Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon products.However,such reactions require stringent conditions on local environments of catalyst surfaces,...Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon products.However,such reactions require stringent conditions on local environments of catalyst surfaces,which currently are the global pressing challenges.Here,a stabilized activation of Cu^(0)/Cu^(+)-onAg interface by N_(2) cold plasma treatment was developed for improving Faradaic efficiency(FE) of CO_(2)RR into C2 products.The resultant Ag@Cu-CuN_x exhibits a C2 FE of 72% with a partial current density of-14.9 mA cm^(-2) at-1.0 V vs.RHE(reversible hydrogen electrode).Combining density functional theory(DFT) and experimental investigations,we unveiled that Cu^(0)/Cu^(+) species can be co ntrollably tu ned by the incorporation of nitrogen to form CuN_x on Ag surface,i.e.,Ag@Cu-CuN_x.This strategy enhances ^(*)CO intermediates generation and accelerates C-C coupling both thermodynamically and kinetically.The intermediates O^(*)C^(*)CO,^(*)COOH,and ^(*)CO were detected by in-situ attenuated total internal reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS).The uncovered CO_(2)RR-into-C2 products were carried out along CO_(2)→^(*)COOH→^(*)CO→O^(*)C^(*)CO→^(*)C_(2)H_(3)O→^(*)C_(2)H_(4)O→ C_(2)H_(5)OH(or ^(*)C_(2)H_(3)O→^(*)O+C_(2)H_(4)) paths over Ag@Cu-CuN_x electrocatalyst.This work provides a new approach to design Cu-based electrocatalysts with high-efficiency,mild condition,and stable CO_(2)RR to C2 products.展开更多
Non-thermal plasma(NTP)is considered to be a promising technology for the removal of volatile organic compounds;however,its application is limited by low CO_(2) selectivity and undesirable by-products.To overcome thes...Non-thermal plasma(NTP)is considered to be a promising technology for the removal of volatile organic compounds;however,its application is limited by low CO_(2) selectivity and undesirable by-products.To overcome these issues,this paper discusses the degradation of chlorobenzene(CB)in systems of NTP coupled with catalysts,and the influence of catalyst locations in the NTP was investigated.In addition,the interaction between plasma and catalyst was also explored.The results indicated that the degradability of CB was remarkably improved through the combination of NTP with catalysts,and the formation of ozone was effectively inhibited.The degradation efficiency increased from 33.9%to 79.6%at 14 kV in the NTPcatalytic system,while the ozone concentration decreased from 437 to 237 mg m^(-3),and the degradation efficiency of in plasma catalysis(IPC)systems was superior to that of the post plasma catalysis system,while the inhibition ability of ozone exhibited an opposing trend.In the IPC system,the degradation efficiency was 87.7%at 14 k V,while the ozone concentration was151 mg m^(-3).Besides,the plasma did not destroy the pore structure and crystal structure of the catalyst,but affected the surface morphology and redox performance of the catalyst.Thus,NTP coupled catalytic system could improve the degradation performance of CB.Furthermore,the plasma discharge characteristics played a major role in the NTP synergistic catalytic degradation of CB.Finally,based on the experiment analysis results,the general reaction mechanism of CB degradation in an IPC reaction system was proposed.展开更多
Electrocatalytic CO_(2)reduction reaction to low-carbon alcohol is a challenging task,especially high selectivity for ethanol,which is mainly limited by the regulation of reaction intermediates and subsequent C–C cou...Electrocatalytic CO_(2)reduction reaction to low-carbon alcohol is a challenging task,especially high selectivity for ethanol,which is mainly limited by the regulation of reaction intermediates and subsequent C–C coupling.A Cu-Co bimetallic catalyst with CN vacancies is successfully developed by H_(2)cold plasma toward a high-efficiency CO_(2)RR into low-carbon alcohol.The Cu-Co PBA-V_(CN)(Prussian blue analogues with CN vacancies)electrocatalyst yields methanol and ethanol as major products with a total low-carbon alcohol FE of 83.8%(methanol:39.2%,ethanol:44.6%)at-0.9 V vs.RHE,excellent durability(100 h)and a small onset potential of-0.21 V.ATR-SEIRAS(attenuated total internal reflection surface enhanced infrared absorption spectroscopy)and DFT(density functional theory)reveal that the steric hindrance of V_(CN)can enhance the CO generation from*COOH,and the C–C coupling can also be increased by CO spillover on uniformly dispersed Cu atoms.This work provides a strategy for the design and preparation of electrocatalysts for CO_(2)RR into low-carbon alcohol products and highlights the impact of catalyst steric hindrance to catalytic performance.展开更多
In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can r...In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.展开更多
High activity and productivity of MoVNbTeO_(x) catalyst are challenging tasks in oxidative dehydrogenation of ethane(ODHE)for industrial application.In this work,phase-pure M1 with 30 wt%CeO_(2) composite catalyst was...High activity and productivity of MoVNbTeO_(x) catalyst are challenging tasks in oxidative dehydrogenation of ethane(ODHE)for industrial application.In this work,phase-pure M1 with 30 wt%CeO_(2) composite catalyst was treated by oxygen plasma to further enhance catalyst performance.The results show that the oxygen vacancies generated by the solid-state redox reaction between M1 and CeO_(2) capture active oxygen species in gas and transform V^(4+)to V^(5+)without damage to M1 structure.The space-time yield of ethylene of the plasma-treated catalyst was significantly increased,in which the catalyst shows an enhancement near~100% than that of phase-pure M1 at 400℃ for ODHE process.Plasma treatment for catalysts demonstrates an effective way to convert electrical energy into chemical energy in catalyst materials.Energy conversion is achieved by using the catalyst as a medium.展开更多
Efficient,stable and economical catalysts play a crucial role in enhancing the kinetics of slow oxygen reduction reactions(ORR)in Aluminum-air batteries.Among the potential next-generation candidates,Ag catalysts are ...Efficient,stable and economical catalysts play a crucial role in enhancing the kinetics of slow oxygen reduction reactions(ORR)in Aluminum-air batteries.Among the potential next-generation candidates,Ag catalysts are promising due to their high activity and low cost,but weaker oxygen adsorption has hindered industrialization.To address this bottleneck,Ag-alloying has emerged as a principal strategy.In this work,we successfully prepared Ag-Cu nanoparticles(NPs)with a rich eutectic phase and uniform dispersion structure using plasma evaporation.The increased solid solution of Ag and Cu led to changes in the electronic structure,resulting in an upward shift of the d-band center,which significantly improved oxygen adsorption.The combination of Ag and Cu in the NPs synergistically enhanced the adsorption of Ag and the desorption of Cu.Density functional theory(DFT)calculations revealed that Ag-Cu25 NPs exhibited the smallest limiting reaction barrier,leading to increased ORR activity.To further optimize the catalyst’s performance,we utilized N-doped porous nanocarbon(N-PC)with high electrical conductivity and abundant mesoporous channels as the support for the Ag-Cu NPs.The N-PC support provided optimal mass transfer carriers for the highly active Ag-Cu25 NPs.As a result,the Ag-Cu25/NPC catalyst displayed excellent ORR activity in alkaline media,with a half-wave potential(E_(1/2))of 0.82 V.Furthermore,the Al-air battery incorporating the Ag-Cu25/NPC catalyst exhibited outstanding electrochemical performance.It demonstrated high open-circuit voltages of 1.89 V and remarkable power densities of 193 m W cm^(-2).The battery also sustained a high current output and maintained a stable high voltage for 120 hours under mechanical charging,showcasing its significant potential for practical applications.展开更多
A study of the behaviors of air discharge plasma inside a catalyst’s pores is important to understand the plasma catalysis mechanism;however,few articles have reported the generation characteristics of air plasma in ...A study of the behaviors of air discharge plasma inside a catalyst’s pores is important to understand the plasma catalysis mechanism;however,few articles have reported the generation characteristics of air plasma in the pores of catalysts.The production of air microdischarge in a pore was studied by a two-dimensional fluid model,mainly focusing on the effect of pore size and applied voltage.The results show that an increase in the pore size in the range of 20–100μm facilitates the occurrence of microdischarge in the pore.In addition,at an applied voltage of 9 kV,the ionization of air mainly occurs near the topside of the pore when the pore diameter is less than 20μm,leading to a low plasma density in the pore,but the time-averaged plasma density in the pore reaches a maximum value at a 70μm pore diameter.Moreover,the applied voltage also has an important effect on the production of air microdischarge in the pore.The existence of a pore of 80μm diameter on the dielectric has no obvious influence on the plasma density in the pore at 2 kV applied voltage,but the plasma density in the pore begins to sharply rise when the voltage exceeds 3 kV due to the enhanced air ionization at higher applied voltage.The study indicates that microdischarge can be generated in a pore with a size of tens of micrometers,and the microdischarge in porous catalysts will affect the catalytic degradation efficacy of gaseous pollutants.展开更多
Plasma-catalytic dry reforming of CH_(4)(DRM) is promising to convert the greenhouse gasses CH_(4) and CO_(2) into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock f...Plasma-catalytic dry reforming of CH_(4)(DRM) is promising to convert the greenhouse gasses CH_(4) and CO_(2) into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products,because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex,as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, high-lighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems.Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures,at which vibrational excitation can enhance the surface reactions.展开更多
Efficient sterilization by a plasma photocatalytic system(PPS)requires strong synergy between plasma and photocatalyst to inactivate microorganisms while suppressing the formation of secondary pollutants.Here,we repor...Efficient sterilization by a plasma photocatalytic system(PPS)requires strong synergy between plasma and photocatalyst to inactivate microorganisms while suppressing the formation of secondary pollutants.Here,we report that a PPS constructed from a needle array corona discharge and Au/TiO2plasmonic nanocatalyst could remarkably improve the sterilization of Escherichia coli(E.coli)and alleviate formation of the discharge pollutant O3.At 6 kV,the combination of corona discharge and Au/TiO2achieves sterilization efficiency of 100%within an exposure time of 5 min.At 5 kV and an exposure time of 8 min,the presence of Au/TiO2improves sterilization efficiency of the corona discharge from 73%to 91%and reduces the O3concentration from 0.38 to 0.04 ppm,whereas the presence of TiO2reduces the sterilization efficiency and O3concentration to 66%and 0.17 ppm,respectively.The Au/TiO2in the PPS enables a uniform corona discharge,enhances the interaction between plasma,E.coli and nanocatalysts,and suppresses the formation of O3.Further,the Au/TiO2can be excited by ultraviolet-visible light emitted from the plasma to generate electron-hole pairs,and thus contributes to the formation of reactive radicals and the oxidative inactivation of E.coli.The PPS constructed from a needle array corona discharge and Au-based plasmonic nanocatalyst provides a promising approach for developing high-efficiency sterilization techniques.展开更多
Coaxial plasma guns are a type of plasma source that produces plasma which propagates radially and axially controlled by the shape of the ground electrode, which has attracted much interest in several applications. In...Coaxial plasma guns are a type of plasma source that produces plasma which propagates radially and axially controlled by the shape of the ground electrode, which has attracted much interest in several applications. In this work, a 120° opening angle of CPG nozzle is used as a plasma gun configuration that operates at the energy of 150 J. The ionization of polyethylene insulator between the electrodes of the gun produces a cloud of hydrogen and carbon plasma.The triple Langmuir probe and Faraday cup are used to measure plasma density and plasma temperature. These methods are used to measure the on-axis and off-axis plasma divergence of the coaxial plasma gun. The peak values of ion densities measured at a distance of 25 mm on-axis from the plasma gun are(1.6±0.5)×10^(19)m^(-3)and(2.8±0.6)×10^(19)m^(-3)for hydrogen and carbon plasma respectively and the peak temperature is 3.02±0.5 eV. The mean propagation velocity of plasma is calculated using the transit times of plasma at different distances from the plasma gun and is found to be 4.54±0.25 cm/μs and 1.81±0.18 cm/μs for hydrogen and carbon plasma respectively. The Debye radius is obtained from the measured experimental data that satisfies the thin sheath approximation. The shot-to-shot stability of plasma parameters facilitates the use of plasma guns in laboratory experiments. These types of plasma sources can be used in many applications like plasma opening switches, plasma devices, and as plasma sources.展开更多
In astrophysics, the boundary conditions for plasma phenomena are provided by nature and the astronomer faces the problem of understanding them from a variety of observations [Hester J J et al 1996 Astrophys. J. 456 2...In astrophysics, the boundary conditions for plasma phenomena are provided by nature and the astronomer faces the problem of understanding them from a variety of observations [Hester J J et al 1996 Astrophys. J. 456 225], on the other hand, in laboratory plasma experiments the electromagnetic boundary conditions become a major problem in the set-up of the machine that produces the plasma, an issue that has to be investigated step by step and to be modified and adapted with great patience, in particular in the case of an innovative plasma confinement experiment. The PROTO-SPHERA machine [Alladio F et al 2006 Nucl. Fusion 46 S613] is a magnetic confinement experiment, that emulates in the laboratory the jet + torus plasma configurations often observed in astrophysics: an inner magnetized jet of plasma centered on the(approximate) axis of symmetry and surrounded by a magnetized plasma torus orthogonal to this jet. The PROTO-SPHERA plasma is simply connected, i.e., no metal current conducting rod is linked to the plasma torus, while instead it is the inner magnetized plasma jet(in the following always called the plasma centerpost) that is linked to the torus. It is mandatory that no spurious plasma current path modifies the optimal shape of the plasma centerpost. Moreover, as the plasma torus is produced and sustained, in absence of any applied inductive electric field, by the inner plasma centerpost through magnetic reconnections [Taylor J B and Turner M F 1989 Nucl.Fusion 29 219], it is required as well that spurious current paths do not surround the torus on its outboard, in order not to lower the efficiency of the magnetic reconnections that maintain the plasma torus at the expense of the plasma centerpost. Boundary conditions have been corrected,up to the point that the first sustainment in steady state has been achieved for the combined plasma.展开更多
Only a small amount of spectral information is collected because the collection solid angle of the optical fiber probe and lens is very limited when collecting spectral information.To overcome this limitation,this stu...Only a small amount of spectral information is collected because the collection solid angle of the optical fiber probe and lens is very limited when collecting spectral information.To overcome this limitation,this study presents a novel method for acquiring plasma spectral information from various spatial directions.A parabolic-shaped plasma spectral collection device(PSCD)is employed to effectively collect more spectral information into the spectrometer,thereby enhancing the overall spectral intensity.The research objects in this study were soil samples containing different concentrations of heavy metals Pb,Cr,and Cd.The results indicate that the PSCD significantly enhances the spectral signal,with an enhancement rate of up to 45%.Moreover,the signal-to-noise ratio also increases by as much as 36%.Simultaneously,when compared to the absence of a device,it is found that there is no significant variation in plasma temperature when the PSCD is utilized.This observation eliminates the impact of the spatial effect caused by the PSCD on the spectral intensity.Consequently,a concentrationspectral intensity relationship curve is established under the PSCD.The results revealed that the linear fitting R^(2)for Pb,Cr,and Cd increased by 0.011,0.001,and 0.054,respectively.Additionally,the limit of detection(LOD)decreased by 0.361 ppm,0.901 ppm,and 0.602 ppm,respectively.These findings indicate that the spectral enhancement rate elevates with the increase in heavy metal concentration.Hence,the PSCD can effectively enhance the spectral intensity and reduce the detection limit of heavy metals in soil.展开更多
This paper deals with wave propagation and power coupling in blue-core helicon plasma driven by various antennas and frequencies.It is found that compared to non-blue-core mode,for blue-core mode,the wave can propagat...This paper deals with wave propagation and power coupling in blue-core helicon plasma driven by various antennas and frequencies.It is found that compared to non-blue-core mode,for blue-core mode,the wave can propagate in the core region,and it decays sharply outside the core.The power absorption is lower and steeper in radius for blue-core mode.Regarding the effects of antenna geometry for blue-core mode,it shows that half helix antenna yields the strongest wave field and power absorption,while loop antenna yields the lowest.Moreover,near axis,for antennas with m=+1,the wave field increases with axial distance.In the core region,the wave number approaches to a saturation value at much lower frequency for non-blue-core mode compared to blue-core mode.The total loading resistance is much lower for blue-core mode.These findings are valuable to understanding the physics of blue-core helicon discharge and optimizing the experimental performance of blue-core helicon plasma sources for applications such as space propulsion and material treatment.展开更多
Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-elec...Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.展开更多
Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challeng...Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods.In this study,we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al_(2)O_(3) hydrogenation catalysts through crystallization separation and coprecipitation.Furthermore,the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts.Their properties were thoroughly analyzed and investigated using various characterization techniques.The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents.Finally,the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil,specifically focusing on denitrogenation and aromatic saturation.This work not only offers an effective solution for recycling catalysts but also promotes sustainable development.展开更多
The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results s...The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results show that plasma exists inside the cavity when the sheath inside the hollow electrode hole is fully collapsed, which is an essential condition for the plasma density enhancement outside hollow electrodes. In addition, the existence of the electron density peak at the orifice is generated via the hollow cathode effect(HCE), which plays an important role in the density enhancement. It is also found that the radial width of bulk plasma at the orifice affects the magnitude of the density enhancement, and narrow radial plasma bulk width at the orifice is not beneficial to obtain high-density plasma outside hollow electrodes.Higher electron density at the orifice, combined with larger radial plasma bulk width at the orifice,causes higher electron density outside hollow electrodes. The results also imply that the HCE strength inside the cavity cannot be determined by the magnitude of the electron density outside hollow electrodes.展开更多
Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic applications.Significant progress has been made to design DACs electrocatalysts with various geometri-cal configurations,...Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic applications.Significant progress has been made to design DACs electrocatalysts with various geometri-cal configurations,but in-depth understanding the relationship between geometrical configurations and metal-metal interaction mechanisms for designing targeted DACs is still required.In this review,the recent progress in engineering of geometrical configurations of DACs is systematically summarized.Based on the polarity of geometrical configuration,DACs can be classified into two different types that are homonuclear and heteronuclear DACs.Furthermore,with regard to the geometrical configurations of the active sites,homonuclear DACs are identified into adjacent and bridged configurations,and heteronuclear DACs can be classified into adjacent,bridged,and separated configurations.Subsequently,metal-metal interactions in DACs with different geometrical configurations are introduced.Additionally,the applications of DACs in different electrocatalytic reactions are discussed,including the oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER),and other catalysis.Finally,the future challenges and perspectives for advancements in DACs are high-lighted.This review aims to provide inspiration for the design of highly effcient DACs towards energy relatedapplications.展开更多
Carbon-based metal-free nanomaterials are promising alternatives to precious metals as electrocatalysts of key energy storage and conversion technologies.Of paramount significance are the establishment of design princi...Carbon-based metal-free nanomaterials are promising alternatives to precious metals as electrocatalysts of key energy storage and conversion technologies.Of paramount significance are the establishment of design principles by understanding the catalytic mechanisms and identifying the active sites.Distinct from sp2-conjugated graphene and carbon nanotube,fullerene possesses unique characteristics that are growingly being discovered and exploited by the electrocatalysis community.For instance,the well-defined atomic and molecular structures,the good electron affinity to tune the electronic structures of other substances,the intermolecular self-assembly into superlattices,and the on-demand chemical modification have endowed fullerene with incomparable advantages as electrocatalysts that are otherwise not applicable to other carbon ma-terials.As increasing studies are being reported on this intriguing topic,it is necessary to provide a state-of-the-art overview of the recent progress.This review takes such an initiative by summarizing the promises and challenges in the electrocatalytic applications of fullerene and its derivatives.The content is structured according to the composition and structure of fullerene,including intact fullerene(e.g.,fullerene composite and superlattices)and fullerene derivatives(e.g.,doped,endohedral,and disintegrated fullerene).The synthesis,characterization,catalytic mechanisms,and deficiencies of these fullerene-based materials are explicitly elaborated.We conclude it by sharing our perspectives on the key aspects that future efforts shall consider.展开更多
Background:Androgenic alopecia(AGA)is the most common type of hair loss in men,and there are many studies on the treatment of hair loss by platelet-rich plasma(PRP).The human scalp contains a huge microbiome,but its r...Background:Androgenic alopecia(AGA)is the most common type of hair loss in men,and there are many studies on the treatment of hair loss by platelet-rich plasma(PRP).The human scalp contains a huge microbiome,but its role in the process of hair loss remains unclear,and the relationship between PRP and the microbiome needs further study.Therefore,the purpose of this study was to investigate the effect of PRP treatment on scalp microbiota composition.Methods:We performed PRP treatment on 14 patients with AGA,observed their clinical efficacy,and collected scalp swab samples before and after treatment.The scalp microflora of AGA patients before and after treatment was characterized by amplifying the V3-V4 region of the 16 s RNA gene and sequencing for bacterial identification.Results:The results showed that PRP was effective in the treatment of AGA patients,and the hair growth increased significantly.The results of relative abundance analysis of microbiota showed that after treatment,g_Cutibacterium increased and g_Staphylococcus decreased,which played a stable role in scalp microbiota.In addition,g_Lawsonella decreased,indicating that the scalp oil production decreased after treatment.Conclusions:The findings suggest that PRP may play a role in treating AGA through scalp microbiome rebalancing.展开更多
基金the National Natural Science Foundation of China (21902017)the Foundation of technological innovation and application development of Chongqing (cstc2021jscxmsxm X0308, CSTB2022BSXM-JCX0132)+1 种基金the Youth project of science and technology research program of Chongqing Education Commission of China (KJQN20211107)the Scientific Research Foundation of Chongqing University of Technology (2020ZDZ022, 2021PYZ13)。
文摘Cu-based materials are ideal catalysts for CO_(2) electrocatalytic reduction reaction(CO_(2)RR) into multicarbon products.However,such reactions require stringent conditions on local environments of catalyst surfaces,which currently are the global pressing challenges.Here,a stabilized activation of Cu^(0)/Cu^(+)-onAg interface by N_(2) cold plasma treatment was developed for improving Faradaic efficiency(FE) of CO_(2)RR into C2 products.The resultant Ag@Cu-CuN_x exhibits a C2 FE of 72% with a partial current density of-14.9 mA cm^(-2) at-1.0 V vs.RHE(reversible hydrogen electrode).Combining density functional theory(DFT) and experimental investigations,we unveiled that Cu^(0)/Cu^(+) species can be co ntrollably tu ned by the incorporation of nitrogen to form CuN_x on Ag surface,i.e.,Ag@Cu-CuN_x.This strategy enhances ^(*)CO intermediates generation and accelerates C-C coupling both thermodynamically and kinetically.The intermediates O^(*)C^(*)CO,^(*)COOH,and ^(*)CO were detected by in-situ attenuated total internal reflection surface enhanced infrared absorption spectroscopy(ATR-SEIRAS).The uncovered CO_(2)RR-into-C2 products were carried out along CO_(2)→^(*)COOH→^(*)CO→O^(*)C^(*)CO→^(*)C_(2)H_(3)O→^(*)C_(2)H_(4)O→ C_(2)H_(5)OH(or ^(*)C_(2)H_(3)O→^(*)O+C_(2)H_(4)) paths over Ag@Cu-CuN_x electrocatalyst.This work provides a new approach to design Cu-based electrocatalysts with high-efficiency,mild condition,and stable CO_(2)RR to C2 products.
基金supported by the National Key Research and Development Program of China(No.2018YFC1903100)Beijing Municipal Science and Technology Project Program(No.Z191100009119002)the State Environmental Protection Key Laboratory of Odor Pollution Control(No.20210504)。
文摘Non-thermal plasma(NTP)is considered to be a promising technology for the removal of volatile organic compounds;however,its application is limited by low CO_(2) selectivity and undesirable by-products.To overcome these issues,this paper discusses the degradation of chlorobenzene(CB)in systems of NTP coupled with catalysts,and the influence of catalyst locations in the NTP was investigated.In addition,the interaction between plasma and catalyst was also explored.The results indicated that the degradability of CB was remarkably improved through the combination of NTP with catalysts,and the formation of ozone was effectively inhibited.The degradation efficiency increased from 33.9%to 79.6%at 14 kV in the NTPcatalytic system,while the ozone concentration decreased from 437 to 237 mg m^(-3),and the degradation efficiency of in plasma catalysis(IPC)systems was superior to that of the post plasma catalysis system,while the inhibition ability of ozone exhibited an opposing trend.In the IPC system,the degradation efficiency was 87.7%at 14 k V,while the ozone concentration was151 mg m^(-3).Besides,the plasma did not destroy the pore structure and crystal structure of the catalyst,but affected the surface morphology and redox performance of the catalyst.Thus,NTP coupled catalytic system could improve the degradation performance of CB.Furthermore,the plasma discharge characteristics played a major role in the NTP synergistic catalytic degradation of CB.Finally,based on the experiment analysis results,the general reaction mechanism of CB degradation in an IPC reaction system was proposed.
基金the National Natural Science Foundation of China(21902017)the Project of Fundamental Research and Frontier Exploration of Chongqing(cstc2019jcyj-msxmX0052)+5 种基金the Foundation of Technological Innovation and Application Development of Chongqing(cstc2021jscx-msxmX0308)the Key Projects of Technology Innovation and Application Development of Chongqing(cstc2019jscx-gksbX0022)the Banan Science and Technology Foundation of Chongqing(2018TJ03,2020QC374)the Major Project of Science and Technology Research Program of Chongqing Education Commission of China(KJZD-M202101101)the Youth Project of Science and Technology Research Program of Chongqing Education Commission of China(KJQN20211107)the Scientific Research Foundation of Chongqing University of Technology(2020ZDZ022)。
文摘Electrocatalytic CO_(2)reduction reaction to low-carbon alcohol is a challenging task,especially high selectivity for ethanol,which is mainly limited by the regulation of reaction intermediates and subsequent C–C coupling.A Cu-Co bimetallic catalyst with CN vacancies is successfully developed by H_(2)cold plasma toward a high-efficiency CO_(2)RR into low-carbon alcohol.The Cu-Co PBA-V_(CN)(Prussian blue analogues with CN vacancies)electrocatalyst yields methanol and ethanol as major products with a total low-carbon alcohol FE of 83.8%(methanol:39.2%,ethanol:44.6%)at-0.9 V vs.RHE,excellent durability(100 h)and a small onset potential of-0.21 V.ATR-SEIRAS(attenuated total internal reflection surface enhanced infrared absorption spectroscopy)and DFT(density functional theory)reveal that the steric hindrance of V_(CN)can enhance the CO generation from*COOH,and the C–C coupling can also be increased by CO spillover on uniformly dispersed Cu atoms.This work provides a strategy for the design and preparation of electrocatalysts for CO_(2)RR into low-carbon alcohol products and highlights the impact of catalyst steric hindrance to catalytic performance.
基金financial support from National Natural Science Foundation of China(Nos.52004102 and 22078125)Postdoctoral Science Foundation of China(No.2021M690068)+2 种基金Fundamental Research Funds for the Central Universities(Nos.JUSRP221018 and JUSRP622038)Key Laboratory of Green Cleaning Technology and Detergent of Zhejiang Province(No.Q202204)Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(No.GCP202112)。
文摘In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.
基金supported by the National Natural Science Foundation of China (No.21776156).
文摘High activity and productivity of MoVNbTeO_(x) catalyst are challenging tasks in oxidative dehydrogenation of ethane(ODHE)for industrial application.In this work,phase-pure M1 with 30 wt%CeO_(2) composite catalyst was treated by oxygen plasma to further enhance catalyst performance.The results show that the oxygen vacancies generated by the solid-state redox reaction between M1 and CeO_(2) capture active oxygen species in gas and transform V^(4+)to V^(5+)without damage to M1 structure.The space-time yield of ethylene of the plasma-treated catalyst was significantly increased,in which the catalyst shows an enhancement near~100% than that of phase-pure M1 at 400℃ for ODHE process.Plasma treatment for catalysts demonstrates an effective way to convert electrical energy into chemical energy in catalyst materials.Energy conversion is achieved by using the catalyst as a medium.
基金supported by the Fundamental Research Funds for the Central Universities of China(DUT20-LAB307)the Supercomputing Center of Dalian University of Technology。
文摘Efficient,stable and economical catalysts play a crucial role in enhancing the kinetics of slow oxygen reduction reactions(ORR)in Aluminum-air batteries.Among the potential next-generation candidates,Ag catalysts are promising due to their high activity and low cost,but weaker oxygen adsorption has hindered industrialization.To address this bottleneck,Ag-alloying has emerged as a principal strategy.In this work,we successfully prepared Ag-Cu nanoparticles(NPs)with a rich eutectic phase and uniform dispersion structure using plasma evaporation.The increased solid solution of Ag and Cu led to changes in the electronic structure,resulting in an upward shift of the d-band center,which significantly improved oxygen adsorption.The combination of Ag and Cu in the NPs synergistically enhanced the adsorption of Ag and the desorption of Cu.Density functional theory(DFT)calculations revealed that Ag-Cu25 NPs exhibited the smallest limiting reaction barrier,leading to increased ORR activity.To further optimize the catalyst’s performance,we utilized N-doped porous nanocarbon(N-PC)with high electrical conductivity and abundant mesoporous channels as the support for the Ag-Cu NPs.The N-PC support provided optimal mass transfer carriers for the highly active Ag-Cu25 NPs.As a result,the Ag-Cu25/NPC catalyst displayed excellent ORR activity in alkaline media,with a half-wave potential(E_(1/2))of 0.82 V.Furthermore,the Al-air battery incorporating the Ag-Cu25/NPC catalyst exhibited outstanding electrochemical performance.It demonstrated high open-circuit voltages of 1.89 V and remarkable power densities of 193 m W cm^(-2).The battery also sustained a high current output and maintained a stable high voltage for 120 hours under mechanical charging,showcasing its significant potential for practical applications.
基金National Natural Science Foundation of China(Nos.51977024 and 21577011).
文摘A study of the behaviors of air discharge plasma inside a catalyst’s pores is important to understand the plasma catalysis mechanism;however,few articles have reported the generation characteristics of air plasma in the pores of catalysts.The production of air microdischarge in a pore was studied by a two-dimensional fluid model,mainly focusing on the effect of pore size and applied voltage.The results show that an increase in the pore size in the range of 20–100μm facilitates the occurrence of microdischarge in the pore.In addition,at an applied voltage of 9 kV,the ionization of air mainly occurs near the topside of the pore when the pore diameter is less than 20μm,leading to a low plasma density in the pore,but the time-averaged plasma density in the pore reaches a maximum value at a 70μm pore diameter.Moreover,the applied voltage also has an important effect on the production of air microdischarge in the pore.The existence of a pore of 80μm diameter on the dielectric has no obvious influence on the plasma density in the pore at 2 kV applied voltage,but the plasma density in the pore begins to sharply rise when the voltage exceeds 3 kV due to the enhanced air ionization at higher applied voltage.The study indicates that microdischarge can be generated in a pore with a size of tens of micrometers,and the microdischarge in porous catalysts will affect the catalytic degradation efficacy of gaseous pollutants.
基金supported by the FWO-SBO project PlasMaCatDESIGN (FWO grant ID S001619N)the FWO fellowship of R. Michiels (FWO grant ID 1114921N)+2 种基金the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 810182 – SCOPE ERC Synergy project)funded by the Research Foundation - Flanders (FWO)the Flemish Government。
文摘Plasma-catalytic dry reforming of CH_(4)(DRM) is promising to convert the greenhouse gasses CH_(4) and CO_(2) into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products,because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex,as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, high-lighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems.Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures,at which vibrational excitation can enhance the surface reactions.
基金National Natural Science Foundation of China(Nos.52041001,21808024)Natural Science Foundation of Liaoning Province(No.2020-MS-126)Special Foundation for Key Fields of Colleges and Universities in Guangdong Province(No.2021ZDZX4094)。
文摘Efficient sterilization by a plasma photocatalytic system(PPS)requires strong synergy between plasma and photocatalyst to inactivate microorganisms while suppressing the formation of secondary pollutants.Here,we report that a PPS constructed from a needle array corona discharge and Au/TiO2plasmonic nanocatalyst could remarkably improve the sterilization of Escherichia coli(E.coli)and alleviate formation of the discharge pollutant O3.At 6 kV,the combination of corona discharge and Au/TiO2achieves sterilization efficiency of 100%within an exposure time of 5 min.At 5 kV and an exposure time of 8 min,the presence of Au/TiO2improves sterilization efficiency of the corona discharge from 73%to 91%and reduces the O3concentration from 0.38 to 0.04 ppm,whereas the presence of TiO2reduces the sterilization efficiency and O3concentration to 66%and 0.17 ppm,respectively.The Au/TiO2in the PPS enables a uniform corona discharge,enhances the interaction between plasma,E.coli and nanocatalysts,and suppresses the formation of O3.Further,the Au/TiO2can be excited by ultraviolet-visible light emitted from the plasma to generate electron-hole pairs,and thus contributes to the formation of reactive radicals and the oxidative inactivation of E.coli.The PPS constructed from a needle array corona discharge and Au-based plasmonic nanocatalyst provides a promising approach for developing high-efficiency sterilization techniques.
基金supported by Bhabha Atomic Research Centre, Department of Atomic Energy, Government of IndiaDepartment of Atomic Energy, Government of India for financial assistance under DAE Doctoral Fellowship Scheme-2018。
文摘Coaxial plasma guns are a type of plasma source that produces plasma which propagates radially and axially controlled by the shape of the ground electrode, which has attracted much interest in several applications. In this work, a 120° opening angle of CPG nozzle is used as a plasma gun configuration that operates at the energy of 150 J. The ionization of polyethylene insulator between the electrodes of the gun produces a cloud of hydrogen and carbon plasma.The triple Langmuir probe and Faraday cup are used to measure plasma density and plasma temperature. These methods are used to measure the on-axis and off-axis plasma divergence of the coaxial plasma gun. The peak values of ion densities measured at a distance of 25 mm on-axis from the plasma gun are(1.6±0.5)×10^(19)m^(-3)and(2.8±0.6)×10^(19)m^(-3)for hydrogen and carbon plasma respectively and the peak temperature is 3.02±0.5 eV. The mean propagation velocity of plasma is calculated using the transit times of plasma at different distances from the plasma gun and is found to be 4.54±0.25 cm/μs and 1.81±0.18 cm/μs for hydrogen and carbon plasma respectively. The Debye radius is obtained from the measured experimental data that satisfies the thin sheath approximation. The shot-to-shot stability of plasma parameters facilitates the use of plasma guns in laboratory experiments. These types of plasma sources can be used in many applications like plasma opening switches, plasma devices, and as plasma sources.
文摘In astrophysics, the boundary conditions for plasma phenomena are provided by nature and the astronomer faces the problem of understanding them from a variety of observations [Hester J J et al 1996 Astrophys. J. 456 225], on the other hand, in laboratory plasma experiments the electromagnetic boundary conditions become a major problem in the set-up of the machine that produces the plasma, an issue that has to be investigated step by step and to be modified and adapted with great patience, in particular in the case of an innovative plasma confinement experiment. The PROTO-SPHERA machine [Alladio F et al 2006 Nucl. Fusion 46 S613] is a magnetic confinement experiment, that emulates in the laboratory the jet + torus plasma configurations often observed in astrophysics: an inner magnetized jet of plasma centered on the(approximate) axis of symmetry and surrounded by a magnetized plasma torus orthogonal to this jet. The PROTO-SPHERA plasma is simply connected, i.e., no metal current conducting rod is linked to the plasma torus, while instead it is the inner magnetized plasma jet(in the following always called the plasma centerpost) that is linked to the torus. It is mandatory that no spurious plasma current path modifies the optimal shape of the plasma centerpost. Moreover, as the plasma torus is produced and sustained, in absence of any applied inductive electric field, by the inner plasma centerpost through magnetic reconnections [Taylor J B and Turner M F 1989 Nucl.Fusion 29 219], it is required as well that spurious current paths do not surround the torus on its outboard, in order not to lower the efficiency of the magnetic reconnections that maintain the plasma torus at the expense of the plasma centerpost. Boundary conditions have been corrected,up to the point that the first sustainment in steady state has been achieved for the combined plasma.
基金supported by Department of Science and Technology of Jilin Province of China(Nos.YDZJ202301 ZYTS481,202202901032GX,and 20230402068GH)。
文摘Only a small amount of spectral information is collected because the collection solid angle of the optical fiber probe and lens is very limited when collecting spectral information.To overcome this limitation,this study presents a novel method for acquiring plasma spectral information from various spatial directions.A parabolic-shaped plasma spectral collection device(PSCD)is employed to effectively collect more spectral information into the spectrometer,thereby enhancing the overall spectral intensity.The research objects in this study were soil samples containing different concentrations of heavy metals Pb,Cr,and Cd.The results indicate that the PSCD significantly enhances the spectral signal,with an enhancement rate of up to 45%.Moreover,the signal-to-noise ratio also increases by as much as 36%.Simultaneously,when compared to the absence of a device,it is found that there is no significant variation in plasma temperature when the PSCD is utilized.This observation eliminates the impact of the spatial effect caused by the PSCD on the spectral intensity.Consequently,a concentrationspectral intensity relationship curve is established under the PSCD.The results revealed that the linear fitting R^(2)for Pb,Cr,and Cd increased by 0.011,0.001,and 0.054,respectively.Additionally,the limit of detection(LOD)decreased by 0.361 ppm,0.901 ppm,and 0.602 ppm,respectively.These findings indicate that the spectral enhancement rate elevates with the increase in heavy metal concentration.Hence,the PSCD can effectively enhance the spectral intensity and reduce the detection limit of heavy metals in soil.
基金Project supported by the National Natural Science Foundation of China(Grant No.92271113)the Fundamental Research Funds for the Central Universities(Grant No.2022CDJQY-003)+1 种基金Chongqing Entrepreneurship and Innovation Support Program for Overseas Returnees(Grant No.CX2022004)the Fund from Shanghai Engineering Research Center of Space Engine(Grant No.17DZ2280800).
文摘This paper deals with wave propagation and power coupling in blue-core helicon plasma driven by various antennas and frequencies.It is found that compared to non-blue-core mode,for blue-core mode,the wave can propagate in the core region,and it decays sharply outside the core.The power absorption is lower and steeper in radius for blue-core mode.Regarding the effects of antenna geometry for blue-core mode,it shows that half helix antenna yields the strongest wave field and power absorption,while loop antenna yields the lowest.Moreover,near axis,for antennas with m=+1,the wave field increases with axial distance.In the core region,the wave number approaches to a saturation value at much lower frequency for non-blue-core mode compared to blue-core mode.The total loading resistance is much lower for blue-core mode.These findings are valuable to understanding the physics of blue-core helicon discharge and optimizing the experimental performance of blue-core helicon plasma sources for applications such as space propulsion and material treatment.
基金supported by the National Natural Science Foundation of China(52272194)Liaoning Revitalization Talents Program(XLYC2007155)。
文摘Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.
基金supported by grants from the National Key Research and Development Program of China(2023YE41507601)the National Natural Science Foundation of China(22122807,22378038)+1 种基金the Fundamental Research Funds for the Central Universities(DUT23RC(3)044)State Key Laboratory of Heavy Oil Processing,China University of Petroleum(WX20230149)。
文摘Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods.In this study,we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al_(2)O_(3) hydrogenation catalysts through crystallization separation and coprecipitation.Furthermore,the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts.Their properties were thoroughly analyzed and investigated using various characterization techniques.The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents.Finally,the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil,specifically focusing on denitrogenation and aromatic saturation.This work not only offers an effective solution for recycling catalysts but also promotes sustainable development.
文摘The plasma density enhancement outside hollow electrodes in capacitively coupled radio-frequency(RF) discharges is investigated by a two-dimensional(2D) particle-in-cell/Monte-Carlo collision(PIC/MCC) model. Results show that plasma exists inside the cavity when the sheath inside the hollow electrode hole is fully collapsed, which is an essential condition for the plasma density enhancement outside hollow electrodes. In addition, the existence of the electron density peak at the orifice is generated via the hollow cathode effect(HCE), which plays an important role in the density enhancement. It is also found that the radial width of bulk plasma at the orifice affects the magnitude of the density enhancement, and narrow radial plasma bulk width at the orifice is not beneficial to obtain high-density plasma outside hollow electrodes.Higher electron density at the orifice, combined with larger radial plasma bulk width at the orifice,causes higher electron density outside hollow electrodes. The results also imply that the HCE strength inside the cavity cannot be determined by the magnitude of the electron density outside hollow electrodes.
基金supported by the Natural Science Foundation of China (22179062,52125202,and U2004209)the Natural Science Foundation of Jiangsu Province (BK20230035)+1 种基金the Fundamental Research Funds for the Central Universities (30922010303)the Intergovernmental Cooperation Projects in the National Key Research and Development Plan of the Ministry of Science and Technology of PRC (2022YFE0196800)
文摘Geometrical configurations play a crucial role in dual-atom catalysts(DACs)for electrocatalytic applications.Significant progress has been made to design DACs electrocatalysts with various geometri-cal configurations,but in-depth understanding the relationship between geometrical configurations and metal-metal interaction mechanisms for designing targeted DACs is still required.In this review,the recent progress in engineering of geometrical configurations of DACs is systematically summarized.Based on the polarity of geometrical configuration,DACs can be classified into two different types that are homonuclear and heteronuclear DACs.Furthermore,with regard to the geometrical configurations of the active sites,homonuclear DACs are identified into adjacent and bridged configurations,and heteronuclear DACs can be classified into adjacent,bridged,and separated configurations.Subsequently,metal-metal interactions in DACs with different geometrical configurations are introduced.Additionally,the applications of DACs in different electrocatalytic reactions are discussed,including the oxygen reduction reaction(ORR),oxygen evolution reaction(OER),hydrogen evolution reaction(HER),and other catalysis.Finally,the future challenges and perspectives for advancements in DACs are high-lighted.This review aims to provide inspiration for the design of highly effcient DACs towards energy relatedapplications.
基金This study is supported by the National Natural Science Foundation of China(21925104)the Natural Science Foun-dation of Hubei Province(2021CFA020)the start-up funding of Huazhong University of Science and Technology(3004110178).
文摘Carbon-based metal-free nanomaterials are promising alternatives to precious metals as electrocatalysts of key energy storage and conversion technologies.Of paramount significance are the establishment of design principles by understanding the catalytic mechanisms and identifying the active sites.Distinct from sp2-conjugated graphene and carbon nanotube,fullerene possesses unique characteristics that are growingly being discovered and exploited by the electrocatalysis community.For instance,the well-defined atomic and molecular structures,the good electron affinity to tune the electronic structures of other substances,the intermolecular self-assembly into superlattices,and the on-demand chemical modification have endowed fullerene with incomparable advantages as electrocatalysts that are otherwise not applicable to other carbon ma-terials.As increasing studies are being reported on this intriguing topic,it is necessary to provide a state-of-the-art overview of the recent progress.This review takes such an initiative by summarizing the promises and challenges in the electrocatalytic applications of fullerene and its derivatives.The content is structured according to the composition and structure of fullerene,including intact fullerene(e.g.,fullerene composite and superlattices)and fullerene derivatives(e.g.,doped,endohedral,and disintegrated fullerene).The synthesis,characterization,catalytic mechanisms,and deficiencies of these fullerene-based materials are explicitly elaborated.We conclude it by sharing our perspectives on the key aspects that future efforts shall consider.
基金supported by the Guangdong Enterprise Joint Fund(No.2022A1515220137)The Shenzhen Science and Technology Innovation Committee(No.JCYJ20220530141615035)the Internal project of Huazhong University of Science and Technology Union Shenzhen Hospital(Nos.YN2021042 and YN2021045)。
文摘Background:Androgenic alopecia(AGA)is the most common type of hair loss in men,and there are many studies on the treatment of hair loss by platelet-rich plasma(PRP).The human scalp contains a huge microbiome,but its role in the process of hair loss remains unclear,and the relationship between PRP and the microbiome needs further study.Therefore,the purpose of this study was to investigate the effect of PRP treatment on scalp microbiota composition.Methods:We performed PRP treatment on 14 patients with AGA,observed their clinical efficacy,and collected scalp swab samples before and after treatment.The scalp microflora of AGA patients before and after treatment was characterized by amplifying the V3-V4 region of the 16 s RNA gene and sequencing for bacterial identification.Results:The results showed that PRP was effective in the treatment of AGA patients,and the hair growth increased significantly.The results of relative abundance analysis of microbiota showed that after treatment,g_Cutibacterium increased and g_Staphylococcus decreased,which played a stable role in scalp microbiota.In addition,g_Lawsonella decreased,indicating that the scalp oil production decreased after treatment.Conclusions:The findings suggest that PRP may play a role in treating AGA through scalp microbiome rebalancing.