The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts hav...The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.展开更多
The lattice-matched XBn structures of InAsSb,grown on GaSb substrates,exhibit high crystal quali⁃ty,and can achieve extremely low dark currents at high operating temperatures(HOT).Its superior performance is attribute...The lattice-matched XBn structures of InAsSb,grown on GaSb substrates,exhibit high crystal quali⁃ty,and can achieve extremely low dark currents at high operating temperatures(HOT).Its superior performance is attributed to the unipolar barrier,which blocks the majority carriers while allowing unhindered hole transport.To further explore the energy band and carrier transport mechanisms of the XBn unipolar barrier structure,this pa⁃per systematically investigates the influence of doping on the dark current,photocurrent,and tunneling character⁃istics of InAsSb photodetectors in the PBn structure.Three high-quality InAsSb samples with unintentionally doped absorption layers(AL)were prepared,with varying p-type doping concentrations in the GaSb contact layer(CL)and the AlAsSb barrier layer(BL).As the p-type doping concentration in the CL increased,the device’s turn-on bias voltage also increased,and p-type doping in the BL led to tunneling occurring at lower bias voltages.For the sample with UID BL,which exhibited an extremely low dark current of 5×10^(-6) A/cm^(2).The photocurrent characteristics were well-fitted using the back-to-back diode model,revealing the presence of two opposing space charge regions on either side of the BL.展开更多
Er^(3+),Na^(+)co-doped CaF_(2) transparent ceramics with Er^(3+)dopant concentration of 3% and Na^(+)of 0%,0.5%,1.0%,1.5% and 2.0% were fabricated by the vacuum hot pressing method with 16 mm in diameter and 3 mm in t...Er^(3+),Na^(+)co-doped CaF_(2) transparent ceramics with Er^(3+)dopant concentration of 3% and Na^(+)of 0%,0.5%,1.0%,1.5% and 2.0% were fabricated by the vacuum hot pressing method with 16 mm in diameter and 3 mm in thickness.The average grain size of the obtained Er,Na∶CaF_(2) powders varied from 28 nm to 36 nm with the shape of sphere.The effects of Na^(+)doping on the transmittance,microstructure and spectral properties of Er^(3+)∶CaF_(2) transparent ceramics were investigated.The transmittance of all the obtained ceramic samples is above 84%in the wavelength of 1000 nm.The results show that after introducing Na^(+)into Er^(3+)∶CaF_(2) transparent ceramics,charge-neutralized Er^(3+)-Na^(+)structure formed which prevent Er^(3+)from clustering.The emission spectra of Er^(3+)in CaF_(2) transparent ceramics at around 1.5 and 2.7μm could be modulated by adjusting the concentration of Na^(+)and the near-infrared fluorescence lifetime at around 1.5μm increase with the increasing of Na^(+)concentration,reaching a maximum of 56.75 ms.展开更多
For a highly efficient recycling of a wastewater containing a high concentration of MgCl_(2),Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high conce...For a highly efficient recycling of a wastewater containing a high concentration of MgCl_(2),Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concentration MgCl_(2)solution at different pH values and Al/P molar ratios was investigated.The results showed that P507 formed organic complexes of Al_(x)(OH)_y^(Z+)-P507 at pH of 2.0-4.0.At pH of 4.0-5.0,Al(Ⅲ)precipitated and transferred into Al(OH)_(3)with a flocculent amorphous morphology.Active sites on the Al(OH)_(3)surface enhanced the removal efficiency of P507.At pH of 6.0-6.5,Al(Ⅲ)and Mg(Ⅱ)formed layered crystalline Al(OH)_(3)and MgAl_(2)(OH)_(8with)small pore channels and fewer active sites,resulting in a reduced removal efficiency of P507.When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0,the removal rates of both Al(Ⅲ)and P507 were higher than98%,while the concentration loss of Mg(Ⅱ)was only 0.2%-0.9%.展开更多
Defect engineering by heteroatom doping gives carbon materials some new characteristics such as a different electronic structure and a high electrochemical activity,making them suitable for high-performance applicatio...Defect engineering by heteroatom doping gives carbon materials some new characteristics such as a different electronic structure and a high electrochemical activity,making them suitable for high-performance applications.N-doping has been widely investigated because of its similar atom radius to carbon,high electronegativity as well as many different configurations.We summarize the preparation methods and properties of N-doped carbon materials,and discuss their possible use in sodium ion storage.The relationships between N content/configuration and crystallinity,electronic conductivity,wettability,chemical reactivity as well as sodium ion storage performance are discussed.展开更多
A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incor...A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incorporation of multi⁃wall carbon nanotubes and employing freeze drying technology.The material amalgamates the merits of 1D/2D hybrid carbon materials,wherein 1D carbon nanotubes confer robustness and expedited elec⁃tron transport pathways,while 2D graphene sheets facilitate rapid ion migration.Furthermore,the introduction of nitrogen heteroatoms serves to furnish additional active sites for lithium storage.When served as an anode material for lithium⁃ion batteries,the CS⁃GO⁃NCNT electrode delivered a reversible capacity surpassing 500 mAh·g^(-1),mark⁃edly outperforming commercial graphite anodes.Even after 300 cycles at a high current density of 1 A·g^(-1),it remained a reversible capacity of up to 268 mAh·g^(-1).展开更多
To replace precious metal oxygen reduction reaction(ORR)electrocatalysts,many transition metals and N-doped car-bon composites have been proposed in the last decade resulting in their rapid development as promising no...To replace precious metal oxygen reduction reaction(ORR)electrocatalysts,many transition metals and N-doped car-bon composites have been proposed in the last decade resulting in their rapid development as promising non-precious metal catalysts.We used Ketjenblack carbon as the precursor and mixed it with a polymeric ionic liquid(PIL)of[Hvim]NO_(3) and Fe(NO_(3))_(3),which was thermally calcined at 900℃ to produce a porous FeO_(x),N co-doped carbon material denoted FeO_(x)-N/C.Because the PIL of[Hvim]NO_(3) strongly combines with and disperses Fe^(3+)ions,and NO_(3)−is thermally pyrolyzed to form the porous structure,the FeO_(x)-N/C catalyst has a high electrocatalytic activity for the ORR in both 0.1 mol L^(−1) KOH and 0.5 mol L^(−1) H_(2)SO_(4) electrolytes.It was used as the catalyst to assemble a zinc-air battery,which had a peak power density of 185 mW·cm^(−2).Its superior electrocatalytic activity,wide pH range,and easy preparation make FeO_(x)-N/C a promising electrocatalyst for fuel cells and metal-air batteries.展开更多
To predict complex reservoir spaces(with developed caves,pores,and fractures),based on the results of full-azimuth depth migration processing,we adopted reverse weighted nonlinear inversion to improve the accuracy of ...To predict complex reservoir spaces(with developed caves,pores,and fractures),based on the results of full-azimuth depth migration processing,we adopted reverse weighted nonlinear inversion to improve the accuracy of porous reservoir prediction.Scattering imaging three-parameter wavelet transform technology was used to accurately predict small-scale cave bodies.The joint inversion method of velocity and amplitude anisotropy was developed to improve the accuracy of small and medium-sized fracture prediction.The results of multiscale fracture modeling and characterization,interwell connectivity analysis,and connection path prediction are consistent with the production condition.Finally,based on the above prediction findings,favorable reservoir development areas were predicted.The above ideas and strategies have great application value for the efficient exploration and development of complex storage space reservoirs and the optimization of high-yield well locations.展开更多
In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morpholo...In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morphology and structure of N,S⁃CDs were characterized by transmission electron microscope,X⁃ray diffrac⁃tion,Fourier transform infrared spectroscopy,and X⁃ray photoelectron spectroscopy,and the basic photophysical properties were investigated via UV⁃Vis absorption spectra and fluorescence spectra.Meanwhile,the N,S⁃CDs have excellent luminescence stability with pH,ionic strength,radiation time,and storage time.Experimental results illus⁃trated the present sensor platform exhibited high sensitivity and selectivity in response to baicalein with a detection limit of 85 nmol·L-1.The quenching mechanism is proved to be the inner filter effect.In addition,this sensor can also detect baicalein in biofluids(serum and urine)with good accuracy and reproducibility.展开更多
To clarify the precipitation of silica hydrate from the real desilication solutions of aluminosilicate solid wastes by adding seeds and improve integrated waste utilization,the seeded precipitation was studied using s...To clarify the precipitation of silica hydrate from the real desilication solutions of aluminosilicate solid wastes by adding seeds and improve integrated waste utilization,the seeded precipitation was studied using synthesized sodium silicate solution containing different inorganic salt impurities.The results show that sodium chloride,sodium sulfate,sodium carbonate,or calcium chloride can change the siloxy group structure.The number of high-polymeric siloxy groups decreases with increasing sodium chloride or sodium sulfate concentration,which is detrimental to seeded precipitation.Calcium chloride favors the polymerization of silicate ions,and even the chain groups precipitate with the precipitation of high-polymeric sheet and cage-like siloxy groups.The introduced sodium cations in sodium carbonate render a more open network structure of high-polymeric siloxy groups,although the carbonate ions favor the polymerization of siloxy groups.No matter how the four impurities affect the siloxy group structure,the precipitates are always amorphous opal-A silica hydrate.展开更多
Octahedral Mn_(3)O_(4)nanoparticles with an Ag-doping and nanoporous Ag(NPS)framework was simply fabricated through an alloying-etching engineering.The dual-modified Mn_(3)O_(4)(denoted as Ag−Mn_(3)O_(4)/NPS)consists ...Octahedral Mn_(3)O_(4)nanoparticles with an Ag-doping and nanoporous Ag(NPS)framework was simply fabricated through an alloying-etching engineering.The dual-modified Mn_(3)O_(4)(denoted as Ag−Mn_(3)O_(4)/NPS)consists of Ag-doped Mn_(3)O_(4)nanoparticles crosslinked with three dimensional nanoporous Ag framework.The incorporated Ag dopant is effective in improving the intrinsic ionic and electronic conductivities of Mn_(3)O_(4),while the NPS framework is introduced to improve the electron/mass transfer across the entire electrode.Profiting from the dual-modification strategy,the Ag−Mn_(3)O_(4)/NPS exhibits admirable rate capability and cycling stability.A high reversible capacity of 88.7 mA·h/g can still be retained for over 1000 cycles at a current density of 1 A/g.Moreover,a series of ex-situ experimental techniques indicate that for Ag−Mn_(3)O_(4)/NPS electrode during the zinc ion storage,Mn_(3)O_(4)is electrochemically oxidized into various MnOx(e.g.,Mn_(2)O_(3),MnO2)species in the initial charging,and the subsequent battery reaction is actually the intercalation/deintercalation of H+and Zn2+into MnOx.展开更多
Controlling the local electronic structure of active ingredients to improve the adsorption desorption characteristics of oxygen-containing intermediates over the electrochemical liquid-solid interfaces is a critical c...Controlling the local electronic structure of active ingredients to improve the adsorption desorption characteristics of oxygen-containing intermediates over the electrochemical liquid-solid interfaces is a critical challenge in the field of oxygen reduction reaction(ORR)catalysis.Here,we offer a simple approach for modulating the electronic states of metal nanocrystals by bimetal co-doping into carbon-nitrogen substrate,allowing us to modulate the electronic structure of catalytic active centers.To test our strategy,we designed a typical bimetallic nanoparticle catalyst(Fe-Co NP/NC)to flexibly alter the reaction kinetics of ORR.Our results from synchrotron Xray absorption spectroscopy and X-ray photoelectron spectroscopy showed that the co-doping of iron and cobalt could optimize the intrinsic charge distribution of Fe-Co NP/NC catalyst,promoting the oxygen reduction kinetics and ultimately achieving remarkable ORR activity.Consequently,the carefully designed Fe-Co NP/NC exhibits an ultra-high kinetic current density at the operating voltage(71.94 mA/cm^(2)at 0.80 V),and the half-wave potential achieves 0.915 V,which is obviously better than that of the corresponding controls including Fe NP/NC,Co NP/NC.Our findings provide a unique perspective for optimizing the electronic structure of active centers to achieve higher ORR catalytic activity and faster kinetics.展开更多
Materials with low thermal conductivity are applied extensively in energy management,and breaking the amorphous limits of thermal conductivity to solids has attracted widespread attention from scientists.Doping is a c...Materials with low thermal conductivity are applied extensively in energy management,and breaking the amorphous limits of thermal conductivity to solids has attracted widespread attention from scientists.Doping is a common strategy for achieving low thermal conductivity that can offer abundant scattering centers in which heavier dopants always result in lower phonon group velocities and lower thermal conductivities.However,the amount of equivalent heavyatom single dopant available is limited.Unfortunately,nonequivalent heavy dopants have finite solubility because of charge imbalance.Here,we propose a charge balance strategy for SnS by substituting Sn2+with Ag^(+)and heavy Bi^(3+),improving the doping limit of Ag from 2%to 3%.Ag and Bi codoping increases the point defect concentration and introduces abundant boundaries simultaneously,scattering the phonons at both the atomic scale and nanoscale.The thermal conductivity of Ag0.03Bi0.03Sn0.94S decreased to 0.535 W·m^(−1)·K^(−1)at room temperature and 0.388 W·m^(−1)·K^(−1)at 275°C,which is below the amorphous limit of 0.450 W·m^(−1)·K^(−1)for SnS.This strategy offers a simple way to enhance the doping limit and achieve ultralow thermal conductivity in solids below the amorphous limit without precise structural modification.展开更多
Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile...Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile,identifying the active site also represents a significant obstacle,primarily due to the intricate electronic environment of single atom site doped metal oxide.Herein,a single atom Cu doped TiO_(2)catalyst(Cu_(1)-TiO_(2)) is prepared via a simple“colloid-acid treatment”strategy,which switches aniline oxidation selectivity of TiO_(2) from azoxybenzene to nitrosobenzene,without using additives or changing solvent,while other metal or nonmetal doped TiO_(2) did not possess.Comprehensive mechanistic investigations and DFT calculations unveil that Ti-O active site is responsible for triggering the aniline to form a new PhNOH intermediate,two PhNOH condense to azoxybenzene over TiO_(2) catalyst.As for Cu_(1)-TiO_(2),the charge-specific distribution between the isolated Cu and TiO_(2) generates unique Cu_(1)-O-Ti hybridization structure with nine catalytic active sites,eight of them make PhNOH take place spontaneous dissociation to produce nitrosobenzene.This work not only unveils a new mechanistic pathway featuring the PhNOH intermediate in aniline oxidation for the first time but also presents a novel approach for constructing single-atom doped metal oxides and exploring their intricate active sites.展开更多
To fully exploit the technical advantages of the large-depth and high-precision artificial source electromagnetic method in the complex structure area of southern Sichuan and compensate for the shortcomings of the con...To fully exploit the technical advantages of the large-depth and high-precision artificial source electromagnetic method in the complex structure area of southern Sichuan and compensate for the shortcomings of the conventional electromagnetic method in exploration depth,precision,and accuracy,the large-depth and high-precision wide field electromagnetic method is applied to the complex structure test area of the Luochang syncline and Yuhe nose anticline in the southern Sichuan.The advantages of the wide field electromagnetic method in detecting deep,low-resistivity thin layers are demonstrated.First,on the basis of the analysis of physical property data,a geological–geoelectric model is established in the test area,and the wide field electromagnetic method is numerically simulated to analyze and evaluate the response characteristics of deep thin shale gas layers on wide field electromagnetic curves.Second,a wide field electromagnetic test is conducted in the complex structure area of southern Sichuan.After data processing and inversion imaging,apparent resistivity logging data are used for calibration to develop an apparent resistivity interpretation model suitable for the test area.On the basis of the results,the characteristics of the electrical structure change in the shallow longitudinal formation of 6 km are implemented,and the transverse electrical distribution characteristics of the deep shale gas layer are delineated.In the prediction area near the well,the subsequent data verification shows that the apparent resistivity obtained using the inversion of the wide field electromagnetic method is consistent with the trend of apparent resistivity revealed by logging,which proves that this method can effectively identify the weak response characteristics of deep shale gas formations in complex structural areas.This experiment,it is shown shows that the wide field electromagnetic method with a large depth and high precision can effectively characterize the electrical characteristics of deep,low-resistivity thin layers in complex structural areas,and a new set of low-cost evaluation technologies for shale gas target layers based on the wide field electromagnetic method is explored.展开更多
文摘The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.
基金Supported by the Candidate Talents Training Fund of Yunnan Province(202205AC160054)the National Natural Science Foundation of China(62174156)。
文摘The lattice-matched XBn structures of InAsSb,grown on GaSb substrates,exhibit high crystal quali⁃ty,and can achieve extremely low dark currents at high operating temperatures(HOT).Its superior performance is attributed to the unipolar barrier,which blocks the majority carriers while allowing unhindered hole transport.To further explore the energy band and carrier transport mechanisms of the XBn unipolar barrier structure,this pa⁃per systematically investigates the influence of doping on the dark current,photocurrent,and tunneling character⁃istics of InAsSb photodetectors in the PBn structure.Three high-quality InAsSb samples with unintentionally doped absorption layers(AL)were prepared,with varying p-type doping concentrations in the GaSb contact layer(CL)and the AlAsSb barrier layer(BL).As the p-type doping concentration in the CL increased,the device’s turn-on bias voltage also increased,and p-type doping in the BL led to tunneling occurring at lower bias voltages.For the sample with UID BL,which exhibited an extremely low dark current of 5×10^(-6) A/cm^(2).The photocurrent characteristics were well-fitted using the back-to-back diode model,revealing the presence of two opposing space charge regions on either side of the BL.
基金National Key R&D Program of China(2023YFB3507400)。
文摘Er^(3+),Na^(+)co-doped CaF_(2) transparent ceramics with Er^(3+)dopant concentration of 3% and Na^(+)of 0%,0.5%,1.0%,1.5% and 2.0% were fabricated by the vacuum hot pressing method with 16 mm in diameter and 3 mm in thickness.The average grain size of the obtained Er,Na∶CaF_(2) powders varied from 28 nm to 36 nm with the shape of sphere.The effects of Na^(+)doping on the transmittance,microstructure and spectral properties of Er^(3+)∶CaF_(2) transparent ceramics were investigated.The transmittance of all the obtained ceramic samples is above 84%in the wavelength of 1000 nm.The results show that after introducing Na^(+)into Er^(3+)∶CaF_(2) transparent ceramics,charge-neutralized Er^(3+)-Na^(+)structure formed which prevent Er^(3+)from clustering.The emission spectra of Er^(3+)in CaF_(2) transparent ceramics at around 1.5 and 2.7μm could be modulated by adjusting the concentration of Na^(+)and the near-infrared fluorescence lifetime at around 1.5μm increase with the increasing of Na^(+)concentration,reaching a maximum of 56.75 ms.
基金financial supports from the National Key Research and Development Program of China(No.2022YFB3504501)the National Natural Science Foundation of China(Nos.52274355,91962211)the Gansu Province Science and Technology Major Special Project,China(No.22ZD6GD061)。
文摘For a highly efficient recycling of a wastewater containing a high concentration of MgCl_(2),Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concentration MgCl_(2)solution at different pH values and Al/P molar ratios was investigated.The results showed that P507 formed organic complexes of Al_(x)(OH)_y^(Z+)-P507 at pH of 2.0-4.0.At pH of 4.0-5.0,Al(Ⅲ)precipitated and transferred into Al(OH)_(3)with a flocculent amorphous morphology.Active sites on the Al(OH)_(3)surface enhanced the removal efficiency of P507.At pH of 6.0-6.5,Al(Ⅲ)and Mg(Ⅱ)formed layered crystalline Al(OH)_(3)and MgAl_(2)(OH)_(8with)small pore channels and fewer active sites,resulting in a reduced removal efficiency of P507.When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0,the removal rates of both Al(Ⅲ)and P507 were higher than98%,while the concentration loss of Mg(Ⅱ)was only 0.2%-0.9%.
文摘Defect engineering by heteroatom doping gives carbon materials some new characteristics such as a different electronic structure and a high electrochemical activity,making them suitable for high-performance applications.N-doping has been widely investigated because of its similar atom radius to carbon,high electronegativity as well as many different configurations.We summarize the preparation methods and properties of N-doped carbon materials,and discuss their possible use in sodium ion storage.The relationships between N content/configuration and crystallinity,electronic conductivity,wettability,chemical reactivity as well as sodium ion storage performance are discussed.
文摘A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incorporation of multi⁃wall carbon nanotubes and employing freeze drying technology.The material amalgamates the merits of 1D/2D hybrid carbon materials,wherein 1D carbon nanotubes confer robustness and expedited elec⁃tron transport pathways,while 2D graphene sheets facilitate rapid ion migration.Furthermore,the introduction of nitrogen heteroatoms serves to furnish additional active sites for lithium storage.When served as an anode material for lithium⁃ion batteries,the CS⁃GO⁃NCNT electrode delivered a reversible capacity surpassing 500 mAh·g^(-1),mark⁃edly outperforming commercial graphite anodes.Even after 300 cycles at a high current density of 1 A·g^(-1),it remained a reversible capacity of up to 268 mAh·g^(-1).
文摘To replace precious metal oxygen reduction reaction(ORR)electrocatalysts,many transition metals and N-doped car-bon composites have been proposed in the last decade resulting in their rapid development as promising non-precious metal catalysts.We used Ketjenblack carbon as the precursor and mixed it with a polymeric ionic liquid(PIL)of[Hvim]NO_(3) and Fe(NO_(3))_(3),which was thermally calcined at 900℃ to produce a porous FeO_(x),N co-doped carbon material denoted FeO_(x)-N/C.Because the PIL of[Hvim]NO_(3) strongly combines with and disperses Fe^(3+)ions,and NO_(3)−is thermally pyrolyzed to form the porous structure,the FeO_(x)-N/C catalyst has a high electrocatalytic activity for the ORR in both 0.1 mol L^(−1) KOH and 0.5 mol L^(−1) H_(2)SO_(4) electrolytes.It was used as the catalyst to assemble a zinc-air battery,which had a peak power density of 185 mW·cm^(−2).Its superior electrocatalytic activity,wide pH range,and easy preparation make FeO_(x)-N/C a promising electrocatalyst for fuel cells and metal-air batteries.
文摘To predict complex reservoir spaces(with developed caves,pores,and fractures),based on the results of full-azimuth depth migration processing,we adopted reverse weighted nonlinear inversion to improve the accuracy of porous reservoir prediction.Scattering imaging three-parameter wavelet transform technology was used to accurately predict small-scale cave bodies.The joint inversion method of velocity and amplitude anisotropy was developed to improve the accuracy of small and medium-sized fracture prediction.The results of multiscale fracture modeling and characterization,interwell connectivity analysis,and connection path prediction are consistent with the production condition.Finally,based on the above prediction findings,favorable reservoir development areas were predicted.The above ideas and strategies have great application value for the efficient exploration and development of complex storage space reservoirs and the optimization of high-yield well locations.
文摘In this work,p⁃phenylenediamine and L⁃cysteine were used as raw materials,and water⁃soluble N,S co⁃doped carbon dots(N,S⁃CDs)with excellent performance were prepared through a one⁃step solvothermal method.The morphology and structure of N,S⁃CDs were characterized by transmission electron microscope,X⁃ray diffrac⁃tion,Fourier transform infrared spectroscopy,and X⁃ray photoelectron spectroscopy,and the basic photophysical properties were investigated via UV⁃Vis absorption spectra and fluorescence spectra.Meanwhile,the N,S⁃CDs have excellent luminescence stability with pH,ionic strength,radiation time,and storage time.Experimental results illus⁃trated the present sensor platform exhibited high sensitivity and selectivity in response to baicalein with a detection limit of 85 nmol·L-1.The quenching mechanism is proved to be the inner filter effect.In addition,this sensor can also detect baicalein in biofluids(serum and urine)with good accuracy and reproducibility.
基金financial support from the National Natural Science Foundation of China(No.52074364)。
文摘To clarify the precipitation of silica hydrate from the real desilication solutions of aluminosilicate solid wastes by adding seeds and improve integrated waste utilization,the seeded precipitation was studied using synthesized sodium silicate solution containing different inorganic salt impurities.The results show that sodium chloride,sodium sulfate,sodium carbonate,or calcium chloride can change the siloxy group structure.The number of high-polymeric siloxy groups decreases with increasing sodium chloride or sodium sulfate concentration,which is detrimental to seeded precipitation.Calcium chloride favors the polymerization of silicate ions,and even the chain groups precipitate with the precipitation of high-polymeric sheet and cage-like siloxy groups.The introduced sodium cations in sodium carbonate render a more open network structure of high-polymeric siloxy groups,although the carbonate ions favor the polymerization of siloxy groups.No matter how the four impurities affect the siloxy group structure,the precipitates are always amorphous opal-A silica hydrate.
基金financially supported by the Natural Science Foundation of Shandong Province,China (Nos.ZR2023ME155,ZR2023ME085)the National Natural Science Foundation of China (No.52201254)+1 种基金the Project of“20 Items of University”of Jinan,China (No.202228046)the Taishan Scholar Project of Shandong Province,China (No.tsqn202306226)。
文摘Octahedral Mn_(3)O_(4)nanoparticles with an Ag-doping and nanoporous Ag(NPS)framework was simply fabricated through an alloying-etching engineering.The dual-modified Mn_(3)O_(4)(denoted as Ag−Mn_(3)O_(4)/NPS)consists of Ag-doped Mn_(3)O_(4)nanoparticles crosslinked with three dimensional nanoporous Ag framework.The incorporated Ag dopant is effective in improving the intrinsic ionic and electronic conductivities of Mn_(3)O_(4),while the NPS framework is introduced to improve the electron/mass transfer across the entire electrode.Profiting from the dual-modification strategy,the Ag−Mn_(3)O_(4)/NPS exhibits admirable rate capability and cycling stability.A high reversible capacity of 88.7 mA·h/g can still be retained for over 1000 cycles at a current density of 1 A/g.Moreover,a series of ex-situ experimental techniques indicate that for Ag−Mn_(3)O_(4)/NPS electrode during the zinc ion storage,Mn_(3)O_(4)is electrochemically oxidized into various MnOx(e.g.,Mn_(2)O_(3),MnO2)species in the initial charging,and the subsequent battery reaction is actually the intercalation/deintercalation of H+and Zn2+into MnOx.
基金supported by the Natural Science Foundation of Anhui Province(No.2208085J01 and No.2208085QA28).
文摘Controlling the local electronic structure of active ingredients to improve the adsorption desorption characteristics of oxygen-containing intermediates over the electrochemical liquid-solid interfaces is a critical challenge in the field of oxygen reduction reaction(ORR)catalysis.Here,we offer a simple approach for modulating the electronic states of metal nanocrystals by bimetal co-doping into carbon-nitrogen substrate,allowing us to modulate the electronic structure of catalytic active centers.To test our strategy,we designed a typical bimetallic nanoparticle catalyst(Fe-Co NP/NC)to flexibly alter the reaction kinetics of ORR.Our results from synchrotron Xray absorption spectroscopy and X-ray photoelectron spectroscopy showed that the co-doping of iron and cobalt could optimize the intrinsic charge distribution of Fe-Co NP/NC catalyst,promoting the oxygen reduction kinetics and ultimately achieving remarkable ORR activity.Consequently,the carefully designed Fe-Co NP/NC exhibits an ultra-high kinetic current density at the operating voltage(71.94 mA/cm^(2)at 0.80 V),and the half-wave potential achieves 0.915 V,which is obviously better than that of the corresponding controls including Fe NP/NC,Co NP/NC.Our findings provide a unique perspective for optimizing the electronic structure of active centers to achieve higher ORR catalytic activity and faster kinetics.
基金supported by the CAS Project for Young Scientists in Basic Research(YSBR-070)the National Natural Science Foundation of China(21925110,21890750,U2032161,12147105)+8 种基金the USTC Research Funds of the Double First-Class Initiative(YD2060002004)the National Key Research and Development Program of China(2022YFA1203600,2022YFA1203601,2022YFA1203602)the Natural Science Foundation of China-Anhui Joint Fund(U23A20121)the Outstanding Youth Foundation of Anhui Province(2208085J14)the Anhui Provincial Key Research and Development Project(202004a050200760)the Key R&D Program of Shandong Province(2021CXGC010302)the Users with Excellence Project of Hefei Science Center CAS(2021HSC-UE004)the Fellowship of the China Postdoctoral Science Foundation(2022M710141)the open foundation of the Key Laboratory of the Engineering Research Center of Building Energy Efficiency Control and Evaluation,Ministry of Education(AHJZNX-2023-04).
文摘Materials with low thermal conductivity are applied extensively in energy management,and breaking the amorphous limits of thermal conductivity to solids has attracted widespread attention from scientists.Doping is a common strategy for achieving low thermal conductivity that can offer abundant scattering centers in which heavier dopants always result in lower phonon group velocities and lower thermal conductivities.However,the amount of equivalent heavyatom single dopant available is limited.Unfortunately,nonequivalent heavy dopants have finite solubility because of charge imbalance.Here,we propose a charge balance strategy for SnS by substituting Sn2+with Ag^(+)and heavy Bi^(3+),improving the doping limit of Ag from 2%to 3%.Ag and Bi codoping increases the point defect concentration and introduces abundant boundaries simultaneously,scattering the phonons at both the atomic scale and nanoscale.The thermal conductivity of Ag0.03Bi0.03Sn0.94S decreased to 0.535 W·m^(−1)·K^(−1)at room temperature and 0.388 W·m^(−1)·K^(−1)at 275°C,which is below the amorphous limit of 0.450 W·m^(−1)·K^(−1)for SnS.This strategy offers a simple way to enhance the doping limit and achieve ultralow thermal conductivity in solids below the amorphous limit without precise structural modification.
文摘Utilizing single atom sites doping into metal oxides to modulate their intrinsic active sites,achieving precise selectivity control in complex organic reactions,is a highly desirable yet challenging endeavor.Meanwhile,identifying the active site also represents a significant obstacle,primarily due to the intricate electronic environment of single atom site doped metal oxide.Herein,a single atom Cu doped TiO_(2)catalyst(Cu_(1)-TiO_(2)) is prepared via a simple“colloid-acid treatment”strategy,which switches aniline oxidation selectivity of TiO_(2) from azoxybenzene to nitrosobenzene,without using additives or changing solvent,while other metal or nonmetal doped TiO_(2) did not possess.Comprehensive mechanistic investigations and DFT calculations unveil that Ti-O active site is responsible for triggering the aniline to form a new PhNOH intermediate,two PhNOH condense to azoxybenzene over TiO_(2) catalyst.As for Cu_(1)-TiO_(2),the charge-specific distribution between the isolated Cu and TiO_(2) generates unique Cu_(1)-O-Ti hybridization structure with nine catalytic active sites,eight of them make PhNOH take place spontaneous dissociation to produce nitrosobenzene.This work not only unveils a new mechanistic pathway featuring the PhNOH intermediate in aniline oxidation for the first time but also presents a novel approach for constructing single-atom doped metal oxides and exploring their intricate active sites.
文摘To fully exploit the technical advantages of the large-depth and high-precision artificial source electromagnetic method in the complex structure area of southern Sichuan and compensate for the shortcomings of the conventional electromagnetic method in exploration depth,precision,and accuracy,the large-depth and high-precision wide field electromagnetic method is applied to the complex structure test area of the Luochang syncline and Yuhe nose anticline in the southern Sichuan.The advantages of the wide field electromagnetic method in detecting deep,low-resistivity thin layers are demonstrated.First,on the basis of the analysis of physical property data,a geological–geoelectric model is established in the test area,and the wide field electromagnetic method is numerically simulated to analyze and evaluate the response characteristics of deep thin shale gas layers on wide field electromagnetic curves.Second,a wide field electromagnetic test is conducted in the complex structure area of southern Sichuan.After data processing and inversion imaging,apparent resistivity logging data are used for calibration to develop an apparent resistivity interpretation model suitable for the test area.On the basis of the results,the characteristics of the electrical structure change in the shallow longitudinal formation of 6 km are implemented,and the transverse electrical distribution characteristics of the deep shale gas layer are delineated.In the prediction area near the well,the subsequent data verification shows that the apparent resistivity obtained using the inversion of the wide field electromagnetic method is consistent with the trend of apparent resistivity revealed by logging,which proves that this method can effectively identify the weak response characteristics of deep shale gas formations in complex structural areas.This experiment,it is shown shows that the wide field electromagnetic method with a large depth and high precision can effectively characterize the electrical characteristics of deep,low-resistivity thin layers in complex structural areas,and a new set of low-cost evaluation technologies for shale gas target layers based on the wide field electromagnetic method is explored.