Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with ...Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.展开更多
The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)R...The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)RRs)in solid oxide elec-trolysis cells(SOECs).However,practical appli-cation of nanofiber-based electrodes faces chal-lenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte.To tackle this challenge,a novel hybrid nanofiber electrode,La_(0.6)Sr_(0.4)Co_(0.15)Fe_(0.8)Pd_(0.05)O_(3-δ)(H-LSCFP),is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique.After consecutive treatment in 100% H_(2) and CO_(2) at 700°C,LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface,enhancing CO_(2) adsorption.The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm^(-2) in CO_(2) at 800°C and 1.5 V,setting a new benchmark among reported nanofiber-based electrodes.Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO_(2)RR.The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure,paving the way for further advancements and nanofiber applications in CO_(2)-SOECs.展开更多
To investigate the impacts of mineral composition on physical and mechanical properties of carbonate rocks,limestone specimens containing different contents in calcite and dolomite are selected to perform CO_(2)-water...To investigate the impacts of mineral composition on physical and mechanical properties of carbonate rocks,limestone specimens containing different contents in calcite and dolomite are selected to perform CO_(2)-water-rock reaction experiments.The X-ray Diffraction(XRD) and Nuclear Magnetic Resonance(NMR) are carried out to examine the change characteristics of mineral dissolution and pore structure after reaction.The core flooding experiments with Fiber Bragg gratings are implemented to examine the stress sensitivity of carbonate rocks.The results show that the limestones containing pure calcite are more susceptible to acid dissolution compared to limestone containing impure dolomite.The calcite content in pure limestone decreases as the reaction undergoes.The dissolution of dolomite leads to the formation of calcite in impure limestone.Calcite dissolution leads to the formation of macropore and flow channels in pure limestone,while the effects of impure dolomite in impure limestone results in mesopore formation.When confining pressure is lower than 12 MPa,pure limestones demonstrate higher strain sensitivity coefficients compared to impure limestone containing dolomite after reaction.When confining pressure exceeds 12 MPa,the strain sensitivity coefficients of both pure and impure limestones become almost equal.展开更多
The multi-point simultaneous long-term measurement of CO_(2) concentration in seawater can provide more-valuable data for further understanding of the spatial and temporal distribution of CO_(2).Thus,the requirement f...The multi-point simultaneous long-term measurement of CO_(2) concentration in seawater can provide more-valuable data for further understanding of the spatial and temporal distribution of CO_(2).Thus,the requirement for a low-cost sensor with high precision,low power consumption,and a small size is becoming urgent.In this work,an in-situ sensor for CO_(2) detection in seawater,based on a permeable membrane and non-dispersive infrared(NDIR)technology,is developed.The sensor has a small size(Ф66 mm×124 mm),light weight(0.7 kg in air),low power consumption(<0.9 W),low cost(<US$1000),and high-pressure tolerance(<200 m).After laboratory performance tests,the sensor was found to have a measurement range of(0–2000)×10^(-6),and the gas linear correlation R^(2) is 0.99,with a precision of about 0.98%at a sampling rate of 1 s.A comparison measurement was carried out with a commercial sensor in a pool for 7 days,and the results showed a consistent trend.Further,the newly developed sensor was deployed in Qingdao nearshore water for 35 days.The results proved that the sensor could measure the dynamic changes of CO_(2) concentration in seawater continuously,and had the potential to carry out long-term observations on an oceanic platform.It is hoped that the sensor could be applied to field ocean observations in near future.展开更多
SnO_(2)/Co_(3)O_(4)nanofibers(NFs)are synthesized by using a homopolar electrospinning system with double jets of positive polarity electric fields.The morphology and structure of SnO_(2)/Co_(3)O_(4)hetero-nanofibers ...SnO_(2)/Co_(3)O_(4)nanofibers(NFs)are synthesized by using a homopolar electrospinning system with double jets of positive polarity electric fields.The morphology and structure of SnO_(2)/Co_(3)O_(4)hetero-nanofibers are characterized by using field emission scanning electron microscope(FE-SEM),transmission electron microscope(TEM),x-ray diffraction(XRD),and x-ray photoelectron spectrometer(XPS).The analyses of SnO_(2)/Co_(3)O_(4)NFs by EDS and HRTEM show that the cobalt and tin exist on one nanofiber,which is related to the homopolar electrospinning and the crystallization during sintering.As a typical n-type semiconductor,Sn O_(2)has the disadvantages of high optimal operating temperature and poor reproducibility.Comparing with Sn O_(2),the optimal operating temperature of SnO_(2)/Co_(3)O_(4)NFs is reduced from 350℃to 250℃,which may be related to the catalysis of Co_(2)O_(2).The response of SnO_(2)/Co_(3)O_(4)to 100-ppm ethanol at 250℃is 50.9,9 times higher than that of pure Sn O_(2),which may be attributed to the p–n heterojunction between the n-type Sn O_(2)crystalline grain and the p-type Co_(2)O_(2)crystalline grain.The nanoscale p–n heterojunction promotes the electron migration and forms an interface barrier.The synergy effects between Sn O_(2)and Co_(2)O_(2),the crystalline grain p–n heterojunction,the existence of nanofibers and the large specific surface area all jointly contribute to the improved gas sensing performance.展开更多
基金supported by National Natural Science Foundation of China(52208272,41706080 and 51702328)the Basic Scientific Fund for National Public Research Institutes of China(2020S02 and 2019Y03)+3 种基金the Basic Frontier Science Research Program of Chinese Academy of Sciences(ZDBS-LY-DQC025)the Young Elite Scientists Sponsorship Program by CAST(No.YESS20210201)the Strategic Leading Science&Technology Program of the Chinese Academy of Sciences(XDA13040403)the Key Research and Development Program of Shandong Province(Major Scientific and Technological Innovation Project)(2019JZZY020711).
文摘Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.
基金This work was supported by the National Research Foundation of Korea(NRF)grant funded by the Korean Government(MSIT)(2019M3E6A1103944,2020R1A2C2010690).
文摘The unique characteristics of nanofibers in rational electrode design enable effec-tive utilization and maximizing material properties for achieving highly efficient and sustainable CO_(2) reduction reactions( CO_(2)RRs)in solid oxide elec-trolysis cells(SOECs).However,practical appli-cation of nanofiber-based electrodes faces chal-lenges in establishing sufficient interfacial contact and adhesion with the dense electrolyte.To tackle this challenge,a novel hybrid nanofiber electrode,La_(0.6)Sr_(0.4)Co_(0.15)Fe_(0.8)Pd_(0.05)O_(3-δ)(H-LSCFP),is developed by strategically incorporating low aspect ratio crushed LSCFP nanofibers into the excess porous interspace of a high aspect ratio LSCFP nanofiber framework synthesized via electrospinning technique.After consecutive treatment in 100% H_(2) and CO_(2) at 700°C,LSCFP nanofibers form a perovskite phase with in situ exsolved Co metal nanocatalysts and a high concentration of oxygen species on the surface,enhancing CO_(2) adsorption.The SOEC with the H-LSCFP electrode yielded an outstanding current density of 2.2 A cm^(-2) in CO_(2) at 800°C and 1.5 V,setting a new benchmark among reported nanofiber-based electrodes.Digital twinning of the H-LSCFP reveals improved contact adhesion and increased reaction sites for CO_(2)RR.The present work demonstrates a highly catalytically active and robust nanofiber-based fuel electrode with a hybrid structure,paving the way for further advancements and nanofiber applications in CO_(2)-SOECs.
基金partially supported by Creative Group of Natural Science Foundation of Hubei Province (Grant No. 2021CFA030)National Natural Science Foundation of China (Grant No. 41872210)。
文摘To investigate the impacts of mineral composition on physical and mechanical properties of carbonate rocks,limestone specimens containing different contents in calcite and dolomite are selected to perform CO_(2)-water-rock reaction experiments.The X-ray Diffraction(XRD) and Nuclear Magnetic Resonance(NMR) are carried out to examine the change characteristics of mineral dissolution and pore structure after reaction.The core flooding experiments with Fiber Bragg gratings are implemented to examine the stress sensitivity of carbonate rocks.The results show that the limestones containing pure calcite are more susceptible to acid dissolution compared to limestone containing impure dolomite.The calcite content in pure limestone decreases as the reaction undergoes.The dissolution of dolomite leads to the formation of calcite in impure limestone.Calcite dissolution leads to the formation of macropore and flow channels in pure limestone,while the effects of impure dolomite in impure limestone results in mesopore formation.When confining pressure is lower than 12 MPa,pure limestones demonstrate higher strain sensitivity coefficients compared to impure limestone containing dolomite after reaction.When confining pressure exceeds 12 MPa,the strain sensitivity coefficients of both pure and impure limestones become almost equal.
基金Supported by the National Nature Science Foundation of China(No.41527901)the Provincial Key Research and Development Program of Shandong,China(No.2019JZZY010417)the Special Program of Shandong Province for Qingdao Pilot National Laboratory of Marine Science and Technology(No.2021QNLM020002).
文摘The multi-point simultaneous long-term measurement of CO_(2) concentration in seawater can provide more-valuable data for further understanding of the spatial and temporal distribution of CO_(2).Thus,the requirement for a low-cost sensor with high precision,low power consumption,and a small size is becoming urgent.In this work,an in-situ sensor for CO_(2) detection in seawater,based on a permeable membrane and non-dispersive infrared(NDIR)technology,is developed.The sensor has a small size(Ф66 mm×124 mm),light weight(0.7 kg in air),low power consumption(<0.9 W),low cost(<US$1000),and high-pressure tolerance(<200 m).After laboratory performance tests,the sensor was found to have a measurement range of(0–2000)×10^(-6),and the gas linear correlation R^(2) is 0.99,with a precision of about 0.98%at a sampling rate of 1 s.A comparison measurement was carried out with a commercial sensor in a pool for 7 days,and the results showed a consistent trend.Further,the newly developed sensor was deployed in Qingdao nearshore water for 35 days.The results proved that the sensor could measure the dynamic changes of CO_(2) concentration in seawater continuously,and had the potential to carry out long-term observations on an oceanic platform.It is hoped that the sensor could be applied to field ocean observations in near future.
文摘SnO_(2)/Co_(3)O_(4)nanofibers(NFs)are synthesized by using a homopolar electrospinning system with double jets of positive polarity electric fields.The morphology and structure of SnO_(2)/Co_(3)O_(4)hetero-nanofibers are characterized by using field emission scanning electron microscope(FE-SEM),transmission electron microscope(TEM),x-ray diffraction(XRD),and x-ray photoelectron spectrometer(XPS).The analyses of SnO_(2)/Co_(3)O_(4)NFs by EDS and HRTEM show that the cobalt and tin exist on one nanofiber,which is related to the homopolar electrospinning and the crystallization during sintering.As a typical n-type semiconductor,Sn O_(2)has the disadvantages of high optimal operating temperature and poor reproducibility.Comparing with Sn O_(2),the optimal operating temperature of SnO_(2)/Co_(3)O_(4)NFs is reduced from 350℃to 250℃,which may be related to the catalysis of Co_(2)O_(2).The response of SnO_(2)/Co_(3)O_(4)to 100-ppm ethanol at 250℃is 50.9,9 times higher than that of pure Sn O_(2),which may be attributed to the p–n heterojunction between the n-type Sn O_(2)crystalline grain and the p-type Co_(2)O_(2)crystalline grain.The nanoscale p–n heterojunction promotes the electron migration and forms an interface barrier.The synergy effects between Sn O_(2)and Co_(2)O_(2),the crystalline grain p–n heterojunction,the existence of nanofibers and the large specific surface area all jointly contribute to the improved gas sensing performance.
