Hierarchical mesoporous MoO2/Mo2C/C microspheres,which are composed of primary nanoparticles with a size of about 30 nm,have been designed and synthesized through polymer regulation and subsequent carbonization proces...Hierarchical mesoporous MoO2/Mo2C/C microspheres,which are composed of primary nanoparticles with a size of about 30 nm,have been designed and synthesized through polymer regulation and subsequent carbonization processes.The as-synthesized microspheres were characterized by XRD,Raman,SEM,TEM,XPS measurements and so on.It was found that polyethylene glycol acted as a structure-directing agent,mild reducing agent and carbon source in the formation of these hierarchical mesoporous Mo O2/Mo2C/C microspheres.Moreover,the electrochemical property of the microspheres was also investigated in this work.Evaluated as an anode material for lithium ion batteries,the hierarchical mesoporous Mo O2/Mo2C/C electrode delivered the discharge specific capacities of 665 and 588 m Ah/g after 100 cycles at current densities of 100 and 200 m A/g,respectively.The satisfactory cycling performance and controllable process facilitate the practical applications of the hierarchical mesoporous Mo O2/Mo2C/C as a potential anode material in high-energy density lithium-ion batteries.展开更多
Magnesium hydride(MgH2)has received widespread attention because of its high hydrogen capacity and low cost,but the sluggish kinetics limited its practical application.Herein,the two-dimensional Mo2C MXene was c...Magnesium hydride(MgH2)has received widespread attention because of its high hydrogen capacity and low cost,but the sluggish kinetics limited its practical application.Herein,the two-dimensional Mo2C MXene was constructed to motivate the efficient hydrogen storage in MgH2for the first time.After doping 10 wt%Mo2C MXene,the starting dehydriding temperature was lowered to 225℃,presenting a 117℃ reduction compared with that of as-received MgH2.The 10 wt%Mo2C-containing MgH2sample could rapidly release 6.7 wt%H2in 13 min at 300℃,and the product after hydrogen release could absorb 6.0 wt%H2in 12 min at 200℃,showing superior hydriding and dehydriding kinetics.Moreover,the activation energy(Ea)of MgH2–10 wt%Mo2C(107.58±1.57 kJ/mol)was obviously lower than that of pure MgH2(130.45±1.97 kJ/mol),and the reduced activation energy explained the reduced dehydrogenation temperature and enhanced kinetics.Microstructure characterization revealed that Mo-species(Mo0and Mo2+)formed during ball milling served as active species accelerated the hydriding/dehydriding reactions,and the uniformly distributed active species and the interaction between Mo and O jointly promoted the hydrogen storage properties of MgH2.展开更多
The effect of modifying V2C using transition metals(TMs)(Ti,Ni,Zr,and Nb)on the MgH2dehydrogenation properties was investigated using the density functional theory(DFT).The adsorption energy,dehydrogenation ener...The effect of modifying V2C using transition metals(TMs)(Ti,Ni,Zr,and Nb)on the MgH2dehydrogenation properties was investigated using the density functional theory(DFT).The adsorption energy,dehydrogenation energy,and electronic structure of MgH2on TM(Ti,Ni,Zr,and Nb)@V2C were calculated.The results showed that TM atoms tended to occupy the face-centered cubic sites of V2C.MgH2adsorption on V2C was improved by adding a TM and the order of the adsorption energy was as follows:Ni@V2C>Ti@V2C>Zr@V2C>Nb@V2C>V2C.An orbital hybridization peak between H and TM atoms was observed in the electronic structure of MgH2on TM(Ti,Ni,Zr,and Nb)@V2C.The addition of a TM supported on V2C substantially improved the dehydrogenation energy of(MgH2)4 clusters,and the order of improvement was Ni@V2C>Ti@V2C>Nb@V2C>Zr@V2C.The dehydrogenation energy of(MgH2)4 clusters on Ni@V2C was lower than that of pure(MgH2)4 clusters and(MgH2)4 clusters on V2C,by 1.60 and 1.11 eV,respectively.TM@V2C combinations had significantly enhanced MgH2dehydrogenation,providing theoretical justification for conducting experiments to develop novel high-performance catalysts.展开更多
The photocatalytic reduction of carbon dioxide(CO2)into high-value C2+hydrocarbons represents a sustainable pathway to alleviate energy shortages and reduce atmospheric CO2levels.In this study,a unique tandem...The photocatalytic reduction of carbon dioxide(CO2)into high-value C2+hydrocarbons represents a sustainable pathway to alleviate energy shortages and reduce atmospheric CO2levels.In this study,a unique tandem photocatalyst(CoTi-CN)is constructed by integrating bimetallic CoTi-MOF with metal-free half-metallic C(CN)3.This composite demonstrates markedly enhanced activity and selectivity in the photocatalytic CO2reduction to ethylene(C2H4),achieving a C2H4selectivity of 36.8%and a generation yield of 31.3μmol g-1over 5 h.Density functional theory(DFT)calculations combined with in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis reveal that C(CN)3acts as an efficient CO2to CO converter,while CoTi-MOF favors the adsorption and C-C coupling of*CO intermediates.The spatially decoupled CO generation and C-C coupling processes lead to optimized intermediate coverage and reduced energy barriers,resulting in superior selectivity toward multi-carbon products.This work opens new horizons for the design of tandem photocatalysts that combine half-metallic catalysts with bimetallic MOFs,achieving a significant enhancement in the activity and selectivity of photocatalytic C2H4production.展开更多
BACKGROUND The human leukocyte antigen(HLA)system represents one of the most genetically diverse and densely packed genomic regions,playing a fundamental role in orchestrating immune responses.Among molecular markers ...BACKGROUND The human leukocyte antigen(HLA)system represents one of the most genetically diverse and densely packed genomic regions,playing a fundamental role in orchestrating immune responses.Among molecular markers linked to viral pathogenesis and immune modulation are insulin-like growth factor 2(IGF-2)and intestinal fattyacid-binding protein(I-FABP).AIM To investigate the influence of the HLA variant rs1131500,together with IGF-2 and I-FABP,on susceptibility to hepatitis C virus(HCV),coronavirus disease 2019(COVID-19),and their co-occurrence,to identify predictive biomarkers and potential therapeutic targets.METHODS The study involved quantifying circulating levels of IGF-2,I-FABP,and interferon-gamma(IFN-γ)and genotyping HLA rs1131500 using real-time polymerase chain reaction.Participants provided nasopharyngeal swabs for detection of severe acute respiratory syndrome coronavirus 2 RNA and blood samples for HCV RNA analysis and biomarker assessment.RESULTS Levels of IGF-2 and I-FABP were notably higher in all patient categories,with the highest values observed in coinfected individuals(P<0.0001).A moderate positive correlation was observed between I-FABP and IFN-γin COVID-19 cases(r=0.261,P=0.05).IGF-2 had the most substantial predictive value(odds ratio[OR]:4.5-5.5),while IFN-γshowed a protective trend(OR<1)when combined with IGF-2 and I-FABP.CONCLUSION IGF-2 emerged as the most consistent and reliable biomarker across all patient groups,particularly in COVID-19 and co-infections.I-FABP was a strong marker for co-infection,less so for COVID-19,and ineffective for HCV alone.Genetically,the CC genotype was more common in the HCV and Control groups,whereas the TT genotype was associated with COVID-19 and co-infection,suggesting potential diagnostic value.展开更多
BACKGROUND Chronic hepatitis C(CHC)infection remains a significant global health burden often progressing to hepatic fibrosis and cirrhosis,which may ultimately result in hepatocellular carcinoma.Liver fibrosis develo...BACKGROUND Chronic hepatitis C(CHC)infection remains a significant global health burden often progressing to hepatic fibrosis and cirrhosis,which may ultimately result in hepatocellular carcinoma.Liver fibrosis development is governed by complex host-pathogen interaction,including genetic susceptibility and immune dysregulation.IFI16 and AIM2 inflammasomes serve as critical modulators of inflammation and pathogen pathways.AIM To determine the association of variants IFI16(rs1057028)and AIM2(rs2814770)with hepatic fibrosis progression in Pakistani CHC patients.METHODS This study recruited 378 CHC patients from Lahore General Hospital(tertiary care hospital).Study participants were selected based on hepatitis C virus(HCV)-RNA positivity and transient elastography confirmed hepatic fibrosis.A total of 378 CHC patients for IFI16 genetic variant and 140 CHC patients for AIM2 variant were genotyped using amplification refractory mutation system assays.χ2test,ttest,Mann-Whitney U test,combined genotype effect,and logistic regression analysis was performed determine association between target single nucleotide polymorphisms and progression of HCV-related fibrosis and cirrhosis.RESULTS Results of our study showed that only AIM2 rs2841770 variant genotype TT shows significant association with a higher risk of advanced stage of liver fibrosis(OR=4.83,P=0.05).Combined genotype analysis had shown that CHC patients having A allele of rs1057028 and T allele of rs2814770 are significantly associated with increased risk of hepatic fibrosis(OR=2.6,95%CI:1.16-5.86,P=0.022).Our findings also revealed a significant trend of increasing frequency of liver fibrosis with an increased number of risk alleles of IFI16 rs1057028 and AIM2 rs2814770.In univariate regression analysis,body mass index and alanine aminotransferase levels significantly associated with increased risk of liver fibrosis.CONCLUSION This study suggests that AIM2 rs2814770 and its combined effect with IFI16 rs1057028 may be increase susceptibility to hepatic fibrosis in CHC patients,highlighting immunogenetic modulation,warranting further research for predictive biomarkers.展开更多
The selective cleavage of Cα-Cβbonds is of great significance to lignin valorization,and photocataly-sis offers an eco-friendly pathway to achieve this process.Here,graphitic carbon nitride(g-C3N4)modifi...The selective cleavage of Cα-Cβbonds is of great significance to lignin valorization,and photocataly-sis offers an eco-friendly pathway to achieve this process.Here,graphitic carbon nitride(g-C3N4)modified with hollow tubular In2O3was constructed via the calcination method for the photocatalytic cleavage of lignin Cα-Cβbonds.MIL-68(In)was used as the precursor of In2O3,imparting a unique hollow tubular structure and a relatively large specific surface area.The hollow tubular structure is helpful for light penetration and scattering,as well as rapid migration of the lignin substrate.The Z-scheme g-C3N4/In2O3heterojunction exhibited 92.1% conversion(corresponding benzaldehyde yield:82.4%)of the lignin model compound 2-phenoxy-1-phenylethanol(PP-ol),outperforming pure In2O3and g-C3N4by 40-and 2.3-fold,respectively,under 395 nm light illumination.By varying the illumination wavelength,the conversion and yields of the g-C3N4/In2O3composites were found to follow wavelength-dependent reactivities.Additionally,photogenerated holes are capable of converting PP-ol into benzoic acid,whereas1O2mainly converts PP-ol into benzaldehyde.This work could encourage the application of metal-organic frameworks in biomass conversion and provide insight into photocatalytic lignin valorization.展开更多
Electrocatalytic N2 reduction reaction(eNRR)is a green and sustainable approach for producing ammonia.Herein,we synthesized a Ag2-AgNPs@C catalyst by coupling dual-atom Ag sites(Ag2)and Ag nanoparticle(Ag_...Electrocatalytic N2 reduction reaction(eNRR)is a green and sustainable approach for producing ammonia.Herein,we synthesized a Ag2-AgNPs@C catalyst by coupling dual-atom Ag sites(Ag2)and Ag nanoparticle(AgNPs)on the carbon support,which exhibits excellent eNRR performance,with a high NH3 yield rate of 139.9μg h-1 mg-1cat.and an outstanding Faradaic Efficiency of 74.2%,which are superior to those of most reported eNRR catalysts.Density functional thoery calculations and in-situ infrared spectroscopy analysis demonstrate that in Ag2-AgNPs@C catalyst,AgNPs facilitate water dissociation to produce H*intermediate that supplies to adsorbed*N2 on the Ag2 site for promoting the formation of*NNH key intermediate,thus lowering the Gibbs free energy of rate-determining step and substantially enhancing the eNRR performance.This work opens up new avenues for developing efficient electrocatalytic nitrogen reduction catalysts via synergistic effect.展开更多
The fabrication of a dynamic threshold-2T0C(DT-2T0C) DRAM cell incorporating a ZnO charge-trap layer in the write transistor has been successfully achieved, addressing the negative hold voltage(VHOLD) issue of conv...The fabrication of a dynamic threshold-2T0C(DT-2T0C) DRAM cell incorporating a ZnO charge-trap layer in the write transistor has been successfully achieved, addressing the negative hold voltage(VHOLD) issue of conventional 2T0C DRAM cells using oxide channel layers. The proposed device facilitates dynamic modulation of turn-on voltage(VON) through an additional SET operation, allowing VON to shift above 0 V. The retention time in SET operation was extended to 104 s by optimizing the tunneling layer deposition conditions. The device characterization revealed a significant correlation between VON and both the WRITE speed and the retention properties of the DT-2T0C, verifying the trade-off between WRITE time and retention time. A long retention time over 1000 s was achieved, even under VHOLD of 0 V.展开更多
The design and synthesis of fully conjugated covalent organic cages(c COCs)featuring sp2carbon connections pose significant challenges due to the difficulties associated with forming stable C=C bonds.In this study,...The design and synthesis of fully conjugated covalent organic cages(c COCs)featuring sp2carbon connections pose significant challenges due to the difficulties associated with forming stable C=C bonds.In this study,we present a novel anthracene-based c COC linked by C=C bonds,synthesized directly through Knoevenagel condensation.Remarkably,this sp2c COC has shown exceptional performance as an n-type semiconductor,characterized by strong electronic delocalization,an optimized band structure,and extensive light absorption capabilities.It efficiently catalyzes the photodegradation of organic dyes and promotes the photoinduced aerobic oxidation of amines to imines.In comparison to imine-linked c COCs with the same skeleton,the sp2c COC demonstrates distinct advantages as a next-generation photocatalyst,including enhanced chemical stability and superior photocatalytic performance.This research underscores the potential of Knoevenagel condensation in the development of innovative cCOCs,offering valuable insights for their applications in optoelectronic materials and catalysis.展开更多
基金supported by the National Natural Science Foundation of China(No.21376251 and 21406233)the National Basic Research Development Program of China(2013CB632600)
摘要Hierarchical mesoporous MoO2/Mo2C/C microspheres,which are composed of primary nanoparticles with a size of about 30 nm,have been designed and synthesized through polymer regulation and subsequent carbonization processes.The as-synthesized microspheres were characterized by XRD,Raman,SEM,TEM,XPS measurements and so on.It was found that polyethylene glycol acted as a structure-directing agent,mild reducing agent and carbon source in the formation of these hierarchical mesoporous Mo O2/Mo2C/C microspheres.Moreover,the electrochemical property of the microspheres was also investigated in this work.Evaluated as an anode material for lithium ion batteries,the hierarchical mesoporous Mo O2/Mo2C/C electrode delivered the discharge specific capacities of 665 and 588 m Ah/g after 100 cycles at current densities of 100 and 200 m A/g,respectively.The satisfactory cycling performance and controllable process facilitate the practical applications of the hierarchical mesoporous Mo O2/Mo2C/C as a potential anode material in high-energy density lithium-ion batteries.
基金financially supported by the National Natural Science Foundation of China(U22A20120,52071135,51871090,U1804135,and 52401274)the Natural Science Foundation of Hebei Province for Innovation Groups Program(C2022203003)the Fundamental Research Funds for the Universities of Henan Province(NSFRF220201)+2 种基金Key R&D Special Project of Henan Province(241111240200)the Key Project of Henan Provincial Natural Science Foundation(242300421184)the Henan Province Science and Technology Research Projects(242102241035 and 232102231048).
摘要Magnesium hydride(MgH2)has received widespread attention because of its high hydrogen capacity and low cost,but the sluggish kinetics limited its practical application.Herein,the two-dimensional Mo2C MXene was constructed to motivate the efficient hydrogen storage in MgH2for the first time.After doping 10 wt%Mo2C MXene,the starting dehydriding temperature was lowered to 225℃,presenting a 117℃ reduction compared with that of as-received MgH2.The 10 wt%Mo2C-containing MgH2sample could rapidly release 6.7 wt%H2in 13 min at 300℃,and the product after hydrogen release could absorb 6.0 wt%H2in 12 min at 200℃,showing superior hydriding and dehydriding kinetics.Moreover,the activation energy(Ea)of MgH2–10 wt%Mo2C(107.58±1.57 kJ/mol)was obviously lower than that of pure MgH2(130.45±1.97 kJ/mol),and the reduced activation energy explained the reduced dehydrogenation temperature and enhanced kinetics.Microstructure characterization revealed that Mo-species(Mo0and Mo2+)formed during ball milling served as active species accelerated the hydriding/dehydriding reactions,and the uniformly distributed active species and the interaction between Mo and O jointly promoted the hydrogen storage properties of MgH2.
基金supported by National Natural Science Foundation of China(No.52261038)the Natural Science Foundation of Guangxi,China(No.2025GXNSFFA069003)+1 种基金the Innovative Team of Young Scholars from Xiang Si Lake(No.2020RSCXSHQN02)the Scientific Research Foundation of Guangxi MinZu University,China(No.2020KJQD01)。
摘要The effect of modifying V2C using transition metals(TMs)(Ti,Ni,Zr,and Nb)on the MgH2dehydrogenation properties was investigated using the density functional theory(DFT).The adsorption energy,dehydrogenation energy,and electronic structure of MgH2on TM(Ti,Ni,Zr,and Nb)@V2C were calculated.The results showed that TM atoms tended to occupy the face-centered cubic sites of V2C.MgH2adsorption on V2C was improved by adding a TM and the order of the adsorption energy was as follows:Ni@V2C>Ti@V2C>Zr@V2C>Nb@V2C>V2C.An orbital hybridization peak between H and TM atoms was observed in the electronic structure of MgH2on TM(Ti,Ni,Zr,and Nb)@V2C.The addition of a TM supported on V2C substantially improved the dehydrogenation energy of(MgH2)4 clusters,and the order of improvement was Ni@V2C>Ti@V2C>Nb@V2C>Zr@V2C.The dehydrogenation energy of(MgH2)4 clusters on Ni@V2C was lower than that of pure(MgH2)4 clusters and(MgH2)4 clusters on V2C,by 1.60 and 1.11 eV,respectively.TM@V2C combinations had significantly enhanced MgH2dehydrogenation,providing theoretical justification for conducting experiments to develop novel high-performance catalysts.
基金supported by the National Natural Science Foundation of China(51303083)the National Natural Science Foundation of China for Excellent Young Scholars(51922050)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20191293)the Fundamental Research Funds for the Central Universities(30920021123).
摘要The photocatalytic reduction of carbon dioxide(CO2)into high-value C2+hydrocarbons represents a sustainable pathway to alleviate energy shortages and reduce atmospheric CO2levels.In this study,a unique tandem photocatalyst(CoTi-CN)is constructed by integrating bimetallic CoTi-MOF with metal-free half-metallic C(CN)3.This composite demonstrates markedly enhanced activity and selectivity in the photocatalytic CO2reduction to ethylene(C2H4),achieving a C2H4selectivity of 36.8%and a generation yield of 31.3μmol g-1over 5 h.Density functional theory(DFT)calculations combined with in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis reveal that C(CN)3acts as an efficient CO2to CO converter,while CoTi-MOF favors the adsorption and C-C coupling of*CO intermediates.The spatially decoupled CO generation and C-C coupling processes lead to optimized intermediate coverage and reduced energy barriers,resulting in superior selectivity toward multi-carbon products.This work opens new horizons for the design of tandem photocatalysts that combine half-metallic catalysts with bimetallic MOFs,achieving a significant enhancement in the activity and selectivity of photocatalytic C2H4production.
摘要BACKGROUND The human leukocyte antigen(HLA)system represents one of the most genetically diverse and densely packed genomic regions,playing a fundamental role in orchestrating immune responses.Among molecular markers linked to viral pathogenesis and immune modulation are insulin-like growth factor 2(IGF-2)and intestinal fattyacid-binding protein(I-FABP).AIM To investigate the influence of the HLA variant rs1131500,together with IGF-2 and I-FABP,on susceptibility to hepatitis C virus(HCV),coronavirus disease 2019(COVID-19),and their co-occurrence,to identify predictive biomarkers and potential therapeutic targets.METHODS The study involved quantifying circulating levels of IGF-2,I-FABP,and interferon-gamma(IFN-γ)and genotyping HLA rs1131500 using real-time polymerase chain reaction.Participants provided nasopharyngeal swabs for detection of severe acute respiratory syndrome coronavirus 2 RNA and blood samples for HCV RNA analysis and biomarker assessment.RESULTS Levels of IGF-2 and I-FABP were notably higher in all patient categories,with the highest values observed in coinfected individuals(P<0.0001).A moderate positive correlation was observed between I-FABP and IFN-γin COVID-19 cases(r=0.261,P=0.05).IGF-2 had the most substantial predictive value(odds ratio[OR]:4.5-5.5),while IFN-γshowed a protective trend(OR<1)when combined with IGF-2 and I-FABP.CONCLUSION IGF-2 emerged as the most consistent and reliable biomarker across all patient groups,particularly in COVID-19 and co-infections.I-FABP was a strong marker for co-infection,less so for COVID-19,and ineffective for HCV alone.Genetically,the CC genotype was more common in the HCV and Control groups,whereas the TT genotype was associated with COVID-19 and co-infection,suggesting potential diagnostic value.
摘要BACKGROUND Chronic hepatitis C(CHC)infection remains a significant global health burden often progressing to hepatic fibrosis and cirrhosis,which may ultimately result in hepatocellular carcinoma.Liver fibrosis development is governed by complex host-pathogen interaction,including genetic susceptibility and immune dysregulation.IFI16 and AIM2 inflammasomes serve as critical modulators of inflammation and pathogen pathways.AIM To determine the association of variants IFI16(rs1057028)and AIM2(rs2814770)with hepatic fibrosis progression in Pakistani CHC patients.METHODS This study recruited 378 CHC patients from Lahore General Hospital(tertiary care hospital).Study participants were selected based on hepatitis C virus(HCV)-RNA positivity and transient elastography confirmed hepatic fibrosis.A total of 378 CHC patients for IFI16 genetic variant and 140 CHC patients for AIM2 variant were genotyped using amplification refractory mutation system assays.χ2test,ttest,Mann-Whitney U test,combined genotype effect,and logistic regression analysis was performed determine association between target single nucleotide polymorphisms and progression of HCV-related fibrosis and cirrhosis.RESULTS Results of our study showed that only AIM2 rs2841770 variant genotype TT shows significant association with a higher risk of advanced stage of liver fibrosis(OR=4.83,P=0.05).Combined genotype analysis had shown that CHC patients having A allele of rs1057028 and T allele of rs2814770 are significantly associated with increased risk of hepatic fibrosis(OR=2.6,95%CI:1.16-5.86,P=0.022).Our findings also revealed a significant trend of increasing frequency of liver fibrosis with an increased number of risk alleles of IFI16 rs1057028 and AIM2 rs2814770.In univariate regression analysis,body mass index and alanine aminotransferase levels significantly associated with increased risk of liver fibrosis.CONCLUSION This study suggests that AIM2 rs2814770 and its combined effect with IFI16 rs1057028 may be increase susceptibility to hepatic fibrosis in CHC patients,highlighting immunogenetic modulation,warranting further research for predictive biomarkers.
摘要The selective cleavage of Cα-Cβbonds is of great significance to lignin valorization,and photocataly-sis offers an eco-friendly pathway to achieve this process.Here,graphitic carbon nitride(g-C3N4)modified with hollow tubular In2O3was constructed via the calcination method for the photocatalytic cleavage of lignin Cα-Cβbonds.MIL-68(In)was used as the precursor of In2O3,imparting a unique hollow tubular structure and a relatively large specific surface area.The hollow tubular structure is helpful for light penetration and scattering,as well as rapid migration of the lignin substrate.The Z-scheme g-C3N4/In2O3heterojunction exhibited 92.1% conversion(corresponding benzaldehyde yield:82.4%)of the lignin model compound 2-phenoxy-1-phenylethanol(PP-ol),outperforming pure In2O3and g-C3N4by 40-and 2.3-fold,respectively,under 395 nm light illumination.By varying the illumination wavelength,the conversion and yields of the g-C3N4/In2O3composites were found to follow wavelength-dependent reactivities.Additionally,photogenerated holes are capable of converting PP-ol into benzoic acid,whereas1O2mainly converts PP-ol into benzaldehyde.This work could encourage the application of metal-organic frameworks in biomass conversion and provide insight into photocatalytic lignin valorization.
摘要Electrocatalytic N2 reduction reaction(eNRR)is a green and sustainable approach for producing ammonia.Herein,we synthesized a Ag2-AgNPs@C catalyst by coupling dual-atom Ag sites(Ag2)and Ag nanoparticle(AgNPs)on the carbon support,which exhibits excellent eNRR performance,with a high NH3 yield rate of 139.9μg h-1 mg-1cat.and an outstanding Faradaic Efficiency of 74.2%,which are superior to those of most reported eNRR catalysts.Density functional thoery calculations and in-situ infrared spectroscopy analysis demonstrate that in Ag2-AgNPs@C catalyst,AgNPs facilitate water dissociation to produce H*intermediate that supplies to adsorbed*N2 on the Ag2 site for promoting the formation of*NNH key intermediate,thus lowering the Gibbs free energy of rate-determining step and substantially enhancing the eNRR performance.This work opens up new avenues for developing efficient electrocatalytic nitrogen reduction catalysts via synergistic effect.
基金supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (RS-2024-00334190)。
摘要The fabrication of a dynamic threshold-2T0C(DT-2T0C) DRAM cell incorporating a ZnO charge-trap layer in the write transistor has been successfully achieved, addressing the negative hold voltage(VHOLD) issue of conventional 2T0C DRAM cells using oxide channel layers. The proposed device facilitates dynamic modulation of turn-on voltage(VON) through an additional SET operation, allowing VON to shift above 0 V. The retention time in SET operation was extended to 104 s by optimizing the tunneling layer deposition conditions. The device characterization revealed a significant correlation between VON and both the WRITE speed and the retention properties of the DT-2T0C, verifying the trade-off between WRITE time and retention time. A long retention time over 1000 s was achieved, even under VHOLD of 0 V.
基金supported by the Class III Peak Discipline of Shanghai-Materials Science and Engineering (High Energy Beam Intelligent Processing and Green Manufacturing)Fundamental Research Funds for the Central Universities (Nos. YG2023QNA04and YG2022QN027).
摘要The design and synthesis of fully conjugated covalent organic cages(c COCs)featuring sp2carbon connections pose significant challenges due to the difficulties associated with forming stable C=C bonds.In this study,we present a novel anthracene-based c COC linked by C=C bonds,synthesized directly through Knoevenagel condensation.Remarkably,this sp2c COC has shown exceptional performance as an n-type semiconductor,characterized by strong electronic delocalization,an optimized band structure,and extensive light absorption capabilities.It efficiently catalyzes the photodegradation of organic dyes and promotes the photoinduced aerobic oxidation of amines to imines.In comparison to imine-linked c COCs with the same skeleton,the sp2c COC demonstrates distinct advantages as a next-generation photocatalyst,including enhanced chemical stability and superior photocatalytic performance.This research underscores the potential of Knoevenagel condensation in the development of innovative cCOCs,offering valuable insights for their applications in optoelectronic materials and catalysis.