metal-based robust bifunctional electrocatalyst for both hydrogen evolution reaction(HER) and oxygen evolution reactions(OER) in alkaline media is essential for the ele...The development of high-performance non-precious metal-based robust bifunctional electrocatalyst for both hydrogen evolution reaction(HER) and oxygen evolution reactions(OER) in alkaline media is essential for the electrochemical overall water splitting technologies. Herein, we demonstrate that the HER/OER performance of Co Se_(2)can be significantly enhanced by tuning the 3d-orbital electron filling degree through Mo doping. Both density functional theory(DFT) calculations and experimental results imply that the doping of Mo with higher proportion of the unoccupied d-orbital(P_(un)) could not only serve as the active center for water adsorption to enhance the water molecule activation, but also modulate the electronic structures of Co metal center leading to the optimized adsorption strength of*H. As expected, the obtained Mo-Co Se_(2)exhibits a remarkable bifunctional performance with overpotential of only 85 m V for HER and 245 m V for OER to achieve the current density of 10 m A/cm^(2)in alkaline media.This work will provide a valuable insight to design highly efficient bifunctional electrocatalyst towards HER and OER.展开更多
Exploring highly efficient electrocatalysts and understanding the reaction mechanisms for hydrogen electrocatalysis,including hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) in alkaline media a...Exploring highly efficient electrocatalysts and understanding the reaction mechanisms for hydrogen electrocatalysis,including hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) in alkaline media are conducive to the conversion of hydrogen energy.Herein,we reported a new strategy to boost the HER/HOR performances of ruthenium (Ru) nanoparticles through nitrogen (N) modification.The obtained N-Ru/C exhibit remarkable catalytic performance,with normalized HOR exchange current density and mass activity of 0.56 m A/cm^(2)and 0.54 m A/μg,respectively,about 4 and 4.5 times higher than those of Ru/C,and even twofold enhancement compared to commercial Pt/C.Moreover,at the overpotential of 50 m V,the normalized HER current density of N-Ru/C is 5.5 times higher than that of Ru/C.Experimental and density functional theory (DFT) results verify the electronic regulation of Ru after N incorporation,resulting in the optimized hydrogen adsorption Gibbs free energy (ΔG_(H*)) and hence enhancing the HOR/HER performance.展开更多
Background and Objectives:To investigate the correlation between weight-adjusted-waist index(WWI),a novel obesity index,and serum ferritin(SF)level in patients with type 2 diabetes mellitus(T2DM),and the association b...Background and Objectives:To investigate the correlation between weight-adjusted-waist index(WWI),a novel obesity index,and serum ferritin(SF)level in patients with type 2 diabetes mellitus(T2DM),and the association between WWI and the prevalence of hyperferritinemia.Methods and Study Design:A total of 943 patients with T2DM were divided into three groups based on WWI tertile levels.Disparities in SF levels and the prevalence of hyperferritinemia were compared among these groups.The correlations among WWI,SF levels,and hyperferritinemia were analyzed in patients with T2DM.Results:As WWI tertile levels increased,SF levels tended to increase(p for trend<0.01).A statistically significant positive correlation was observed between the WWI and SF levels(R=0.263,p<0.001).After adjusting for confounders by multiple linear regression,a significant positive correlation was maintained between the WWI and SF levels[β=0.194,95%CI(49.914,112.120),p<0.01].Binary logistic regression analysis revealed a positive association between the WWI and the likelihood of hyperferritinemia,with a notably stronger correlation observed in females compared to males[OR=3.248,95%CI(2.027,5.204),p<0.01 vs.OR=2.091,95%CI(1.432,3.054),p<0.01].Conclusions:Along with increasing WWI,SF levels gradually increased in patients with T2DM.The WWI exhibited a positive correlation with SF levels and hyperferritinemia,more significantly in female patients.展开更多
基金financially supported by the Fundamental Research Funds for the Central Universities(No.2042021kf0077)Start-up funds for provincial and municipal"double first-class"construction special talents(No.600460001)China postdoctoral Science Foundation(No.2017M612496)。
文摘Available online Integrating transition metal centered MOFs with conductive materials is a feasible route to enhance electron transfer efficiency of materials.Herein,a composite porous structure CQDs_(10)@NiFe-MOF-A was fabricated via introducing carbon quantum dots(CQDs)into porous NiFe-MOF.The CQDs would make partial loss of lattice in MOF during its growth,leading to the composite building block with the coexistance of crystalline region and amorphous region.The calcining treatment would produce an ultrathin protective layer as well as some lattice collapse.The synergy effect between NiFe ions effectively regulated electronic structure of metal active sites,and successful grafting of CQDs to NiFe-MOF significantly improved electrical conductivity.As expected,the catalyst exhibited outstanding OER performances with high mass activity of 91.6 A/g at overpotential of 300 mV and robust durability of 10,000 cycles in 1 mol/L KOH,which outperformed that of noble catalyst IrO_(2)of 25.2 A/g.The strategy paves a feasible and effective avenue for the non-noble metal catalysts.
文摘Mesoporous superacids S2O82–-Fe2O3/SBA-15(SFS)with active nanoparticles are prepared by ultrasonic adsorption method.This method is adopted to ensure a homo-dispersed nanoparticle active phase,large specific surface area and many acidic sites.Compared with bulk S2O82–-Fe2O3,Br?nsted acid catalysts and other reported catalysts,SFS with an Fe2O3 loading of 30%(SFS-30)exhibits an outstanding activity in the probe reaction of alcoholysis of styrene oxide by methanol with 100%yield.Moreover,SFS-30 also shows a more excellent catalytic performance than bulk S2O82–-Fe2O3 towards the alcoholysis of other ROHs(R=C2H5-C4H9).Lewis and Bronsted acid sites on the SFS-30 surfaces are confirmed by pyridine adsorbed infrared spectra.The highly efficient catalytic activity of SFS-30 may be attributed to the synergistic effect from the nano-effect of S2O82–-Fe2O3 nanoparticles and the mesostructure of SBA-15.Finally,SFS-30 shows a good catalytic reusability,providing an 84.1%yield after seven catalytic cycles.
基金supported by the National Natural Science Foundation of China (21506118,21476132,51574160)Shandong Province Founda-tion for Outstanding Young Scientist (BS2014CL030)~~
文摘Self‐assembled mesoporous polyoxometalate‐based ionic hybrid catalyst,[PxyDim]2.5PMoV2,was prepared by combining p‐xylene‐tethered diimidazole ionic liquid[PxyDim]Cl2with Keggin‐structured V‐substituted polyoxometalate H5PMo10V2O40.The obtained hybrid was shown to be a mesostructured and hydrophobic material with good thermal stability.In the H2O2‐based hydroxylation of benzene to phenol,the hybrid showed extraordinary catalytic activity and rate,and quite stable reusability.The unique hydrophobic properties and mesoporous structure of the hybrid were responsible for its excellent catalytic performance.
基金financially supported by the National Natural Science Foundation of China (No. 21972107)Natural Science Foundation of Jiangsu Province (No. BK20191186)Natural Science Foundation of Hubei Province (No. 2020CFA095)。
文摘The development of high-performance non-precious metal-based robust bifunctional electrocatalyst for both hydrogen evolution reaction(HER) and oxygen evolution reactions(OER) in alkaline media is essential for the electrochemical overall water splitting technologies. Herein, we demonstrate that the HER/OER performance of Co Se_(2)can be significantly enhanced by tuning the 3d-orbital electron filling degree through Mo doping. Both density functional theory(DFT) calculations and experimental results imply that the doping of Mo with higher proportion of the unoccupied d-orbital(P_(un)) could not only serve as the active center for water adsorption to enhance the water molecule activation, but also modulate the electronic structures of Co metal center leading to the optimized adsorption strength of*H. As expected, the obtained Mo-Co Se_(2)exhibits a remarkable bifunctional performance with overpotential of only 85 m V for HER and 245 m V for OER to achieve the current density of 10 m A/cm^(2)in alkaline media.This work will provide a valuable insight to design highly efficient bifunctional electrocatalyst towards HER and OER.
基金financially supported by the National Natural Science Foundation of China (No.21972107)National Natural Science Foundation of Hubei Province (No.2020CFA095)+1 种基金the National Natural Science Foundation of Jiangsu Province (No.BK20191186)Yangzhou Key Research Development Program (No.YZ2019025)。
文摘Exploring highly efficient electrocatalysts and understanding the reaction mechanisms for hydrogen electrocatalysis,including hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) in alkaline media are conducive to the conversion of hydrogen energy.Herein,we reported a new strategy to boost the HER/HOR performances of ruthenium (Ru) nanoparticles through nitrogen (N) modification.The obtained N-Ru/C exhibit remarkable catalytic performance,with normalized HOR exchange current density and mass activity of 0.56 m A/cm^(2)and 0.54 m A/μg,respectively,about 4 and 4.5 times higher than those of Ru/C,and even twofold enhancement compared to commercial Pt/C.Moreover,at the overpotential of 50 m V,the normalized HER current density of N-Ru/C is 5.5 times higher than that of Ru/C.Experimental and density functional theory (DFT) results verify the electronic regulation of Ru after N incorporation,resulting in the optimized hydrogen adsorption Gibbs free energy (ΔG_(H*)) and hence enhancing the HOR/HER performance.
基金funded by the National Natural Science Foundation of China(No.81960155 and No.82360161)the Science Foundation of Gansu Provincial Maternity and Child-care Hospital(GMCCH2024-3-2)the Lanzhou Science and Technology Bureau(2022-3-46).
文摘Background and Objectives:To investigate the correlation between weight-adjusted-waist index(WWI),a novel obesity index,and serum ferritin(SF)level in patients with type 2 diabetes mellitus(T2DM),and the association between WWI and the prevalence of hyperferritinemia.Methods and Study Design:A total of 943 patients with T2DM were divided into three groups based on WWI tertile levels.Disparities in SF levels and the prevalence of hyperferritinemia were compared among these groups.The correlations among WWI,SF levels,and hyperferritinemia were analyzed in patients with T2DM.Results:As WWI tertile levels increased,SF levels tended to increase(p for trend<0.01).A statistically significant positive correlation was observed between the WWI and SF levels(R=0.263,p<0.001).After adjusting for confounders by multiple linear regression,a significant positive correlation was maintained between the WWI and SF levels[β=0.194,95%CI(49.914,112.120),p<0.01].Binary logistic regression analysis revealed a positive association between the WWI and the likelihood of hyperferritinemia,with a notably stronger correlation observed in females compared to males[OR=3.248,95%CI(2.027,5.204),p<0.01 vs.OR=2.091,95%CI(1.432,3.054),p<0.01].Conclusions:Along with increasing WWI,SF levels gradually increased in patients with T2DM.The WWI exhibited a positive correlation with SF levels and hyperferritinemia,more significantly in female patients.
