Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,par...Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,particularly the presence of aggressive Cl^(-),has been proven to be prone to parasitic chloride ion oxidation and corrosion reactions,thus restricting seawater electrolyzer lifetime.Herein,hierarchical structure(Ni,Fe)O(OH)@NiCoS nanorod arrays(NAs)catalysts with heterointerfaces and localized oxygen vacancies were synthesized at nickel foam substrates via the combination of hydrothermal and annealing methods to boost seawater dissociation.The hiera rchical nanostructure of NiCoS NAs enhanced electrode charge transfer rate and active surface area to accelerate oxygen evolution reaction(OER)and generated sulfate gradient layers to repulsive aggressive Cl^(-).The fabricated heterostructure and vacancies of(Ni,Fe)O(OH)tuned catalyst electronic structure into an electrophilic state to enhance the binding affinity of hydroxyl intermediates and facilitate the structural transformation into amorphousγ-NiFeOOH for promoting OER.Furthermore,through operando electrochemistry techniques,we found that theγ-NiFeOOH possessing an unsaturated coordination environment and lattice-oxygen-participated OER mechanism can minimize electrode Cl^(-)corrosion enabled by stabilizing the adsorption of OH*intermediates,making it one of the best OER catalysts in the seawater medium reported to date.Consequently,these catalysts can deliver current densities of 100 and 500 mA cm-2for boosting OER at minimal overpotentials of 245and 316 mV,respectively,and thus prevent chloride ion oxidation simultaneously.Impressively,a highly stable anion exchange membrane(AEM)seawater electrolyzer based on the non-noble metal heterostructure electrodes reached a record low degradation rate under 100μV h-1at constant industrial current densities of 400 and 600 mA cm-2over 300 h,which exhibits a promising future for the nonprecious and stable AEMWE in the direct seawater electrolysis industry.展开更多
Mangrove and salt-marsh wetlands are important coastal carbon sinks.In order to quantify carbon export via pore water exchange and to evaluate subsequent fate of the exported carbon,we carried out continuous observati...Mangrove and salt-marsh wetlands are important coastal carbon sinks.In order to quantify carbon export via pore water exchange and to evaluate subsequent fate of the exported carbon,we carried out continuous observations in a mangrove-Spartina alterniflora ecozone in the Zhangjiang River Estuary,China.The carbon fluxes via pore water exchange were estimated using^(222)Rn and^(228)Ra as tracers to be(2.15±0.63)mol/(m^(2)∙d)for dissolved inorganic carbon(DIC)and(-0.008±0.07)mol/(m^(2)∙d)for dissolved organic carbon(DOC)in the wet season and(3.02±0.65)mol/(m^(2)∙d)for DIC and(-0.15±0.007)mol/(m^(2)∙d)for DOC in the dry season in the mangrove-dominated creek(M-creek),while(2.52±0.82)mol/(m^(2)∙d)for DIC and(0.02±0.09)mol/(m^(2)∙d)for DOC in the dry season in the S.alterniflora-dominated creek(SA-creek).The negative value means that pore water was a sink of DOC in the creek.The total carbon via pore water exchange in the tidal creeks in the mangroves accounted for 41%-55%of the net carbon fixed by mangrove vegetation and was 3-4 times as much as the soil carbon accretion in the mangroves.The exported carbon in the form of DIC contributed all of the carbon outwelling from the M-creek and 79%of the carbon outwelling from the SA-creek,implying effective fixation of carbon by the wetland ecosystem.Moreover,it resulted in 54%in the dry season,75%in the wet season of the carbon dioxide released from the M-creek to the atmosphere,and 84%of the release from the SA-creek.Therefore,quantification of pore water exchange and related soil carbon loss is essential to trace the fate of carbon fixed in intertidal wetlands.展开更多
Anion exchange membrane(AEM)electrolysis is a promising membrane-based green hydrogen production technology.However,AEM electrolysis still remains in its infancy,and the performance of AEM electrolyzers is far behind ...Anion exchange membrane(AEM)electrolysis is a promising membrane-based green hydrogen production technology.However,AEM electrolysis still remains in its infancy,and the performance of AEM electrolyzers is far behind that of well-developed alkaline and proton exchange membrane electrolyzers.Therefore,breaking through the technical barriers of AEM electrolyzers is critical.On the basis of the analysis of the electrochemical performance tested in a single cell,electrochemical impedance spectroscopy,and the number of active sites,we evaluated the main technical factors that affect AEM electrolyzers.These factors included catalyst layer manufacturing(e.g.,catalyst,carbon black,and anionic ionomer)loadings,membrane electrode assembly,and testing conditions(e.g.,the KOH concentration in the electrolyte,electrolyte feeding mode,and operating temperature).The underlying mechanisms of the effects of these factors on AEM electrolyzer performance were also revealed.The irreversible voltage loss in the AEM electrolyzer was concluded to be mainly associated with the kinetics of the electrode reaction and the transport of electrons,ions,and gas-phase products involved in electrolysis.Based on the study results,the performance and stability of AEM electrolyzers were significantly improved.展开更多
The formation of multiple oxygen intermediates supporting efficient oxygen evolution reaction(OER)are affinitive with hydroxyl adsorption.However,ability of the catalyst to capture hydroxyl and maintain the continuous...The formation of multiple oxygen intermediates supporting efficient oxygen evolution reaction(OER)are affinitive with hydroxyl adsorption.However,ability of the catalyst to capture hydroxyl and maintain the continuous supply at active sits remains a tremendous challenge.Herein,an affordable Ni2P/FeP2 heterostructure is presented to form the internal polarization field(IPF),arising hydroxyl spillover(HOSo)during OER.Facilitated by IPF,the oriented HOSo from FeP2 to Ni2P can activate the Ni site with a new hydroxyl transmission channel and build the optimized reaction path of oxygen intermediates for lower adsorption energy,boosting the OER activity(242 mV vs.RHE at 100 mA cm-2)for least 100 h.More interestingly,for the anion exchange membrane water electrolyzer(AEMWE)with low concentration electrolyte,the advantage of HOSo effect is significantly amplified,delivering 1 A cm^(-2)at a low cell voltage of 1.88 V with excellent stability for over 50 h.展开更多
The water exchange matrix is an efficient tool to study the water exchange among the sub-areas in large-scale bays.The application of the random walk method to calculate the water exchange matrix is studied.Compared w...The water exchange matrix is an efficient tool to study the water exchange among the sub-areas in large-scale bays.The application of the random walk method to calculate the water exchange matrix is studied.Compared with the advection-diffusion model,the random walk model is more flexible to calculate the water exchange matrix. The forecast matrix suggested by Thompson et al.is used to evaluate the water exchange characteristics among the sub-areas fast.According to the theoretic analysis,it is found that the precision of the predicted results is mainly affected by three factors,namely, the particle number,the generated time of the forecast matrix,and the number of the sub-areas.The impact of the above factors is analyzed based on the results of a series of numerical tests.The results show that the precision of the forecast matrix increases with the increase of the generated time of the forecast matrix and the number of the particles. If there are enough particles in each sub-area,the precision of the forecast matrix will increase with the number of the sub-areas.Moreover,if the particles in each sub-area are not enough,the excessive number of the sub-areas can result in the decrease of the precision of the forecast matrix.展开更多
Anion exchange membrane(AEM)water electrolyzers are promising energy devices for the production of clean hydrogen from seawater.However,the lack of active and robust electrocatalysts for the oxygen evolution reaction(...Anion exchange membrane(AEM)water electrolyzers are promising energy devices for the production of clean hydrogen from seawater.However,the lack of active and robust electrocatalysts for the oxygen evolution reaction(OER)severely impedes the development of this technology.In this study,a ternary layered double hydroxide(LDH)OER electrocatalyst(NiFeCo-LDH)is developed for high-performance AEM alkaline seawater electrolyzers.The AEM alkaline seawater electrolyzer catalyzed by the NiFeCo LDH shows high seawater electrolysis performance(0.84 A/cm^(2)at 1.7 Vcell)and high hydrogen production efficiency(77.6%at 0.5 A/cm^(2)),thus outperforming an electrolyzer catalyzed by a benchmark IrO_(2)electrocatalyst.The NiFeCo-LDH electrocatalyst greatly improves the kinetics of the AEM alkaline seawater electrolyzer,consequently reducing its activation loss and leading to high performance.Based on the results,this NiFeCo-LDH-catalyzed AEM alkaline seawater electrolyzer can likely surpass the energy conversion targets of the US Department of Energy.展开更多
For estuaries,inland lakes play a vital role in the ecological balance under the impact of tide s.The effect of tides-induced water exchange on phytoplankton community in a semi-closed lake was studied and compared wi...For estuaries,inland lakes play a vital role in the ecological balance under the impact of tide s.The effect of tides-induced water exchange on phytoplankton community in a semi-closed lake was studied and compared with that of an adjacent closed lake in the Oujiang River mouth in Zhejiang,East China Sea,from June 29,2020 to June 14,2021.Results show that the dominant species,abundance,dominance,and diversity of the phytoplankton species between the two lakes were significantly different.In the closed lake,cyanobacteria were the dominant species during the study period.However.in the semi-closed lake,the diversification of the dominant species was greater,and some species of diatoms and green algae became dominant.The average phytoplankton abundance in the closed lake was 6 times of that in the semi-closed lake.The average dominance of cyanobacteria in the closed lake was 0.96,and those in the semi-closed lake and the Oujiang River were 0.51 and 0.22,respectively.Cyanobacterial blooms occurred throughout the study time in the closed lake but not in the semi-closed one.Furthermore,the species diversity richness of the phytoplankton in the semi-closed lake was higher than that of the closed one,and the phytoplankton community between the closed lake and semi-closed lake could be divided into distinctly different groups based on non-metic multidimensional scaling analysis(NMDS)and analysis of similarities(ANOSIM)analysis.The salinity of the water was significantly greater and the transparency significantly smaller in the semi-closed lake than those in the closed lake.Therefore,water exchange driven by local tidal movement increased salinity and decreased transparency of water,which consequently shaped the community structures of different phytoplankton and reduced the risk of a cyanobacterial bloom outbreak in the semi-closed lake.展开更多
The characteristics of the T/S structures,water mass exchange and deep circulation in the Andaman Sea are investigated based on the simulation from a high-resolution general circulation model(MITgcm).The results show ...The characteristics of the T/S structures,water mass exchange and deep circulation in the Andaman Sea are investigated based on the simulation from a high-resolution general circulation model(MITgcm).The results show that,below 1000 m,the water mass is saltier,warmer and more homogeneous in the Andaman Sea than that in the Bay of Bengal,attributing to the strong vertical mixing at the depth of^1800 m.The water mass exchange between the Andaman Sea and the Bay of Bengal goes through three major channels,which manifests itself as follows:the northern channel(Preparis Channel)is the main passage of water mass transport from the Bay of Bengal to the Andaman Sea,whereas the Middle Channel(the south of Andaman Islands and the north of Nicobar Islands)has an opposite transport;the southern channel(Great Channel)features with a four-layer water exchange which results in the least net transport among the three channels;all the transports through the three channels have an intra-annual variation with a period of half a year.At 1000-m depth,the entire Andaman Sea is occupied by a cyclonic circulation in January and July while by an anticyclonic one in April and October.The semiannual cycle found in both the deep circulation and water mass exchange is likely associated with the downwelling eastward-propagating Kelvin waves induced by the semiannual westerly component in the equatorial Indian Ocean during intermonsoon seasons.展开更多
Transmembrane water exchange(TWE)including transcytolemmal water exchange and transvascular water exchange is involved in many in vivo measurements and makes different contributions to the measuring results.In this st...Transmembrane water exchange(TWE)including transcytolemmal water exchange and transvascular water exchange is involved in many in vivo measurements and makes different contributions to the measuring results.In this study,we focus on the potential influence of TWE on the cell density parameter,intracellular water mole fraction pi,derived by dynamic contrast enhanced-magnetic resonance imaging(DCE-MRI)which has been reported as a technique to characterize perfusion and vascularization of tissues,but its accuracy in measuring cell density(or interstitial space)has been questioned.Sixteen patients with glioblastoma multiforme(GBM)were enrolled since GBM shows strong intratumor heterogeneity in both cell density and TWE.All the subjects were collected with DCE-MRI and apparent diffusion coefficient(ADC)map.The latter was considered as a valid surrogate of cell density.Extended Tofts(eTofts)model considering TWE as infinitely large variables and shutter-speed model(SSM)considering TWE as finite ones were used to fit DCE-MRI data.Monte Carlo(MC)and finite difference(FD)methods were used to simulate the influence of TWE on DCE-MRI-derived pi and ADC,respectively.The eTofts model shows a significant overestimation of pi in comparison with SSM in GBM(P<0.001),which is in accordance with MC simulations,and this overestimation shows dependence on the intra-to-extracellular water exchange rate constant(kio).Significant negative correlations between ADC and SSM-derived pi were found in both voxel-wise analyses(t-test P<0.001,average r=-0.74)and inter-subject comparisons(r=-0.63,P=0.009).But no consistent voxel-wise correlations(P>0.05)and a weaker inter-subject negative correlation(r=-0.56,P=0.02)were found between ADC and eTofts-derived pi.Further experimental and FD results revealed that kio made a limited contribution to ADC values in the physiological kio range in GBM,supporting ADC as a valid biomarker of cell density.These results suggest that the DCE-MRI pharmacokinetic shutter-speed model could significantly improve its accuracy in cell density estimation because of the considering transmembrane water exchange.展开更多
Water exchange between the different compartments of a heterogeneous specimen can be characterized via diffusion magnetic resonance imaging(dMRI).Many analysis frameworks using dMRI data have been proposed to describe...Water exchange between the different compartments of a heterogeneous specimen can be characterized via diffusion magnetic resonance imaging(dMRI).Many analysis frameworks using dMRI data have been proposed to describe exchange,often using a double diffusion encoding(DDE)stimulated echo sequence.Techniques such as diffusion exchange weighted imaging(DEWI)and the filter exchange and rapid exchange models,use a specific subset of the full space DDE signal.In this work,a general representation of the DDE signal was employed with different sampling schemes(namely constant b1,diagonal and anti-diagonal)from the data reduction models to estimate exchange.A near-uniform sampling scheme was proposed and compared with the other sampling schemes.The filter exchange and rapid exchange models were also applied to estimate exchange with their own subsampling schemes.These subsampling schemes and models were compared on both simulated data and experimental data acquired with a benchtop MR scanner.In synthetic data,the diagonal and near-uniform sampling schemes performed the best due to the consistency of their estimates with the ground truth.In experimental data,the shifted diagonal and near-uniform sampling schemes outperformed the others,yielding the most consistent estimates with the full space estimation.The results suggest the feasibility of measuring exchange using a general representation of the DDE signal along with variable sampling schemes.In future studies,algorithms could be further developed for the optimization of sampling schemes,as well as incorporating additional properties,such as geometry and diffusion anisotropy,into exchange frameworks.展开更多
The increasing demand for hydrogen energy to address environmental issues and achieve carbon neutrality has elevated interest in green hydrogen production,which does not rely on fossil fuels.Among various hydrogen pro...The increasing demand for hydrogen energy to address environmental issues and achieve carbon neutrality has elevated interest in green hydrogen production,which does not rely on fossil fuels.Among various hydrogen production technologies,anion exchange membrane water electrolyzer(AEMWE)has emerged as a next-generation technology known for its high hydrogen production efficiency and its ability to use non-metal catalysts.However,this technology faces significant challenges,particularly in terms of the membrane durability and low ionic conductivity.To address these challenges,research efforts have focused on developing membranes with a new backbone structure and anion exchange groups to enhance durability and ionic conductivity.Notably,the super-acid-catalyzed condensation(SACC)synthesis method stands out due to its user convenience,the ability to create high molecular weight(MW)polymers,and the use of oxygen-tolerant organic catalysts.Although the synthesis of anion exchange membranes(AEMs)using the SACC method began in 2015,and despite growing interest in this synthesis approach,there remains a scarcity of review papers focusing on AEMs synthesized using the SACC method.The review covers the basics of SACC synthesis,presents various polymers synthesized using this method,and summarizes the development of these polymers,particularly their building blocks including aryl,ketone,and anion exchange groups.We systematically describe the effects of changes in the molecular structure of each polymer component,conducted by various research groups,on the mechanical properties,conductivity,and operational stability of the membrane.This review will provide insights into the development of AEMs with superior performance and operational stability suitable for water electrolysis applications.展开更多
Due to the high heterogeneity and complexity of water flow movement for multiple karst water-bearing mediums,the evaluation,effective development,and utilization of karst water resources are significantly limited.Matr...Due to the high heterogeneity and complexity of water flow movement for multiple karst water-bearing mediums,the evaluation,effective development,and utilization of karst water resources are significantly limited.Matrix flow is usually laminar,whereas conduit flow is usually turbulent.The driving mechanisms of water exchange that occur between the karst conduit and its adjacent matrix are not well understood.This paper investigates the hydrodynamic characteristics and the mechanism of flow exchange in dual water-bearing mediums(conduit and matrix)of karst aquifers through laboratory experimentation and numerical simulation.A karst aquifer consisting of a matrix network and a conduit was proposed,and the relationship between the water exchange flux and hydraulic head differences generated from the laboratory experiments was analyzed.Two modes of experimental tests were performed with different fixed water level boundaries in the laboratory karst aquifer.The results indicate that the water exchange capacity was proportional to the square root of hydraulic head differences.The linear exchange term in the conduit flow process(CFP)source program was modified according to experimental results.The modified CFP and the original CFP model experimental data results were compared,and it was found that the modified CFP model had better fitting effects.These results showed that the water exchange mechanism between conduit and matrix is very important for solid-liquid interface reaction,water resource evaluation,and understanding of karst hydrodynamic behavior.展开更多
Thousands of lakes on the Tibetan Plateau(TP) play a critical role in the regional water cycle, weather, and climate. In recent years, the areas of TP lakes underwent drastic changes and have become a research hotspot...Thousands of lakes on the Tibetan Plateau(TP) play a critical role in the regional water cycle, weather, and climate. In recent years, the areas of TP lakes underwent drastic changes and have become a research hotspot. However, the characteristics of the lake-atmosphere interaction over the high-altitude lakes are still unclear, which inhibits model development and the accurate simulation of lake climate effects. The source region of the Yellow River(SRYR) has the largest outflow lake and freshwater lake on the TP and is one of the most densely distributed lakes on the TP. Since 2011,three observation sites have been set up in the Ngoring Lake basin in the SRYR to monitor the lake-atmosphere interaction and the differences among water-heat exchanges over the land and lake surfaces. This study presents an eight-year(2012–19), half-hourly, observation-based dataset related to lake–atmosphere interactions composed of three sites. The three sites represent the lake surface, the lakeside, and the land. The observations contain the basic meteorological elements,surface radiation, eddy covariance system, soil temperature, and moisture(for land). Information related to the sites and instruments, the continuity and completeness of data, and the differences among the observational results at different sites are described in this study. These data have been used in the previous study to reveal a few energy and water exchange characteristics of TP lakes and to validate and improve the lake and land surface model. The dataset is available at National Cryosphere Desert Data Center and Science Data Bank.展开更多
Platinum(Pt)-based electrocatalysts remain the only practical cathode catalysts for proton exchange membrane water electrolysis(PEMWE),due to their excellent catalytic activity for acidic hydrogen evolution reaction(H...Platinum(Pt)-based electrocatalysts remain the only practical cathode catalysts for proton exchange membrane water electrolysis(PEMWE),due to their excellent catalytic activity for acidic hydrogen evolution reaction(HER),but are greatly limited by their low reserves and high cost.Here,we report an interfacial engineering strategy to obtain a promising low-Pt loading catalyst with atomically Pt-doped molybdenum carbide quantum dots decorated on conductive porous carbon(Pt-MoCx@C)for high-rate and stable HER in PEMWE.Benefiting from the strong interfacial interaction between Pt atoms and the ultra-small MoCx quantum dots substrate,the Pt-MoCx catalyst exhibits a high mass activity of 8.00 A·mgPt−1,5.6 times higher than that of commercial 20 wt.%Pt/C catalyst.Moreover,the strong interfacial coupling of Pt and MoCx substrate greatly improves the HER stability of the Pt-MoCx catalyst.Density functional theory studies further confirm the strong metal-support interaction on Pt-MoCx,the critical role of MoCx substrate in the stabilization of surface Pt atoms,as well as activation of MoCx substrate by Pt atoms for improving HER durability and activity.The optimized Pt-MoCx@C catalyst demonstrates>2000 h stability under a water-splitting current of 1000 mA·cm^(−2)when applied to the cathode of a PEM water electrolyzer,suggesting the potential for practical applications.展开更多
Proton exchangemembrane(PEM)water electrolysis represents one of the most promising technologies to achieve green hydrogen production,but currently its practical viability is largely affected by the slow reaction kine...Proton exchangemembrane(PEM)water electrolysis represents one of the most promising technologies to achieve green hydrogen production,but currently its practical viability is largely affected by the slow reaction kinetics of the anodic oxygen evolution reaction(OER)in an acidic environment.While noble metal-based catalysts containing iridium or ruthenium are excellent catalysts for the acidic OER,their practical use in PEM electrolyzers is hindered due to their low abundance and high cost.Most recently,metal-organic frameworks(MOFs)have been demonstrated as a perfect platform to facilitate the design of acidic OER catalysts with both high efficiency and cost-effectiveness.Here,we pro-vide a timely and comprehensive overview of the recent progress on MOF-based acidic OER catalysts.The fundamental mechanisms of the acidic OER are first introduced,followed by a summary of the development of pristine MOFs and MOF derivatives as acidic OER catalysts.Importantly,a number of catalyst design strategies are discussed aiming at improving the acidic OER catalytic per-formance of MOF-based candidates.The integration of MOF-based catalysts into real PEM water electrolyzers is also included.Finally,future research directions are provided to achieve better MOF-based catalysts operational in acidic envi-ronments and PEM devices.展开更多
It is well known that one unit of electrical energy saved is equal to more than two units produced. One way of economizing the power is utilization of energy efficient systems at all locations. In the present study, t...It is well known that one unit of electrical energy saved is equal to more than two units produced. One way of economizing the power is utilization of energy efficient systems at all locations. In the present study, the air conditioning system is analysed and an innovative way is suggested. We use natural low temperature of shallow sub surface (1 - 3 m) of the earth—geothermal cooling system. It is known that majority of the households and the apartment complexes in India have two tanks for water storage. One is the underground water sump and the other is the overhead water tank. In our study, we use these two water storage systems for space cooling during summer and also for heating during winter. The main aim of our paper is air-conditioning of the space in an economic way to save electricity. It is based on a simple idea of transferring the low temperature from underground water sump to the room in the house using water as a mode of transport. Since India is a tropical country located at low latitude, most of the year, the air temperature is high and demands space cooling. However, for a couple of months during severe winter months (Dec.-Jan.) at Ahmedabad, heating of the space is required. For heating the space, we suggest to use the well-known solar water heater. Effective use of heat exchanger is shown through computation, modelling schemes and lab experiment. We recommend geothermal cooling for 10 months in a year and solar hot water system during 2 months of winter. It is observed that the ambient air temperature of 35°C - 40°C in the room can be brought down to 26°C without much consumption of electricity. In a similar manner, the room temperature at night (13°C) during winter in Ahmedabad can be increased to 27°C through circulation of water from solar water heater in the heat exchanger.展开更多
Electrochemical water splitting is one of the most reliable approaches for environmental-friendly hydrogen production.Because of their stability and abundance,Mn-based materials have been studied as electrocatalysts f...Electrochemical water splitting is one of the most reliable approaches for environmental-friendly hydrogen production.Because of their stability and abundance,Mn-based materials have been studied as electrocatalysts for the oxygen evolution reaction(OER),which is a more sluggish reaction in the water splitting system.To increase the OER activity of Mn,it is imperative to facilitate the structural change of Mn oxide to the active phase with Mn_(3)+species,known as the active site.Here,we present the relationship between the electronic conductivity in the catalyst layer and the formation of the Mn active phase,δ-MnO_(2),from wrinkled Mn(OH)_(2).Mn(OH)_(2) has poor conductivity,and it disrupts the oxidation reaction toward MnOOH orδ-MnO_(2).Adjacent conductive carbon to Mn(OH)_(2) enabled Mn(OH)_(2) to be oxidized toδ-MnO_(2).Furthermore,after repetitive cyclic voltammetry activation,the more conductive environment resulted in a higher density ofδ-MnO_(2) through the irreversible phase transition,and thus it contributes to the improvement of the OER activity.展开更多
The regulation and storage capacity of Poyang Lake is infl uenced by the fl ow from the main stream of the Yangtze River and the fi ve rivers in the Poyang Lake basin.After the operation of the Three Gorges Dam(TGD),h...The regulation and storage capacity of Poyang Lake is infl uenced by the fl ow from the main stream of the Yangtze River and the fi ve rivers in the Poyang Lake basin.After the operation of the Three Gorges Dam(TGD),hydrological changes in the main stream of the Yangtze River impact water exchange between the Yangtze River and Poyang Lake.Based on the analysis of measured data and factors infl uencing outfl ow at Hukou station,a new empirical formula describing outfl ow at Hukou station and critical water level for lake storage capacity is established.The change in monthly storage capacity of Poyang Lake before and after the construction of the TGD is analyzed quantitatively.The results show that the fl ows from the main stream of the Yangtze River and the fi ve rivers in the Poyang Lake basin affect outfl ow and water storage capacity by changing the water level difference between Xingzi and Hukou stations and by changing the water level at Hukou station.But the Yangtze River and the fi ve rivers in the Poyang Lake basin differ in process and degree.If the water level at Hukou station remains consistent,when the fl ow from the fi ver rivers increases by 1,000 m3/s,the outfl ow at Hukou station increases by 304 m3/s.When the fl ow from the main stream of the Yangtze River increases by 1,000 m3/s,the outfl ow at Hukou station decreases by 724 m3/s.In addition,the operation of the TGD affects the water storage capacity of Poyang Lake.The water volume of Poyang Lake decreases by 49.4%in September,but increases by 47.7%in May.展开更多
The impeded mass transfer rate by on-site-generated gas bubbles at both cathode and anode dramatically reduces the energy conversion efficiency of the proton exchange membrane water electrolyzer(PEMWE).Herein,we repor...The impeded mass transfer rate by on-site-generated gas bubbles at both cathode and anode dramatically reduces the energy conversion efficiency of the proton exchange membrane water electrolyzer(PEMWE).Herein,we report a surfactant-assistant method to accelerate the nano/micro-bubble detachment and the mass transfer rate by reducing the surface tension,resulting in an increase in overall efficiency.Four kinds of surfactants are studied in this work.Only potassium perfluorobutyl sulfonate(PPFBS),which has the structural similarity to Nafion,shows a significant promotion of activity and stability for both hygrogen evolution reaction(HER)and oxygen evolution reaction(OER)in the acidic medium at the high current density region.The HER overpotential at 0.1 A·cm−2 decreased 22%,and the current density at−0.4 V increased 31%by adding PPFBS.The promotion of overall efficiency by PPFBS on a homemade PEMWE was also proven.The reduced surface tension and electrostatic repulsion were the probable origins of the accelerated bubble detachment.展开更多
Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir d...Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.展开更多
基金supported by the National Key Research and Development Program of China(2022YFB4002100)the Key Program of the National Natural Science Foundation of China(22090032,22090030)。
文摘Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,particularly the presence of aggressive Cl^(-),has been proven to be prone to parasitic chloride ion oxidation and corrosion reactions,thus restricting seawater electrolyzer lifetime.Herein,hierarchical structure(Ni,Fe)O(OH)@NiCoS nanorod arrays(NAs)catalysts with heterointerfaces and localized oxygen vacancies were synthesized at nickel foam substrates via the combination of hydrothermal and annealing methods to boost seawater dissociation.The hiera rchical nanostructure of NiCoS NAs enhanced electrode charge transfer rate and active surface area to accelerate oxygen evolution reaction(OER)and generated sulfate gradient layers to repulsive aggressive Cl^(-).The fabricated heterostructure and vacancies of(Ni,Fe)O(OH)tuned catalyst electronic structure into an electrophilic state to enhance the binding affinity of hydroxyl intermediates and facilitate the structural transformation into amorphousγ-NiFeOOH for promoting OER.Furthermore,through operando electrochemistry techniques,we found that theγ-NiFeOOH possessing an unsaturated coordination environment and lattice-oxygen-participated OER mechanism can minimize electrode Cl^(-)corrosion enabled by stabilizing the adsorption of OH*intermediates,making it one of the best OER catalysts in the seawater medium reported to date.Consequently,these catalysts can deliver current densities of 100 and 500 mA cm-2for boosting OER at minimal overpotentials of 245and 316 mV,respectively,and thus prevent chloride ion oxidation simultaneously.Impressively,a highly stable anion exchange membrane(AEM)seawater electrolyzer based on the non-noble metal heterostructure electrodes reached a record low degradation rate under 100μV h-1at constant industrial current densities of 400 and 600 mA cm-2over 300 h,which exhibits a promising future for the nonprecious and stable AEMWE in the direct seawater electrolysis industry.
基金The Fund of Ministry of Science and Technology of China under contract No.2022YFC3105402the Natural Science Foundation of Fujian Province of China under contract No.2019J01020+1 种基金the National Natural Science Foundation of China under contract No.42141001the Fujian Provincial Central Guided Local Science and Technology Development Special Project under contract No.2022L3078.
文摘Mangrove and salt-marsh wetlands are important coastal carbon sinks.In order to quantify carbon export via pore water exchange and to evaluate subsequent fate of the exported carbon,we carried out continuous observations in a mangrove-Spartina alterniflora ecozone in the Zhangjiang River Estuary,China.The carbon fluxes via pore water exchange were estimated using^(222)Rn and^(228)Ra as tracers to be(2.15±0.63)mol/(m^(2)∙d)for dissolved inorganic carbon(DIC)and(-0.008±0.07)mol/(m^(2)∙d)for dissolved organic carbon(DOC)in the wet season and(3.02±0.65)mol/(m^(2)∙d)for DIC and(-0.15±0.007)mol/(m^(2)∙d)for DOC in the dry season in the mangrove-dominated creek(M-creek),while(2.52±0.82)mol/(m^(2)∙d)for DIC and(0.02±0.09)mol/(m^(2)∙d)for DOC in the dry season in the S.alterniflora-dominated creek(SA-creek).The negative value means that pore water was a sink of DOC in the creek.The total carbon via pore water exchange in the tidal creeks in the mangroves accounted for 41%-55%of the net carbon fixed by mangrove vegetation and was 3-4 times as much as the soil carbon accretion in the mangroves.The exported carbon in the form of DIC contributed all of the carbon outwelling from the M-creek and 79%of the carbon outwelling from the SA-creek,implying effective fixation of carbon by the wetland ecosystem.Moreover,it resulted in 54%in the dry season,75%in the wet season of the carbon dioxide released from the M-creek to the atmosphere,and 84%of the release from the SA-creek.Therefore,quantification of pore water exchange and related soil carbon loss is essential to trace the fate of carbon fixed in intertidal wetlands.
基金National Natural Science Foundation of China(Nos.52071231,51722103)the Natural Science Foundation of Tianjin(No.19JCJQJC61900)。
文摘Anion exchange membrane(AEM)electrolysis is a promising membrane-based green hydrogen production technology.However,AEM electrolysis still remains in its infancy,and the performance of AEM electrolyzers is far behind that of well-developed alkaline and proton exchange membrane electrolyzers.Therefore,breaking through the technical barriers of AEM electrolyzers is critical.On the basis of the analysis of the electrochemical performance tested in a single cell,electrochemical impedance spectroscopy,and the number of active sites,we evaluated the main technical factors that affect AEM electrolyzers.These factors included catalyst layer manufacturing(e.g.,catalyst,carbon black,and anionic ionomer)loadings,membrane electrode assembly,and testing conditions(e.g.,the KOH concentration in the electrolyte,electrolyte feeding mode,and operating temperature).The underlying mechanisms of the effects of these factors on AEM electrolyzer performance were also revealed.The irreversible voltage loss in the AEM electrolyzer was concluded to be mainly associated with the kinetics of the electrode reaction and the transport of electrons,ions,and gas-phase products involved in electrolysis.Based on the study results,the performance and stability of AEM electrolyzers were significantly improved.
基金This work is financially supported by National Natural Science Foundation of China(52174283 and 52274308)Innovation Fund Project for Graduate Student of China University of Petroleum(East China)(22CX04023A)the Fundamental Research Funds for the Central Universities。
文摘The formation of multiple oxygen intermediates supporting efficient oxygen evolution reaction(OER)are affinitive with hydroxyl adsorption.However,ability of the catalyst to capture hydroxyl and maintain the continuous supply at active sits remains a tremendous challenge.Herein,an affordable Ni2P/FeP2 heterostructure is presented to form the internal polarization field(IPF),arising hydroxyl spillover(HOSo)during OER.Facilitated by IPF,the oriented HOSo from FeP2 to Ni2P can activate the Ni site with a new hydroxyl transmission channel and build the optimized reaction path of oxygen intermediates for lower adsorption energy,boosting the OER activity(242 mV vs.RHE at 100 mA cm-2)for least 100 h.More interestingly,for the anion exchange membrane water electrolyzer(AEMWE)with low concentration electrolyte,the advantage of HOSo effect is significantly amplified,delivering 1 A cm^(-2)at a low cell voltage of 1.88 V with excellent stability for over 50 h.
基金supported by the National Natural Science Foundation of China(No.10702050)
文摘The water exchange matrix is an efficient tool to study the water exchange among the sub-areas in large-scale bays.The application of the random walk method to calculate the water exchange matrix is studied.Compared with the advection-diffusion model,the random walk model is more flexible to calculate the water exchange matrix. The forecast matrix suggested by Thompson et al.is used to evaluate the water exchange characteristics among the sub-areas fast.According to the theoretic analysis,it is found that the precision of the predicted results is mainly affected by three factors,namely, the particle number,the generated time of the forecast matrix,and the number of the sub-areas.The impact of the above factors is analyzed based on the results of a series of numerical tests.The results show that the precision of the forecast matrix increases with the increase of the generated time of the forecast matrix and the number of the particles. If there are enough particles in each sub-area,the precision of the forecast matrix will increase with the number of the sub-areas.Moreover,if the particles in each sub-area are not enough,the excessive number of the sub-areas can result in the decrease of the precision of the forecast matrix.
基金supported by the Fundamental Research Program of the Korean Institute of Materials Science(PNK7550)the National Research Council of Science&Technology(NST)grant by the MSIT(CAP21000-000)the New&Renewable Energy Core Technology Program of the KETEP(20213030040520)in the Republic of Korea。
文摘Anion exchange membrane(AEM)water electrolyzers are promising energy devices for the production of clean hydrogen from seawater.However,the lack of active and robust electrocatalysts for the oxygen evolution reaction(OER)severely impedes the development of this technology.In this study,a ternary layered double hydroxide(LDH)OER electrocatalyst(NiFeCo-LDH)is developed for high-performance AEM alkaline seawater electrolyzers.The AEM alkaline seawater electrolyzer catalyzed by the NiFeCo LDH shows high seawater electrolysis performance(0.84 A/cm^(2)at 1.7 Vcell)and high hydrogen production efficiency(77.6%at 0.5 A/cm^(2)),thus outperforming an electrolyzer catalyzed by a benchmark IrO_(2)electrocatalyst.The NiFeCo-LDH electrocatalyst greatly improves the kinetics of the AEM alkaline seawater electrolyzer,consequently reducing its activation loss and leading to high performance.Based on the results,this NiFeCo-LDH-catalyzed AEM alkaline seawater electrolyzer can likely surpass the energy conversion targets of the US Department of Energy.
基金Supported by the National Key R&D Program of China(No.2018YFE0103700)the National Natural Science Foundation(Nos.41876124,61871293,42007372)the Zhejiang Provincial Natural Science Foundation of China(Nos.LZ21C030001,LD21C030001,LQ20C030008)。
文摘For estuaries,inland lakes play a vital role in the ecological balance under the impact of tide s.The effect of tides-induced water exchange on phytoplankton community in a semi-closed lake was studied and compared with that of an adjacent closed lake in the Oujiang River mouth in Zhejiang,East China Sea,from June 29,2020 to June 14,2021.Results show that the dominant species,abundance,dominance,and diversity of the phytoplankton species between the two lakes were significantly different.In the closed lake,cyanobacteria were the dominant species during the study period.However.in the semi-closed lake,the diversification of the dominant species was greater,and some species of diatoms and green algae became dominant.The average phytoplankton abundance in the closed lake was 6 times of that in the semi-closed lake.The average dominance of cyanobacteria in the closed lake was 0.96,and those in the semi-closed lake and the Oujiang River were 0.51 and 0.22,respectively.Cyanobacterial blooms occurred throughout the study time in the closed lake but not in the semi-closed one.Furthermore,the species diversity richness of the phytoplankton in the semi-closed lake was higher than that of the closed one,and the phytoplankton community between the closed lake and semi-closed lake could be divided into distinctly different groups based on non-metic multidimensional scaling analysis(NMDS)and analysis of similarities(ANOSIM)analysis.The salinity of the water was significantly greater and the transparency significantly smaller in the semi-closed lake than those in the closed lake.Therefore,water exchange driven by local tidal movement increased salinity and decreased transparency of water,which consequently shaped the community structures of different phytoplankton and reduced the risk of a cyanobacterial bloom outbreak in the semi-closed lake.
基金The National Natural Science Foundation of China under contract Nos 41931182,41521005 and 41676016Guangdong Key Project under contract No.2019BT2H594+2 种基金the Key Special Project for Introduced Talents Team of Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)under contract Nos GML2019ZD0303 and GML2019ZD0304the Chinese Academy of Sciences under contract Nos ZDRW-XH-2019-2 and ISEE2018PY05the Independent Research Project Program of State Key Laboratory of Tropical Oceanography under contract Nos LTOZZ1902 and LTOZZ1802。
文摘The characteristics of the T/S structures,water mass exchange and deep circulation in the Andaman Sea are investigated based on the simulation from a high-resolution general circulation model(MITgcm).The results show that,below 1000 m,the water mass is saltier,warmer and more homogeneous in the Andaman Sea than that in the Bay of Bengal,attributing to the strong vertical mixing at the depth of^1800 m.The water mass exchange between the Andaman Sea and the Bay of Bengal goes through three major channels,which manifests itself as follows:the northern channel(Preparis Channel)is the main passage of water mass transport from the Bay of Bengal to the Andaman Sea,whereas the Middle Channel(the south of Andaman Islands and the north of Nicobar Islands)has an opposite transport;the southern channel(Great Channel)features with a four-layer water exchange which results in the least net transport among the three channels;all the transports through the three channels have an intra-annual variation with a period of half a year.At 1000-m depth,the entire Andaman Sea is occupied by a cyclonic circulation in January and July while by an anticyclonic one in April and October.The semiannual cycle found in both the deep circulation and water mass exchange is likely associated with the downwelling eastward-propagating Kelvin waves induced by the semiannual westerly component in the equatorial Indian Ocean during intermonsoon seasons.
基金the National Natural Science Foundation of China(NSFC)(Grant No.81873894,Grant No.21922410)Natural Science Foundation of Zhejiang Province,China(Grant No.LR20H180001,Grant No.LR19B050001)Taishan Scholars Program(No.tsqn20161070).
文摘Transmembrane water exchange(TWE)including transcytolemmal water exchange and transvascular water exchange is involved in many in vivo measurements and makes different contributions to the measuring results.In this study,we focus on the potential influence of TWE on the cell density parameter,intracellular water mole fraction pi,derived by dynamic contrast enhanced-magnetic resonance imaging(DCE-MRI)which has been reported as a technique to characterize perfusion and vascularization of tissues,but its accuracy in measuring cell density(or interstitial space)has been questioned.Sixteen patients with glioblastoma multiforme(GBM)were enrolled since GBM shows strong intratumor heterogeneity in both cell density and TWE.All the subjects were collected with DCE-MRI and apparent diffusion coefficient(ADC)map.The latter was considered as a valid surrogate of cell density.Extended Tofts(eTofts)model considering TWE as infinitely large variables and shutter-speed model(SSM)considering TWE as finite ones were used to fit DCE-MRI data.Monte Carlo(MC)and finite difference(FD)methods were used to simulate the influence of TWE on DCE-MRI-derived pi and ADC,respectively.The eTofts model shows a significant overestimation of pi in comparison with SSM in GBM(P<0.001),which is in accordance with MC simulations,and this overestimation shows dependence on the intra-to-extracellular water exchange rate constant(kio).Significant negative correlations between ADC and SSM-derived pi were found in both voxel-wise analyses(t-test P<0.001,average r=-0.74)and inter-subject comparisons(r=-0.63,P=0.009).But no consistent voxel-wise correlations(P>0.05)and a weaker inter-subject negative correlation(r=-0.56,P=0.02)were found between ADC and eTofts-derived pi.Further experimental and FD results revealed that kio made a limited contribution to ADC values in the physiological kio range in GBM,supporting ADC as a valid biomarker of cell density.These results suggest that the DCE-MRI pharmacokinetic shutter-speed model could significantly improve its accuracy in cell density estimation because of the considering transmembrane water exchange.
基金the Swedish Foundation for International Cooperation in Research and Higher Education(STINT),and the Swedish Research Council(Dnr 2022e04715).
文摘Water exchange between the different compartments of a heterogeneous specimen can be characterized via diffusion magnetic resonance imaging(dMRI).Many analysis frameworks using dMRI data have been proposed to describe exchange,often using a double diffusion encoding(DDE)stimulated echo sequence.Techniques such as diffusion exchange weighted imaging(DEWI)and the filter exchange and rapid exchange models,use a specific subset of the full space DDE signal.In this work,a general representation of the DDE signal was employed with different sampling schemes(namely constant b1,diagonal and anti-diagonal)from the data reduction models to estimate exchange.A near-uniform sampling scheme was proposed and compared with the other sampling schemes.The filter exchange and rapid exchange models were also applied to estimate exchange with their own subsampling schemes.These subsampling schemes and models were compared on both simulated data and experimental data acquired with a benchtop MR scanner.In synthetic data,the diagonal and near-uniform sampling schemes performed the best due to the consistency of their estimates with the ground truth.In experimental data,the shifted diagonal and near-uniform sampling schemes outperformed the others,yielding the most consistent estimates with the full space estimation.The results suggest the feasibility of measuring exchange using a general representation of the DDE signal along with variable sampling schemes.In future studies,algorithms could be further developed for the optimization of sampling schemes,as well as incorporating additional properties,such as geometry and diffusion anisotropy,into exchange frameworks.
基金supported by the KRISS(Korea Research Institute of Standards and Science)MPI Lab.program。
文摘The increasing demand for hydrogen energy to address environmental issues and achieve carbon neutrality has elevated interest in green hydrogen production,which does not rely on fossil fuels.Among various hydrogen production technologies,anion exchange membrane water electrolyzer(AEMWE)has emerged as a next-generation technology known for its high hydrogen production efficiency and its ability to use non-metal catalysts.However,this technology faces significant challenges,particularly in terms of the membrane durability and low ionic conductivity.To address these challenges,research efforts have focused on developing membranes with a new backbone structure and anion exchange groups to enhance durability and ionic conductivity.Notably,the super-acid-catalyzed condensation(SACC)synthesis method stands out due to its user convenience,the ability to create high molecular weight(MW)polymers,and the use of oxygen-tolerant organic catalysts.Although the synthesis of anion exchange membranes(AEMs)using the SACC method began in 2015,and despite growing interest in this synthesis approach,there remains a scarcity of review papers focusing on AEMs synthesized using the SACC method.The review covers the basics of SACC synthesis,presents various polymers synthesized using this method,and summarizes the development of these polymers,particularly their building blocks including aryl,ketone,and anion exchange groups.We systematically describe the effects of changes in the molecular structure of each polymer component,conducted by various research groups,on the mechanical properties,conductivity,and operational stability of the membrane.This review will provide insights into the development of AEMs with superior performance and operational stability suitable for water electrolysis applications.
基金funded by the Guangxi Natural Science Foundation(2018JJA150153)China Geological Survey Research Fund(JYYWF20180402)the project of China Geological Survey(DD20190342)。
文摘Due to the high heterogeneity and complexity of water flow movement for multiple karst water-bearing mediums,the evaluation,effective development,and utilization of karst water resources are significantly limited.Matrix flow is usually laminar,whereas conduit flow is usually turbulent.The driving mechanisms of water exchange that occur between the karst conduit and its adjacent matrix are not well understood.This paper investigates the hydrodynamic characteristics and the mechanism of flow exchange in dual water-bearing mediums(conduit and matrix)of karst aquifers through laboratory experimentation and numerical simulation.A karst aquifer consisting of a matrix network and a conduit was proposed,and the relationship between the water exchange flux and hydraulic head differences generated from the laboratory experiments was analyzed.Two modes of experimental tests were performed with different fixed water level boundaries in the laboratory karst aquifer.The results indicate that the water exchange capacity was proportional to the square root of hydraulic head differences.The linear exchange term in the conduit flow process(CFP)source program was modified according to experimental results.The modified CFP and the original CFP model experimental data results were compared,and it was found that the modified CFP model had better fitting effects.These results showed that the water exchange mechanism between conduit and matrix is very important for solid-liquid interface reaction,water resource evaluation,and understanding of karst hydrodynamic behavior.
基金supported by the National Natural Science Foundations of China (Grant Nos. 41930759, 41822501, 42075089, 41975014)the 2nd Scientific Expedition to the Qinghai-Tibet Plateau (2019QZKK0102)+3 种基金The Science and Technology Research Plan of Gansu Province (20JR10RA070)the Chinese Academy of Youth Innovation and Promotion, CAS (Y201874)the Youth Innovation Promotion Association CAS (QCH2019004)iLEAPs (Integrated Land Ecosystem-Atmosphere Processes Study-iLEAPS)。
文摘Thousands of lakes on the Tibetan Plateau(TP) play a critical role in the regional water cycle, weather, and climate. In recent years, the areas of TP lakes underwent drastic changes and have become a research hotspot. However, the characteristics of the lake-atmosphere interaction over the high-altitude lakes are still unclear, which inhibits model development and the accurate simulation of lake climate effects. The source region of the Yellow River(SRYR) has the largest outflow lake and freshwater lake on the TP and is one of the most densely distributed lakes on the TP. Since 2011,three observation sites have been set up in the Ngoring Lake basin in the SRYR to monitor the lake-atmosphere interaction and the differences among water-heat exchanges over the land and lake surfaces. This study presents an eight-year(2012–19), half-hourly, observation-based dataset related to lake–atmosphere interactions composed of three sites. The three sites represent the lake surface, the lakeside, and the land. The observations contain the basic meteorological elements,surface radiation, eddy covariance system, soil temperature, and moisture(for land). Information related to the sites and instruments, the continuity and completeness of data, and the differences among the observational results at different sites are described in this study. These data have been used in the previous study to reveal a few energy and water exchange characteristics of TP lakes and to validate and improve the lake and land surface model. The dataset is available at National Cryosphere Desert Data Center and Science Data Bank.
基金the National Natural Science Foundation of China(Nos.22171287,21901136,51972342,51972345,22105226,and 51872056)Taishan Scholar Project of Shandong Province(Nos.tsqn202103046 and ts20190922)+3 种基金Natural Science Foundation of Shandong Province(Nos.ZR2022QE175 and ZR2019ZD51)Fundamental Research Funds for the Central Universities(Nos.20CX06024A,22CX01002A-1,and 21CX06002A)China Postdoctoral Science Foundation(Nos.2019M650027 and 2019TQ0169)National Natural Science Foundation of Beijing(No.2204082),and Shandong Province Postdoctoral Innovative Talent Support Program(No.SDBX20200004).
文摘Platinum(Pt)-based electrocatalysts remain the only practical cathode catalysts for proton exchange membrane water electrolysis(PEMWE),due to their excellent catalytic activity for acidic hydrogen evolution reaction(HER),but are greatly limited by their low reserves and high cost.Here,we report an interfacial engineering strategy to obtain a promising low-Pt loading catalyst with atomically Pt-doped molybdenum carbide quantum dots decorated on conductive porous carbon(Pt-MoCx@C)for high-rate and stable HER in PEMWE.Benefiting from the strong interfacial interaction between Pt atoms and the ultra-small MoCx quantum dots substrate,the Pt-MoCx catalyst exhibits a high mass activity of 8.00 A·mgPt−1,5.6 times higher than that of commercial 20 wt.%Pt/C catalyst.Moreover,the strong interfacial coupling of Pt and MoCx substrate greatly improves the HER stability of the Pt-MoCx catalyst.Density functional theory studies further confirm the strong metal-support interaction on Pt-MoCx,the critical role of MoCx substrate in the stabilization of surface Pt atoms,as well as activation of MoCx substrate by Pt atoms for improving HER durability and activity.The optimized Pt-MoCx@C catalyst demonstrates>2000 h stability under a water-splitting current of 1000 mA·cm^(−2)when applied to the cathode of a PEM water electrolyzer,suggesting the potential for practical applications.
基金This work was supported by the Australian Research Council Discovery Projects(Grant Nos.ARC DP200103332 and ARC DP200103315).
文摘Proton exchangemembrane(PEM)water electrolysis represents one of the most promising technologies to achieve green hydrogen production,but currently its practical viability is largely affected by the slow reaction kinetics of the anodic oxygen evolution reaction(OER)in an acidic environment.While noble metal-based catalysts containing iridium or ruthenium are excellent catalysts for the acidic OER,their practical use in PEM electrolyzers is hindered due to their low abundance and high cost.Most recently,metal-organic frameworks(MOFs)have been demonstrated as a perfect platform to facilitate the design of acidic OER catalysts with both high efficiency and cost-effectiveness.Here,we pro-vide a timely and comprehensive overview of the recent progress on MOF-based acidic OER catalysts.The fundamental mechanisms of the acidic OER are first introduced,followed by a summary of the development of pristine MOFs and MOF derivatives as acidic OER catalysts.Importantly,a number of catalyst design strategies are discussed aiming at improving the acidic OER catalytic per-formance of MOF-based candidates.The integration of MOF-based catalysts into real PEM water electrolyzers is also included.Finally,future research directions are provided to achieve better MOF-based catalysts operational in acidic envi-ronments and PEM devices.
文摘It is well known that one unit of electrical energy saved is equal to more than two units produced. One way of economizing the power is utilization of energy efficient systems at all locations. In the present study, the air conditioning system is analysed and an innovative way is suggested. We use natural low temperature of shallow sub surface (1 - 3 m) of the earth—geothermal cooling system. It is known that majority of the households and the apartment complexes in India have two tanks for water storage. One is the underground water sump and the other is the overhead water tank. In our study, we use these two water storage systems for space cooling during summer and also for heating during winter. The main aim of our paper is air-conditioning of the space in an economic way to save electricity. It is based on a simple idea of transferring the low temperature from underground water sump to the room in the house using water as a mode of transport. Since India is a tropical country located at low latitude, most of the year, the air temperature is high and demands space cooling. However, for a couple of months during severe winter months (Dec.-Jan.) at Ahmedabad, heating of the space is required. For heating the space, we suggest to use the well-known solar water heater. Effective use of heat exchanger is shown through computation, modelling schemes and lab experiment. We recommend geothermal cooling for 10 months in a year and solar hot water system during 2 months of winter. It is observed that the ambient air temperature of 35°C - 40°C in the room can be brought down to 26°C without much consumption of electricity. In a similar manner, the room temperature at night (13°C) during winter in Ahmedabad can be increased to 27°C through circulation of water from solar water heater in the heat exchanger.
基金supported by the National R&D Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(NRF-2021K1A4A8A01079455)supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)granted financial resource from the Ministry of Trade,Industry&Energy,Republic of Korea(No.20213030040590)。
文摘Electrochemical water splitting is one of the most reliable approaches for environmental-friendly hydrogen production.Because of their stability and abundance,Mn-based materials have been studied as electrocatalysts for the oxygen evolution reaction(OER),which is a more sluggish reaction in the water splitting system.To increase the OER activity of Mn,it is imperative to facilitate the structural change of Mn oxide to the active phase with Mn_(3)+species,known as the active site.Here,we present the relationship between the electronic conductivity in the catalyst layer and the formation of the Mn active phase,δ-MnO_(2),from wrinkled Mn(OH)_(2).Mn(OH)_(2) has poor conductivity,and it disrupts the oxidation reaction toward MnOOH orδ-MnO_(2).Adjacent conductive carbon to Mn(OH)_(2) enabled Mn(OH)_(2) to be oxidized toδ-MnO_(2).Furthermore,after repetitive cyclic voltammetry activation,the more conductive environment resulted in a higher density ofδ-MnO_(2) through the irreversible phase transition,and thus it contributes to the improvement of the OER activity.
基金National Key R&D Program of China(2018YFC0407201).
文摘The regulation and storage capacity of Poyang Lake is infl uenced by the fl ow from the main stream of the Yangtze River and the fi ve rivers in the Poyang Lake basin.After the operation of the Three Gorges Dam(TGD),hydrological changes in the main stream of the Yangtze River impact water exchange between the Yangtze River and Poyang Lake.Based on the analysis of measured data and factors infl uencing outfl ow at Hukou station,a new empirical formula describing outfl ow at Hukou station and critical water level for lake storage capacity is established.The change in monthly storage capacity of Poyang Lake before and after the construction of the TGD is analyzed quantitatively.The results show that the fl ows from the main stream of the Yangtze River and the fi ve rivers in the Poyang Lake basin affect outfl ow and water storage capacity by changing the water level difference between Xingzi and Hukou stations and by changing the water level at Hukou station.But the Yangtze River and the fi ve rivers in the Poyang Lake basin differ in process and degree.If the water level at Hukou station remains consistent,when the fl ow from the fi ver rivers increases by 1,000 m3/s,the outfl ow at Hukou station increases by 304 m3/s.When the fl ow from the main stream of the Yangtze River increases by 1,000 m3/s,the outfl ow at Hukou station decreases by 724 m3/s.In addition,the operation of the TGD affects the water storage capacity of Poyang Lake.The water volume of Poyang Lake decreases by 49.4%in September,but increases by 47.7%in May.
基金This work was supported by the National Natural Science Foundation of China(Nos.21971008 and 22101016)Fundamental Research Funds for the Central Universities(buctrc201916,buctrc201823)China Petroleum&Chemical Corporation(SINOPEC,120052-2).
文摘The impeded mass transfer rate by on-site-generated gas bubbles at both cathode and anode dramatically reduces the energy conversion efficiency of the proton exchange membrane water electrolyzer(PEMWE).Herein,we report a surfactant-assistant method to accelerate the nano/micro-bubble detachment and the mass transfer rate by reducing the surface tension,resulting in an increase in overall efficiency.Four kinds of surfactants are studied in this work.Only potassium perfluorobutyl sulfonate(PPFBS),which has the structural similarity to Nafion,shows a significant promotion of activity and stability for both hygrogen evolution reaction(HER)and oxygen evolution reaction(OER)in the acidic medium at the high current density region.The HER overpotential at 0.1 A·cm−2 decreased 22%,and the current density at−0.4 V increased 31%by adding PPFBS.The promotion of overall efficiency by PPFBS on a homemade PEMWE was also proven.The reduced surface tension and electrostatic repulsion were the probable origins of the accelerated bubble detachment.
基金supported by the National Key R&D Program of China(No.2022YFB4002000)the National Natural Science Foundation of China(No.22232004)+2 种基金the Strategic priority research program of CAS(No.XDA21090400)the Jilin Province Science and Technology Development Program(NOs.20210301008GX and 20210502002ZP)the Jilin Province Development and Reform Commission Program(No.2023C032-6).
文摘Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined strategy.The optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic activity.The high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd motifs.Moreover,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.