Introduction-Nuclei near and beyond the proton drip line represent a fascinating frontier in the nuclear landscape. Proton-rich nuclei exhibit intriguing phenomena, such as the Thomas-Ehrman shift and proton-halo stru...Introduction-Nuclei near and beyond the proton drip line represent a fascinating frontier in the nuclear landscape. Proton-rich nuclei exhibit intriguing phenomena, such as the Thomas-Ehrman shift and proton-halo structure. Beyond the proton dripline, nuclei become unbound, allowing protons to be emitted and giving rise to novel radioactive decay modes. Single-proton radioactivity, a process in which some nuclei with an odd number of protons(Z) decay by ejecting a proton, was discovered several decades ago and has been extensively studied [1, 2].展开更多
This work presents a systematic analysis of proton-induced total ionizing dose(TID)effects in 1.2 k V silicon carbide(SiC)power devices with various edge termination structures.Three edge terminations including ring-a...This work presents a systematic analysis of proton-induced total ionizing dose(TID)effects in 1.2 k V silicon carbide(SiC)power devices with various edge termination structures.Three edge terminations including ring-assisted junction termination extension(RA-JTE),multiple floating zone JTE(MFZ-JTE),and field limiting rings(FLR)were fabricated and irradiated with45 Me V protons at fluences ranging from 1×10^(12) to 1×10^(14) cm^(-2).Experimental results,supported by TCAD simulations,show that the RA-JTE structure maintained stable breakdown performance with less than 1%variation due to its effective electric field redistribution by multiple P+rings.In contrast,MFZ-JTE and FLR exhibit breakdown voltage shifts of 6.1%and 15.2%,respectively,under the highest fluence.These results demonstrate the superior radiation tolerance of the RA-JTE structure under TID conditions and provide practical design guidance for radiation-hardened Si C power devices in space and other highradiation environments.展开更多
Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy convers...Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy conversion efficiency.In certain application scenarios,the use of N_(2)O(a potent greenhouse gas),as an alternative oxidant to air,presents a feasible strategy.Herein,we report for the first time the operation of PCFCs employing N_(2)O as the oxidant.A hybrid Pr_(2)Ni_(0.6)Co_(0.4)O_(4-δ)(PNCO-214)catalyst is developed,comprising Ruddlesden-Popper(R-P)structured Pr_(4)Ni_(1.8)Co_(1.2)O_(10-δ)(PNCO-4310)and fluorite structured Pr_(6)O_(11)(PO-611),which synergistically exhibits exceptional catalytic activity toward both N_(2)O decomposition and the oxygen reduction reaction,achieving a conversion over 92% and an area specific resistance of 1.301Ω·cm^(2) at 600℃.Quasi-insitu temperature-dependent Fourier transform infrared(FTIR)and electrochemical impedance spectroscopy analyses reveal that abundant oxygen vacancies in PNCO-214 facilitate rapid adsorption and dissociation of N_(2)O into N_(2) and O_(2),while also promoting the surface exchange kinetics of proton/oxygen during oxygen reduction reaction(ORR).When applied in an anode-supported single cell with PNCO-214 cathode operating under N_(2)O,outstanding power density and low resistance are achieved,delivering 0.801 W·cm^(-2) and 0.245Ω·cm^(2) at 600℃.Satisfactory performance is also maintained even when the temperature is reduced to 500℃.Furthermore,the single cell demonstrates relatively good stability with negligible degradation over 130 h at 600℃ and 0.7 V.These findings underscore the potential of PNCO-214 as a highly effective cathode catalyst for enabling the use of N_(2)O as a viable oxidant in PCFCs for specific industrial applications.展开更多
Understanding the proton dynamic behavior in inorganic materials has long been a topic of intense fascination[1],especially in the field of electrochemical energy storage[2].One of the examples is the research of prot...Understanding the proton dynamic behavior in inorganic materials has long been a topic of intense fascination[1],especially in the field of electrochemical energy storage[2].One of the examples is the research of proton transport in transition metal oxides,which dates back to 1971[3]when RuO_(2) was discovered to be capable of storing protons via reversible redox reactions[4].In aqueous electrolytes,the thin film RuO_(2) electrode exhibits a surface pseudocapacitive behavior[5],which could be modified by the structural water in its hydrated form due to the facile Grotthuss hopping mode of protons along the established hydrogen bonds inside the bulk phase[6].Soon later,Goodenough et al.reported the capacitor-like behavior of amorphous MnO_(2)·xH_(2)O electrode in an aqueous KCl electrolyte[7],and further studies on the hydrated MnO_(2) electrodes prepared by sol-gel processes have soon discovered that the intercalation of protons from aqueous electrolytes plays an indispensable role in the charge storage mechanism[8].In recent years,the research interest on rechargeable aqueous batteries has fueled the renaissance of mechanistic study of proton transport in transition metal oxides[9],which can operate as cathodes or anodes via a topotactic insertion mechanism similar to that in Li-ion batteries[10].However,due to the challenges for experimental detection of local chemical environments of the inserted protons,a comprehensive understanding of proton dynamic behavior in these electrodes remains largely lacking.展开更多
The significance of laser-driven polarized beam acceleration has been increasingly recognized in recent years.We propose an efficient method for generating polarized proton beams from a pre-polarized hydrogen halide g...The significance of laser-driven polarized beam acceleration has been increasingly recognized in recent years.We propose an efficient method for generating polarized proton beams from a pre-polarized hydrogen halide gas jet,utilizing magnetic vortex acceleration enhanced by a laser-driven plasma bubble.When a petawatt laser pulse passes through a pre-polarized gas jet,a bubble-like ultra-nonlinear plasma wave is formed.As a portion of the particles constituting this wave,background protons are swept by the acceleration field of the bubble and oscillate significantly along the laser propagation axis.Some of the pre-accelerated protons in the plasma wave are trapped by the acceleration field at the rear side of the target.This acceleration field is intensified by the transverse expansion of the laser-driven magnetic vortex,resulting in energetic polarized proton beams.The spin of energetic protons is determined by their precession within the electromagnetic field,which is described using the Thomas-Bargmann-Michel-Telegdi equation in analytical models and particle-in-cell simulations.Multidimensional simulations reveal that monoenergetic proton beams with an energy of hundreds of MeV,a beam charge of hundreds of pC,and a beam polarization of tens of percent can be produced at laser powers of several petawatts.Such laser-driven polarized proton beams have promise for application in polarized beam colliders,where they can be utilized to investigate particle interactions and to explore the properties of matter under extreme conditions.展开更多
Proton exchange membrane water electrolysis(PEMWE)technology is widely recognized as a cornerstone for green hydrogen production,offering high operational current densities exceeding 1.0 A cm^(-2),rapid dynamic respon...Proton exchange membrane water electrolysis(PEMWE)technology is widely recognized as a cornerstone for green hydrogen production,offering high operational current densities exceeding 1.0 A cm^(-2),rapid dynamic response capabilities,and zero-carbon emission characteristics[1].However,the sluggish kinetics of oxygen evolution reaction(OER)at the anode presents a critical bottleneck for large-scale commercial deployment(Fig.1(a)).Despite significant advancements through electronic structure modulation[2]and coordination environment optimization[3],the deprotonation energy barrier of oxygen-containing intermediates and the stability of active sites under acidic conditions remain unresolved challenges.展开更多
“Three-in-one”cathode,achieved via B-site heavy-doping of transition elements(typically Co,Fe)into proton-conductive perovskite,holds promise for enhancing the performance of proton-conducting solid oxide fuel cell(...“Three-in-one”cathode,achieved via B-site heavy-doping of transition elements(typically Co,Fe)into proton-conductive perovskite,holds promise for enhancing the performance of proton-conducting solid oxide fuel cell(H-SOFC)operated below 650℃for electricity generation.However,its electrochemical behavior above 650℃,essential for improving the efficiency of H-SOFC for fuel conversion,remains insufficiently explored.It is still challenging to propose guidance for the design of“threein-one”cathode toward optimal H-SOFC performance below and above 650℃,with the prerequisite of gaining a comprehensive understanding of the roles of Co and Fe in determining the H-SOFC performance.This work is to address this challenge.Through theoretical/experimental studies,Co is identified to play a role in improving the oxygen reduction reaction(ORR)activity while Fe plays a role in facilitating the cathode/electrolyte interfacial proton conduction.Therefore,if the operating temperature is above 650℃,lowering the Co/Fe ratio in“three-in-one”cathode becomes crucial since the limiting factor shifts from ORR activity to proton conduction.Implementing this strategy,the SOFC using BaCo_(0.15)-Fe_(0.55)Zr_(0.1)Y_(0.1)Yb_(0.1)O_(3−δ)cathode achieves peak power densities of 1.67Wcm^(−2)under H-SOFC mode at 700℃and 2.32Wcm^(−2)under dual ion-conducting SOFC mode at 750℃,which are the highest reported values so far.展开更多
GaN diodes for high energy(64.8 MeV)proton detection were fabricated and investigated.A comparison of the performance of GaN diodes with different structures is presented,with a focus on sapphire and on GaN substrates...GaN diodes for high energy(64.8 MeV)proton detection were fabricated and investigated.A comparison of the performance of GaN diodes with different structures is presented,with a focus on sapphire and on GaN substrates,Schottky and pin diodes,and different active layer thicknesses.Pin diodes fabricated on a sapphire substrate are the best choice for a GaN proton detector working at 0 V bias.They are sensitive(minimum detectable proton beam<1 pA/cm^(2)),linear as a function of proton current and fast(<1 s).High proton current sensitivity and high spatial resolution of GaN diodes can be exploited in the future for proton imaging of patients in proton therapy.展开更多
We put forward a new design of a compact beam transport system for intense laser-driven proton therapy,where instead of using conventional pulsed solenoids,our design relies on a helical coil irradiated by a nanosecon...We put forward a new design of a compact beam transport system for intense laser-driven proton therapy,where instead of using conventional pulsed solenoids,our design relies on a helical coil irradiated by a nanosecond laser pulse to generate strong magnetic fields for focusing protons.A pair of dipole magnets and apertures are employed to further filter protons with large divergences and low energies.Our numerical studies combine particle-in-cell simulations for laser-plasma interaction to generate high-energy monoenergetic proton beams,finite element analysis for evaluating the magnetic field distribution inside the coil,and MonteCarlo simulations for beam transport and energy deposition.Our results show that with this design,a spread-out Bragg peak in a range of several centimeters to a deep-seated tumor with a dose of approximately 16.5 cGy and fluctuation around 2% can be achieved.The instantaneous dose rate reaches up to 10^(9)Gy/s,holding the potential for future FLASH radiotherapy research.展开更多
The thiol-imidazole functionalized(p-triphenyl-pentafluorobenzaldehyde)polymer(IMPTP)was prepared and quaternized with different side chains to obtain imidazolium-modified Me-IMPTP,He-IMPTP and BIM-IMPTP membranes for...The thiol-imidazole functionalized(p-triphenyl-pentafluorobenzaldehyde)polymer(IMPTP)was prepared and quaternized with different side chains to obtain imidazolium-modified Me-IMPTP,He-IMPTP and BIM-IMPTP membranes for application in high-temperature proton exchange membrane fuel cells(HT-PEMFCs).The presence of the thioether group in the polymers enabled radical scavenging for antioxidant properties,while imidazolium cations interacted strongly with H_(2)PO_(4) to prevent phosphoric acid(PA)leaching.The prepared BIM-IMPTP membrane incorporating bisimidazolium cation string with a long alkyl spacer demonstrated the highest mass retention of 82.93%after being immersed in Fenton's reagent for 24 h.Additionally,the PA-doped BIM-IMPTP membranes exhibited excellent PA retention under high-humidity conditions(80℃/100%RH).The single cell equipped with the BIM-IMPTP/320%PA membrane achieved a maximum power density(PDmax)of 945 mW cm^(-2)at 160℃.Among the four membranes with a similar acid doping content(ADC),the BIM-IMPTP/163%PA membrane with bis-cation pairs in the side chains exhibited a well-developed microphase-separated structure and high proton conductivity(119.0 mS cm^(-1)at 180℃).The single cell assembled with BIM-IMPTP/163%PA membrane maintained a PDmax of 613 mW cm^(-2)at 160℃ and demonstrated long-term operational stability under both 150/400 mA cm^(-2)and 80℃/200 mA cm^(-2)conditions.These results indicate that the introduction of thioether and bis-cation pairs in the structural design of polymers contributes significantly to the long-term stability of HT-PEMs.展开更多
Laser-driven ion acceleration,as produced by interaction of a high-intensity laser with a target,is a growing field of interest.One of the current challenges is to enhance the acceleration process,i.e.,to increase the...Laser-driven ion acceleration,as produced by interaction of a high-intensity laser with a target,is a growing field of interest.One of the current challenges is to enhance the acceleration process,i.e.,to increase the produced ion energy and the ion number and to shape the energy distribution for future applications.In this paper,we investigate the effect of helical coil(HC)targets on the laser-matter interaction process using a 150 TW laser.We demonstrate that HC targets significantly enhance proton acceleration,improving energy bunching and beam focusing and increasing the cutoff energy.For the first time,we extend this analysis to carbon ions,revealing a marked reduction in the number of low-energy carbon ions and the potential for energy bunching and post-acceleration through an optimized HC design.Simulations using the particle-in-cell code SOPHIE confirm the experimental results,providing insights into the current propagation and ion synchronization mechanisms in HCs.Our findings suggest that HC targets can be optimized for multispecies ion acceleration.展开更多
To address the challenge of insufficient oxygen vacancies in proton-conducting solid oxide fuel cells(H-SOFC),transition metal elements were doped into the B site of lanthanum ferrite perovskite(ABO3)to enhance its ca...To address the challenge of insufficient oxygen vacancies in proton-conducting solid oxide fuel cells(H-SOFC),transition metal elements were doped into the B site of lanthanum ferrite perovskite(ABO3)to enhance its catalytic activity further.The Mo-doped La_(0.6)Sr_(0.4)Fe_(0.9)Ni_(0.1)O_(3-δ)(LSFNMx,x=0.05,0.1)powder was synthesized via the sol−gel method,and its crystal structure,conductivity,defect chemistry,and electrochemical performance as an H-SOFC cathode were investigated.The prepared material exhibited a hexagonal structure with the R-3c space group and demonstrates good chemical stability under simulated working conditions.Mo doping increased the surface concentration of oxygen vacancies,leading to the accelerated oxygen transportation.Consequently,the polarization resistance(Rpol)and activation energy(Ea)are reduced.Specifically,LSFNM0.05 showed the lowest polarization resistance(approximately 0.26Ω·cm^(2))at 700°C.LSFNM0.05 achieved a maximum power density of 484 mW/cm^(2)at this temperature,outperforming those of LSFN(353 mW/cm^(2))and LSFNM0.1(365 mW/cm^(2)).展开更多
Protonic solid oxide electrolysis cells(P-SOECs)are a promising technology for water electrolysis to produce green hydrogen.However,there are still challenges related key materials and anode/electrolyte interface.P-SO...Protonic solid oxide electrolysis cells(P-SOECs)are a promising technology for water electrolysis to produce green hydrogen.However,there are still challenges related key materials and anode/electrolyte interface.P-SOECs with Zr-rich electrolyte,called Zr-rich side P-SOECs,possess high thermodynamically stability under high steam concentrations but the large reaction resistances and the current leakage,thus the inferior performances.In this study,an efficient functional interlayer Ba_(0.95)La_(0.05)Fe_(0.8)Zn_(0.2)O_(3-δ)(BLFZ)in-between the anode and the electrolyte is developed.The electrochemical performances of P-SOECs are greatly enhanced because the BLFZ can greatly increase the interface contact,boost anode reaction kinetics,and increase proton injection into electrolyte.As a result,the P-SOEC yields high current density of 0.83 A cm^(-2) at 600℃ in 1.3 Vamong all the reported Zr-rich side cells.This work not only offers an efficient functional interlayer for P-SOECs but also holds the potential to achieve P-SOECs with high performances and long-term stability.展开更多
Proton-conducting materials have attracted considerable interest because of their extensive application in energy storage and conversion devices.Among them,metal-organic frameworks(MOFs)present tremendous development ...Proton-conducting materials have attracted considerable interest because of their extensive application in energy storage and conversion devices.Among them,metal-organic frameworks(MOFs)present tremendous development potential and possibilities for constructing novel advanced proton conductors due to their special advantages in crystallinity,designability,and porosity.In particular,several special design strategies for the structure of MOFs have opened new doors for the advancement of MOF proton conductors,such as charged network construction,ligand functionalization,metal-center manipulation,defective engineering,vip molecule incorporation,and pore-space manipulation.With the implementation of these strategies,proton-conducting MOFs have developed significantly and profoundly within the last decade.Therefore,in this review,we critically discuss and analyze the fundamental principles,design strategies,and implementation methods targeted at improving the proton conductivity of MOFs through representative examples.Besides,the structural features,the proton conduction mechanism and the behavior of MOFs are discussed thoroughly and meticulously.Future endeavors are also proposed to address the challenges of proton-conducting MOFs in practical research.We sincerely expect that this review will bring guidance and inspiration for the design of proton-conducting MOFs and further motivate the research enthusiasm for novel proton-conducting materials.展开更多
Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promisi...Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promising technology for hydrogen production,which is equipped to combine efficiently with intermittent electricity from renewable energy sources.In this review,PEM-based electrocatalytic systems for H2 production are summarized systematically from low to high operating temperature systems.When the operating temperature is below 130℃,the representative device is a PEM water electrolyzer;its core components and respective functions,research status,and design strategies of key materials especially in electrocatalysts are presented and discussed.However,strong acidity,highly oxidative operating conditions,and the sluggish kinetics of the anode reaction of PEM water electrolyzers have limited their further development and shifted our attention to higher operating temperature PEM systems.Increasing the temperature of PEM-based electrocatalytic systems can cause an increase in current density,accelerate reaction kinetics and gas transport and reduce the ohmic value,activation losses,ΔGH*,and power consumption.Moreover,further increasing the operating temperature(120-300℃)of PEM-based devices endows various hydrogen carriers(e.g.,methanol,ethanol,and ammonia)with electrolysis,offering a new opportunity to produce hydrogen using PEM-based electrocatalytic systems.Finally,several future directions and prospects for developing PEM-based electrocatalytic systems for H_(2) production are proposed through devoting more efforts to the key components of devices and reduction of costs.展开更多
The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for...The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for hydrogen production.Despite remarkable advancements in this field,confronting the sluggish electrochemical kinetics and inherent high-energy consumption arising from deteriorated mass transport within PEMWE systems remains a formidable obstacle.This impediment stems primarily from the hindered protons mass transfer and the untimely hydrogen bubbles detachment.To address these challenges,we harness the inherent variability of electrical energy and introduce an innovative pulsed dynamic water electrolysis system.Compared to constant voltage electrolysis(hydrogen production rate:51.6 m L h^(-1),energy consumption:5.37 kWh Nm-^(3)H_(2)),this strategy(hydrogen production rate:66 m L h^(-1),energy consumption:3.83 kWh Nm-^(3)H_(2))increases the hydrogen production rate by approximately 27%and reduces the energy consumption by about 28%.Furthermore,we demonstrate the practicality of this system by integrating it with an off-grid photovoltaic(PV)system designed for outdoor operation,successfully driving a hydrogen production current of up to 500 mA under an average voltage of approximately 2 V.The combined results of in-situ characterization and finite element analysis reveal the performance enhancement mechanism:pulsed dynamic electrolysis(PDE)dramatically accelerates the enrichment of protons at the electrode/solution interface and facilitates the release of bubbles on the electrode surface.As such,PDE-enhanced PEMWE represents a synergistic advancement,concurrently enhancing both the hydrogen generation reaction and associated transport processes.This promising technology not only redefines the landscape of electrolysis-based hydrogen production but also holds immense potential for broadening its application across a diverse spectrum of electrocatalytic endeavors.展开更多
To develop proton-conducting materials with high hydrothermal and acid-base stability and to elucidate the proton-transport mechanism through visualized structural analysis,two new lanthanum phosphite-oxalates with 3D...To develop proton-conducting materials with high hydrothermal and acid-base stability and to elucidate the proton-transport mechanism through visualized structural analysis,two new lanthanum phosphite-oxalates with 3D frameworks,designated as[La(HPO_(3))(C_(2)O_(4))0.5(H_(2)O)_(2)](La‑1)and(C_(6)H_(16)N_(2))(H_(3)O)[La_(2)(H_(2)PO_(3))_(3)(C_(2)O_(4))_(3)(H_(2)O)](La‑2)(C_(6)H_(14)N_(2)=cis-2,6-dimethylpiperazine),were prepared by hydrothermal and solvothermal conduction,respectively.La‑1 was constructed with lanthanum phosphite 2D layers and C_(2)O_(4)^(2-)groups,whereas La‑2 was constructed with lanthanum oxalate 2D layers and H_(2)PO^(3-)groups.Alternating current(AC)impedance spectra indicate that the pro-ton conductivities of both compounds could reach 10^(-4)S·cm^(-1)and remain highly durable at 75℃and 98%of rela-tive humidity(RH).Due to the abundance of H-bonds in La‑2,theσof La‑2 was higher than that of La‑1.La‑1 exhibited excellent water and pH stability.CCDC:2439965,La‑1;443776,La‑2.展开更多
BACKGROUND Proton pump inhibitors(PPIs)are widely used,including among cancer patients,to manage gastroesophageal reflux and other gastric acid-related disorders.Recent evidence suggests associations between long-term...BACKGROUND Proton pump inhibitors(PPIs)are widely used,including among cancer patients,to manage gastroesophageal reflux and other gastric acid-related disorders.Recent evidence suggests associations between long-term PPI use and higher risks for various adverse health outcomes,including greater mortality.AIM To investigate the association between PPI use and all-cause mortality among cancer patients by a comprehensive analysis after adjustment for various confounders and a robust methodological approach to minimize bias.METHODS This retrospective cohort study used data from the TriNetX research network,with electronic health records from multiple healthcare organizations.The study employed a new-user,active comparator design,which compared newly treated PPI users with non-users and newly treated histamine2 receptor antagonists(H2RA)users among adult cancer patients.Newly prescribed PPIs(esomeprazole,lansoprazole,omeprazole,pantoprazole,or rabeprazole)users were compared to non-users or newly prescribed H2RAs(cimetidine,famotidine,nizatidine,or ranitidine)users.The primary outcome was all-cause mortality.Each patient in the main group was matched to a patient in the control group using 1:1 propensity score matching to reduce confounding effects.Multivariable Cox regression models were used to estimate hazard ratios(HRs)and 95% confidence interval(CI).RESULTS During the follow-up period(median 5.4±1.8 years for PPI users and 6.5±1.0 years for non-users),PPI users demonstrated a higher all-cause mortality rate than non-users after 1 year,2 years,and at the end of follow up(HRs:2.34-2.72).Compared with H2RA users,PPI users demonstrated a higher rate of all-cause mortality HR:1.51(95%CI:1.41-1.69).Similar results were observed across sensitivity analyses by excluding deaths from the first 9 months and 1-year post-exposure,confirming the robustness of these findings.In a sensitivity analysis,we analyzed all-cause mortality outcomes between former PPI users and individuals who have never used PPIs,providing insights into the long-term effects of past PPI use.In addition,at 1-year follow-up,the analysis revealed a significant difference in mortality rates between former PPI users and non-users(HR:1.84;95%CI:1.82-1.96).CONCLUSION PPI use among cancer patients was associated with a higher risk of all-cause mortality compared to non-users or H2RA users.These findings emphasize the need for cautious use of PPIs in cancer patients and suggest that alternative treatments should be considered when clinically feasible.However,further studies are needed to corroborate our findings,given the significant adverse outcomes in cancer patients.展开更多
On the surfaces of celestial bodies with no or thin atmospheres,such as the Moon and Mars,the solar wind irradiation process leads to the formation of hydrogen and helium enriched regions in the extraterrestrial soil ...On the surfaces of celestial bodies with no or thin atmospheres,such as the Moon and Mars,the solar wind irradiation process leads to the formation of hydrogen and helium enriched regions in the extraterrestrial soil particles.However,soil particles on the Earth with the similar composition lack such structures and properties.This discrepancy raises a key question whether there is a direct relationship between solar wind irradiation and the alterations in the structure and chemical performance of extraterrestrial materials.To address this question,this work investigates the effects of proton irradiation,simulating solar wind radiation,on the structure and photothermal catalytic properties of the classic catalyst In_(2)O_(3).It reveals that proton irradiation induces structural features in In_(2)O_(3) analogous to those characteristics of solar wind weathering observed in extraterrestrial materials.Furthermore,after proton beam irradiation with an energy of 30 keV and a dose of 3×10^(17) protons·cm^(-2),the methanol production yield of the In_(2)O_(3) catalyst increased to 2.6 times of its preirradiation level,and the methanol selectivity improved to 2.1 times of the original value.This work provides both theoretical and experimental support for the development of high-efficiency,radiation-resistant photothermal catalysts.展开更多
The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled elec...The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.展开更多
文摘Introduction-Nuclei near and beyond the proton drip line represent a fascinating frontier in the nuclear landscape. Proton-rich nuclei exhibit intriguing phenomena, such as the Thomas-Ehrman shift and proton-halo structure. Beyond the proton dripline, nuclei become unbound, allowing protons to be emitted and giving rise to novel radioactive decay modes. Single-proton radioactivity, a process in which some nuclei with an odd number of protons(Z) decay by ejecting a proton, was discovered several decades ago and has been extensively studied [1, 2].
基金supported by the IITP(Institute for Information&Communications Technology Planning&Evaluation)under the ITRC(Information Technology Research Center)support program(IITP-2025-RS-2024-00438288)grant funded by the Korea government(MSIT)+1 种基金National Research Council of Science&Technology(NST)grant by the MSIT(Aerospace Semiconductor Strategy Research Project No.GTL25051-000)supported by the IC Design Education Center(IDEC),Korea。
文摘This work presents a systematic analysis of proton-induced total ionizing dose(TID)effects in 1.2 k V silicon carbide(SiC)power devices with various edge termination structures.Three edge terminations including ring-assisted junction termination extension(RA-JTE),multiple floating zone JTE(MFZ-JTE),and field limiting rings(FLR)were fabricated and irradiated with45 Me V protons at fluences ranging from 1×10^(12) to 1×10^(14) cm^(-2).Experimental results,supported by TCAD simulations,show that the RA-JTE structure maintained stable breakdown performance with less than 1%variation due to its effective electric field redistribution by multiple P+rings.In contrast,MFZ-JTE and FLR exhibit breakdown voltage shifts of 6.1%and 15.2%,respectively,under the highest fluence.These results demonstrate the superior radiation tolerance of the RA-JTE structure under TID conditions and provide practical design guidance for radiation-hardened Si C power devices in space and other highradiation environments.
基金financially supported by the National Key R&D Program of China(No.2024YFF0506300)National Natural Science Foundation of China(No.52336009)+5 种基金Key Research and Development Program of Shaanxi(No.2024CY2-GJHX-66)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010429)Natural Science Basic Research Plan in Shaanxi Province of China(No.2024JC-YBQN-0475)Xidian University Specially Funded Project for Interdisciplinary Exploration(No.TZJH2024063)the Fundamental Research Funds for the Central Universities(No.QTZX23061)the Innovation Center of Nuclear Power Technology(No.HDLCXZX-2022-ZH-013).
文摘Protonic ceramic fuel cells(PCFCs)have been recognized as promising power generation devices for future clean energy systems,owing to their relatively low activation energy for proton migration and high energy conversion efficiency.In certain application scenarios,the use of N_(2)O(a potent greenhouse gas),as an alternative oxidant to air,presents a feasible strategy.Herein,we report for the first time the operation of PCFCs employing N_(2)O as the oxidant.A hybrid Pr_(2)Ni_(0.6)Co_(0.4)O_(4-δ)(PNCO-214)catalyst is developed,comprising Ruddlesden-Popper(R-P)structured Pr_(4)Ni_(1.8)Co_(1.2)O_(10-δ)(PNCO-4310)and fluorite structured Pr_(6)O_(11)(PO-611),which synergistically exhibits exceptional catalytic activity toward both N_(2)O decomposition and the oxygen reduction reaction,achieving a conversion over 92% and an area specific resistance of 1.301Ω·cm^(2) at 600℃.Quasi-insitu temperature-dependent Fourier transform infrared(FTIR)and electrochemical impedance spectroscopy analyses reveal that abundant oxygen vacancies in PNCO-214 facilitate rapid adsorption and dissociation of N_(2)O into N_(2) and O_(2),while also promoting the surface exchange kinetics of proton/oxygen during oxygen reduction reaction(ORR).When applied in an anode-supported single cell with PNCO-214 cathode operating under N_(2)O,outstanding power density and low resistance are achieved,delivering 0.801 W·cm^(-2) and 0.245Ω·cm^(2) at 600℃.Satisfactory performance is also maintained even when the temperature is reduced to 500℃.Furthermore,the single cell demonstrates relatively good stability with negligible degradation over 130 h at 600℃ and 0.7 V.These findings underscore the potential of PNCO-214 as a highly effective cathode catalyst for enabling the use of N_(2)O as a viable oxidant in PCFCs for specific industrial applications.
基金financial support from the National Natural Science Foundation of China(22109003)the Basic and Applied Basic Research Foundation of Guangdong Province(2023A1515011391)+1 种基金Soft Science Research Project of Guangdong Province(No.2017B030301013)the Major Science and Technology Infrastructure Project of Material Genome Big-science Facilities Platform supported by Municipal Development and Reform Commission of Shenzhen.
文摘Understanding the proton dynamic behavior in inorganic materials has long been a topic of intense fascination[1],especially in the field of electrochemical energy storage[2].One of the examples is the research of proton transport in transition metal oxides,which dates back to 1971[3]when RuO_(2) was discovered to be capable of storing protons via reversible redox reactions[4].In aqueous electrolytes,the thin film RuO_(2) electrode exhibits a surface pseudocapacitive behavior[5],which could be modified by the structural water in its hydrated form due to the facile Grotthuss hopping mode of protons along the established hydrogen bonds inside the bulk phase[6].Soon later,Goodenough et al.reported the capacitor-like behavior of amorphous MnO_(2)·xH_(2)O electrode in an aqueous KCl electrolyte[7],and further studies on the hydrated MnO_(2) electrodes prepared by sol-gel processes have soon discovered that the intercalation of protons from aqueous electrolytes plays an indispensable role in the charge storage mechanism[8].In recent years,the research interest on rechargeable aqueous batteries has fueled the renaissance of mechanistic study of proton transport in transition metal oxides[9],which can operate as cathodes or anodes via a topotactic insertion mechanism similar to that in Li-ion batteries[10].However,due to the challenges for experimental detection of local chemical environments of the inserted protons,a comprehensive understanding of proton dynamic behavior in these electrodes remains largely lacking.
基金supported by the National Natural Science Foundation of China(Grant Nos.12075081 and 12404395)the Innovation Group Project of the Natural Science Foundation of Hubei Province of China(Grant No.2024AFA038)Bin Liu acknowledges the support of Guangdong High Level Innovation Research Institute Project,Grant No.2021B0909050006.
文摘The significance of laser-driven polarized beam acceleration has been increasingly recognized in recent years.We propose an efficient method for generating polarized proton beams from a pre-polarized hydrogen halide gas jet,utilizing magnetic vortex acceleration enhanced by a laser-driven plasma bubble.When a petawatt laser pulse passes through a pre-polarized gas jet,a bubble-like ultra-nonlinear plasma wave is formed.As a portion of the particles constituting this wave,background protons are swept by the acceleration field of the bubble and oscillate significantly along the laser propagation axis.Some of the pre-accelerated protons in the plasma wave are trapped by the acceleration field at the rear side of the target.This acceleration field is intensified by the transverse expansion of the laser-driven magnetic vortex,resulting in energetic polarized proton beams.The spin of energetic protons is determined by their precession within the electromagnetic field,which is described using the Thomas-Bargmann-Michel-Telegdi equation in analytical models and particle-in-cell simulations.Multidimensional simulations reveal that monoenergetic proton beams with an energy of hundreds of MeV,a beam charge of hundreds of pC,and a beam polarization of tens of percent can be produced at laser powers of several petawatts.Such laser-driven polarized proton beams have promise for application in polarized beam colliders,where they can be utilized to investigate particle interactions and to explore the properties of matter under extreme conditions.
基金financially supported by the Natural Science Foundation of Hunan Province(2023JJ40608,2024JJ6413)the Majoy Project of the Education Department of Hunan Province(24A0610).
文摘Proton exchange membrane water electrolysis(PEMWE)technology is widely recognized as a cornerstone for green hydrogen production,offering high operational current densities exceeding 1.0 A cm^(-2),rapid dynamic response capabilities,and zero-carbon emission characteristics[1].However,the sluggish kinetics of oxygen evolution reaction(OER)at the anode presents a critical bottleneck for large-scale commercial deployment(Fig.1(a)).Despite significant advancements through electronic structure modulation[2]and coordination environment optimization[3],the deprotonation energy barrier of oxygen-containing intermediates and the stability of active sites under acidic conditions remain unresolved challenges.
基金supported by the Natural Sciences and Engineering Research Council(NSERC)of Canada,Discovery Grant(GRPIN-2016-05494)Strategic Research Projects of Alberta Innovates Technology Futures(#G2016000655)funding from the Canada First Research Excellence Fund(CFREF-2015-00001).
文摘“Three-in-one”cathode,achieved via B-site heavy-doping of transition elements(typically Co,Fe)into proton-conductive perovskite,holds promise for enhancing the performance of proton-conducting solid oxide fuel cell(H-SOFC)operated below 650℃for electricity generation.However,its electrochemical behavior above 650℃,essential for improving the efficiency of H-SOFC for fuel conversion,remains insufficiently explored.It is still challenging to propose guidance for the design of“threein-one”cathode toward optimal H-SOFC performance below and above 650℃,with the prerequisite of gaining a comprehensive understanding of the roles of Co and Fe in determining the H-SOFC performance.This work is to address this challenge.Through theoretical/experimental studies,Co is identified to play a role in improving the oxygen reduction reaction(ORR)activity while Fe plays a role in facilitating the cathode/electrolyte interfacial proton conduction.Therefore,if the operating temperature is above 650℃,lowering the Co/Fe ratio in“three-in-one”cathode becomes crucial since the limiting factor shifts from ORR activity to proton conduction.Implementing this strategy,the SOFC using BaCo_(0.15)-Fe_(0.55)Zr_(0.1)Y_(0.1)Yb_(0.1)O_(3−δ)cathode achieves peak power densities of 1.67Wcm^(−2)under H-SOFC mode at 700℃and 2.32Wcm^(−2)under dual ion-conducting SOFC mode at 750℃,which are the highest reported values so far.
基金support from MATRIX(ANR-22-CE92-0047)with financial support from ITMI Cancer of Aviesan within the framework of the 2021−2030 Cancer Control Strategy,on funds administrated by INSERM through the project NECTAR.Matilde Siviero acknowledges funding from the French−German University/Saarbrücken(contract CDOC-06-2022).
文摘GaN diodes for high energy(64.8 MeV)proton detection were fabricated and investigated.A comparison of the performance of GaN diodes with different structures is presented,with a focus on sapphire and on GaN substrates,Schottky and pin diodes,and different active layer thicknesses.Pin diodes fabricated on a sapphire substrate are the best choice for a GaN proton detector working at 0 V bias.They are sensitive(minimum detectable proton beam<1 pA/cm^(2)),linear as a function of proton current and fast(<1 s).High proton current sensitivity and high spatial resolution of GaN diodes can be exploited in the future for proton imaging of patients in proton therapy.
基金supported by the National Key R&D Program of China(Nos.2022YFA1603200 and 2022YFA1603201)National Natural Science Foundation of China(Nos.12135001,11921006,12475243 and 11825502)+1 种基金Strategic Priority Research Program of CAS(No.XDA25050900)support from the National Natural Science Funds for Distinguished Young Scholar(No.11825502)。
文摘We put forward a new design of a compact beam transport system for intense laser-driven proton therapy,where instead of using conventional pulsed solenoids,our design relies on a helical coil irradiated by a nanosecond laser pulse to generate strong magnetic fields for focusing protons.A pair of dipole magnets and apertures are employed to further filter protons with large divergences and low energies.Our numerical studies combine particle-in-cell simulations for laser-plasma interaction to generate high-energy monoenergetic proton beams,finite element analysis for evaluating the magnetic field distribution inside the coil,and MonteCarlo simulations for beam transport and energy deposition.Our results show that with this design,a spread-out Bragg peak in a range of several centimeters to a deep-seated tumor with a dose of approximately 16.5 cGy and fluctuation around 2% can be achieved.The instantaneous dose rate reaches up to 10^(9)Gy/s,holding the potential for future FLASH radiotherapy research.
基金supported by the National Natural Science Foundation of China(No.22179047)the Development of Scientific and Technological Project of Jilin Province(20230201139GX).
文摘The thiol-imidazole functionalized(p-triphenyl-pentafluorobenzaldehyde)polymer(IMPTP)was prepared and quaternized with different side chains to obtain imidazolium-modified Me-IMPTP,He-IMPTP and BIM-IMPTP membranes for application in high-temperature proton exchange membrane fuel cells(HT-PEMFCs).The presence of the thioether group in the polymers enabled radical scavenging for antioxidant properties,while imidazolium cations interacted strongly with H_(2)PO_(4) to prevent phosphoric acid(PA)leaching.The prepared BIM-IMPTP membrane incorporating bisimidazolium cation string with a long alkyl spacer demonstrated the highest mass retention of 82.93%after being immersed in Fenton's reagent for 24 h.Additionally,the PA-doped BIM-IMPTP membranes exhibited excellent PA retention under high-humidity conditions(80℃/100%RH).The single cell equipped with the BIM-IMPTP/320%PA membrane achieved a maximum power density(PDmax)of 945 mW cm^(-2)at 160℃.Among the four membranes with a similar acid doping content(ADC),the BIM-IMPTP/163%PA membrane with bis-cation pairs in the side chains exhibited a well-developed microphase-separated structure and high proton conductivity(119.0 mS cm^(-1)at 180℃).The single cell assembled with BIM-IMPTP/163%PA membrane maintained a PDmax of 613 mW cm^(-2)at 160℃ and demonstrated long-term operational stability under both 150/400 mA cm^(-2)and 80℃/200 mA cm^(-2)conditions.These results indicate that the introduction of thioether and bis-cation pairs in the structural design of polymers contributes significantly to the long-term stability of HT-PEMs.
基金supported by the CEA/DAM Laser Plasma Experiments Validation Project and the CEA/DAM Basic Technical and Scientific Studies Projectsupported by the National Sciences and Engineering Research Council of Canada(NSERC)(Grant Nos.RGPIN-2023-05459 and ALLRP 556340-20)+3 种基金the Digital Research Alliance of Canada(Job pve-323-ac)the Canada Foundation for Innovation(CFI)the Ministère de l’Économie,de l’Innovation et de l’Énergie(MEIE)from QuébecThis study was granted access to the HPC resources of IRENE under allocation Grant No.A0170512899 made by GENCI.We acknowledge the financial support of the IdEx University of Bordeaux/Grand Research Program“GPR LIGHT”and of the Graduate Program on Light Sciences and Technologies of the University of Bordeaux.
文摘Laser-driven ion acceleration,as produced by interaction of a high-intensity laser with a target,is a growing field of interest.One of the current challenges is to enhance the acceleration process,i.e.,to increase the produced ion energy and the ion number and to shape the energy distribution for future applications.In this paper,we investigate the effect of helical coil(HC)targets on the laser-matter interaction process using a 150 TW laser.We demonstrate that HC targets significantly enhance proton acceleration,improving energy bunching and beam focusing and increasing the cutoff energy.For the first time,we extend this analysis to carbon ions,revealing a marked reduction in the number of low-energy carbon ions and the potential for energy bunching and post-acceleration through an optimized HC design.Simulations using the particle-in-cell code SOPHIE confirm the experimental results,providing insights into the current propagation and ion synchronization mechanisms in HCs.Our findings suggest that HC targets can be optimized for multispecies ion acceleration.
基金financial support from the National Natural Science Foundation of China(Nos.51922003,52274406)the Fundamental Research Funds for the Central Universities,China(No.FRF-BD-23-02)。
文摘To address the challenge of insufficient oxygen vacancies in proton-conducting solid oxide fuel cells(H-SOFC),transition metal elements were doped into the B site of lanthanum ferrite perovskite(ABO3)to enhance its catalytic activity further.The Mo-doped La_(0.6)Sr_(0.4)Fe_(0.9)Ni_(0.1)O_(3-δ)(LSFNMx,x=0.05,0.1)powder was synthesized via the sol−gel method,and its crystal structure,conductivity,defect chemistry,and electrochemical performance as an H-SOFC cathode were investigated.The prepared material exhibited a hexagonal structure with the R-3c space group and demonstrates good chemical stability under simulated working conditions.Mo doping increased the surface concentration of oxygen vacancies,leading to the accelerated oxygen transportation.Consequently,the polarization resistance(Rpol)and activation energy(Ea)are reduced.Specifically,LSFNM0.05 showed the lowest polarization resistance(approximately 0.26Ω·cm^(2))at 700°C.LSFNM0.05 achieved a maximum power density of 484 mW/cm^(2)at this temperature,outperforming those of LSFN(353 mW/cm^(2))and LSFNM0.1(365 mW/cm^(2)).
基金financial support from the JSPS KAKENHI Grant-in-Aid for Scientific Research(B),No.21H02035KAKENHI Grant-in-Aid for Challenging Research(Exploratory),No.21K19017+2 种基金KAKENHI Grant-in-Aid for Transformative Research Areas(B),No.21H05100National Natural Science Foundation of China,No.22409033 and No.22409035Basic and Applied Basic Research Foundation of Guangdong Province,No.2022A1515110470.
文摘Protonic solid oxide electrolysis cells(P-SOECs)are a promising technology for water electrolysis to produce green hydrogen.However,there are still challenges related key materials and anode/electrolyte interface.P-SOECs with Zr-rich electrolyte,called Zr-rich side P-SOECs,possess high thermodynamically stability under high steam concentrations but the large reaction resistances and the current leakage,thus the inferior performances.In this study,an efficient functional interlayer Ba_(0.95)La_(0.05)Fe_(0.8)Zn_(0.2)O_(3-δ)(BLFZ)in-between the anode and the electrolyte is developed.The electrochemical performances of P-SOECs are greatly enhanced because the BLFZ can greatly increase the interface contact,boost anode reaction kinetics,and increase proton injection into electrolyte.As a result,the P-SOEC yields high current density of 0.83 A cm^(-2) at 600℃ in 1.3 Vamong all the reported Zr-rich side cells.This work not only offers an efficient functional interlayer for P-SOECs but also holds the potential to achieve P-SOECs with high performances and long-term stability.
基金supported by the China Scholarship Council(No.202408120105)National Natural Science Foundation of China(32301530)+5 种基金Young Elite Scientist Sponsorship Program by CAST(No.YESS20230242)Tianjin Excellent Special Commissioner for Agricultural Science and Technology Project(23ZYCGSN00580)Natural Science Foundation of Tianjin(23JCZDJC00630)China Postdoctoral Science Foundation(2023M740563)State Key Laboratory of Pulp and Paper Engineering(202412,202413)the Central Publicinterest Scientific Institution Basa Research Fund(No.Y2022QC30).
文摘Proton-conducting materials have attracted considerable interest because of their extensive application in energy storage and conversion devices.Among them,metal-organic frameworks(MOFs)present tremendous development potential and possibilities for constructing novel advanced proton conductors due to their special advantages in crystallinity,designability,and porosity.In particular,several special design strategies for the structure of MOFs have opened new doors for the advancement of MOF proton conductors,such as charged network construction,ligand functionalization,metal-center manipulation,defective engineering,vip molecule incorporation,and pore-space manipulation.With the implementation of these strategies,proton-conducting MOFs have developed significantly and profoundly within the last decade.Therefore,in this review,we critically discuss and analyze the fundamental principles,design strategies,and implementation methods targeted at improving the proton conductivity of MOFs through representative examples.Besides,the structural features,the proton conduction mechanism and the behavior of MOFs are discussed thoroughly and meticulously.Future endeavors are also proposed to address the challenges of proton-conducting MOFs in practical research.We sincerely expect that this review will bring guidance and inspiration for the design of proton-conducting MOFs and further motivate the research enthusiasm for novel proton-conducting materials.
基金National Key R&D Program of China,Grant/Award Number:2021YFA1500900Basic and Applied Basic Research Foundation of Guangdong Province-Regional Joint Fund Project,Grant/Award Number:2021B1515120024+9 种基金Science Funds of the Education Office of Jiangxi Province,Grant/Award Number:GJJ2201324Science Funds of Jiangxi Province,Grant/Award Numbers:20242BAB25168,20224BAB213018Doctoral Research Start-up Funds of JXSTNU,Grant/Award Number:2022BSQD05China Postdoctoral Science Foundation,Grant/Award Number:2023M741121National Natural Science Foundation of China,Grant/Award Number:22172047Provincial Natural Science Foundation of Hunan,Grant/Award Number:2021JJ30089Shenzhen Science and Technology Program,Grant/Award Number:JCYJ20210324122209025Changsha Municipal Natural Science Foundation,Grant/Award Number:kq2107008Hunan Province of Huxiang Talent project,Grant/Award Number:2023rc3118Natural Science Foundation of Hunan Province,Grant/Award Number:2022JJ10006.
文摘Hydrogen energy from electrocatalysis driven by sustainable energy has emerged as a solution against the background of carbon neutrality.Proton exchange membrane(PEM)-based electrocatalytic systems represent a promising technology for hydrogen production,which is equipped to combine efficiently with intermittent electricity from renewable energy sources.In this review,PEM-based electrocatalytic systems for H2 production are summarized systematically from low to high operating temperature systems.When the operating temperature is below 130℃,the representative device is a PEM water electrolyzer;its core components and respective functions,research status,and design strategies of key materials especially in electrocatalysts are presented and discussed.However,strong acidity,highly oxidative operating conditions,and the sluggish kinetics of the anode reaction of PEM water electrolyzers have limited their further development and shifted our attention to higher operating temperature PEM systems.Increasing the temperature of PEM-based electrocatalytic systems can cause an increase in current density,accelerate reaction kinetics and gas transport and reduce the ohmic value,activation losses,ΔGH*,and power consumption.Moreover,further increasing the operating temperature(120-300℃)of PEM-based devices endows various hydrogen carriers(e.g.,methanol,ethanol,and ammonia)with electrolysis,offering a new opportunity to produce hydrogen using PEM-based electrocatalytic systems.Finally,several future directions and prospects for developing PEM-based electrocatalytic systems for H_(2) production are proposed through devoting more efforts to the key components of devices and reduction of costs.
基金National Natural Science Foundation of China(No.52476192,No.52106237)Natural Science Foundation of Heilongjiang Province(No.YQ2022E027)。
文摘The transition of hydrogen sourcing from carbon-intensive to water-based methodologies is underway,with renewable energy-powered proton exchange membrane water electrolysis(PEMWE)emerging as the preeminent pathway for hydrogen production.Despite remarkable advancements in this field,confronting the sluggish electrochemical kinetics and inherent high-energy consumption arising from deteriorated mass transport within PEMWE systems remains a formidable obstacle.This impediment stems primarily from the hindered protons mass transfer and the untimely hydrogen bubbles detachment.To address these challenges,we harness the inherent variability of electrical energy and introduce an innovative pulsed dynamic water electrolysis system.Compared to constant voltage electrolysis(hydrogen production rate:51.6 m L h^(-1),energy consumption:5.37 kWh Nm-^(3)H_(2)),this strategy(hydrogen production rate:66 m L h^(-1),energy consumption:3.83 kWh Nm-^(3)H_(2))increases the hydrogen production rate by approximately 27%and reduces the energy consumption by about 28%.Furthermore,we demonstrate the practicality of this system by integrating it with an off-grid photovoltaic(PV)system designed for outdoor operation,successfully driving a hydrogen production current of up to 500 mA under an average voltage of approximately 2 V.The combined results of in-situ characterization and finite element analysis reveal the performance enhancement mechanism:pulsed dynamic electrolysis(PDE)dramatically accelerates the enrichment of protons at the electrode/solution interface and facilitates the release of bubbles on the electrode surface.As such,PDE-enhanced PEMWE represents a synergistic advancement,concurrently enhancing both the hydrogen generation reaction and associated transport processes.This promising technology not only redefines the landscape of electrolysis-based hydrogen production but also holds immense potential for broadening its application across a diverse spectrum of electrocatalytic endeavors.
文摘To develop proton-conducting materials with high hydrothermal and acid-base stability and to elucidate the proton-transport mechanism through visualized structural analysis,two new lanthanum phosphite-oxalates with 3D frameworks,designated as[La(HPO_(3))(C_(2)O_(4))0.5(H_(2)O)_(2)](La‑1)and(C_(6)H_(16)N_(2))(H_(3)O)[La_(2)(H_(2)PO_(3))_(3)(C_(2)O_(4))_(3)(H_(2)O)](La‑2)(C_(6)H_(14)N_(2)=cis-2,6-dimethylpiperazine),were prepared by hydrothermal and solvothermal conduction,respectively.La‑1 was constructed with lanthanum phosphite 2D layers and C_(2)O_(4)^(2-)groups,whereas La‑2 was constructed with lanthanum oxalate 2D layers and H_(2)PO^(3-)groups.Alternating current(AC)impedance spectra indicate that the pro-ton conductivities of both compounds could reach 10^(-4)S·cm^(-1)and remain highly durable at 75℃and 98%of rela-tive humidity(RH).Due to the abundance of H-bonds in La‑2,theσof La‑2 was higher than that of La‑1.La‑1 exhibited excellent water and pH stability.CCDC:2439965,La‑1;443776,La‑2.
文摘BACKGROUND Proton pump inhibitors(PPIs)are widely used,including among cancer patients,to manage gastroesophageal reflux and other gastric acid-related disorders.Recent evidence suggests associations between long-term PPI use and higher risks for various adverse health outcomes,including greater mortality.AIM To investigate the association between PPI use and all-cause mortality among cancer patients by a comprehensive analysis after adjustment for various confounders and a robust methodological approach to minimize bias.METHODS This retrospective cohort study used data from the TriNetX research network,with electronic health records from multiple healthcare organizations.The study employed a new-user,active comparator design,which compared newly treated PPI users with non-users and newly treated histamine2 receptor antagonists(H2RA)users among adult cancer patients.Newly prescribed PPIs(esomeprazole,lansoprazole,omeprazole,pantoprazole,or rabeprazole)users were compared to non-users or newly prescribed H2RAs(cimetidine,famotidine,nizatidine,or ranitidine)users.The primary outcome was all-cause mortality.Each patient in the main group was matched to a patient in the control group using 1:1 propensity score matching to reduce confounding effects.Multivariable Cox regression models were used to estimate hazard ratios(HRs)and 95% confidence interval(CI).RESULTS During the follow-up period(median 5.4±1.8 years for PPI users and 6.5±1.0 years for non-users),PPI users demonstrated a higher all-cause mortality rate than non-users after 1 year,2 years,and at the end of follow up(HRs:2.34-2.72).Compared with H2RA users,PPI users demonstrated a higher rate of all-cause mortality HR:1.51(95%CI:1.41-1.69).Similar results were observed across sensitivity analyses by excluding deaths from the first 9 months and 1-year post-exposure,confirming the robustness of these findings.In a sensitivity analysis,we analyzed all-cause mortality outcomes between former PPI users and individuals who have never used PPIs,providing insights into the long-term effects of past PPI use.In addition,at 1-year follow-up,the analysis revealed a significant difference in mortality rates between former PPI users and non-users(HR:1.84;95%CI:1.82-1.96).CONCLUSION PPI use among cancer patients was associated with a higher risk of all-cause mortality compared to non-users or H2RA users.These findings emphasize the need for cautious use of PPIs in cancer patients and suggest that alternative treatments should be considered when clinically feasible.However,further studies are needed to corroborate our findings,given the significant adverse outcomes in cancer patients.
基金National Key Research and Development Program of China(2020YFA0710302)The Major Research Plan of the National Natural Science Foundation of China(91963206)+2 种基金The National Natural Science Foundation of China(52072169,51972164,51972167,22279053)The Fundamental Research Funds for the Central Universities(14380193)The Program for Guangdong Introducing Innovative and Entrepreneurial Teams(2019ZT08L101).
文摘On the surfaces of celestial bodies with no or thin atmospheres,such as the Moon and Mars,the solar wind irradiation process leads to the formation of hydrogen and helium enriched regions in the extraterrestrial soil particles.However,soil particles on the Earth with the similar composition lack such structures and properties.This discrepancy raises a key question whether there is a direct relationship between solar wind irradiation and the alterations in the structure and chemical performance of extraterrestrial materials.To address this question,this work investigates the effects of proton irradiation,simulating solar wind radiation,on the structure and photothermal catalytic properties of the classic catalyst In_(2)O_(3).It reveals that proton irradiation induces structural features in In_(2)O_(3) analogous to those characteristics of solar wind weathering observed in extraterrestrial materials.Furthermore,after proton beam irradiation with an energy of 30 keV and a dose of 3×10^(17) protons·cm^(-2),the methanol production yield of the In_(2)O_(3) catalyst increased to 2.6 times of its preirradiation level,and the methanol selectivity improved to 2.1 times of the original value.This work provides both theoretical and experimental support for the development of high-efficiency,radiation-resistant photothermal catalysts.
基金supported by the National Natural Science Foundation of China(22209040,22202063).
文摘The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.
