The atmospheric carbon dioxide(CO_(2))concentration has been increasing rapidly since the Industrial Revolution,which has led to unequivocal global warming and crucial environmental change.It is extremely important to...The atmospheric carbon dioxide(CO_(2))concentration has been increasing rapidly since the Industrial Revolution,which has led to unequivocal global warming and crucial environmental change.It is extremely important to investigate the interactions among atmospheric CO_(2),the physical climate system,and the carbon cycle of the underlying surface for a better understanding of the Earth system.Earth system models are widely used to investigate these interactions via coupled carbon-climate simulations.The Chinese Academy of Sciences Earth System Model version 2(CAS-ESM2.0)has successfully fixed a two-way coupling of atmospheric CO_(2)with the climate and carbon cycle on land and in the ocean.Using CAS-ESM2.0,we conducted a coupled carbon-climate simulation by following the CMIP6 proposal of a historical emissions-driven experiment.This paper examines the modeled CO_(2)by comparison with observed CO_(2)at the sites of Mauna Loa and Barrow,and the Greenhouse Gases Observing Satellite(GOSAT)CO_(2)product.The results showed that CAS-ESM2.0 agrees very well with observations in reproducing the increasing trend of annual CO_(2)during the period 1850-2014,and in capturing the seasonal cycle of CO_(2)at the two baseline sites,as well as over northern high latitudes.These agreements illustrate a good ability of CAS-ESM2.0 in simulating carbon-climate interactions,even though uncertainties remain in the processes involved.This paper reports an important stage of the development of CAS-ESM with the coupling of carbon and climate,which will provide significant scientific support for climate research and China’s goal of carbon neutrality.展开更多
Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance...Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).展开更多
A novel color image encryption scheme is developed to enhance the security of encryption without increasing the complexity. Firstly, the plain color image is decomposed into three grayscale plain images, which are con...A novel color image encryption scheme is developed to enhance the security of encryption without increasing the complexity. Firstly, the plain color image is decomposed into three grayscale plain images, which are converted into the frequency domain coefficient matrices(FDCM) with discrete cosine transform(DCT) operation. After that, a twodimensional(2D) coupled chaotic system is developed and used to generate one group of embedded matrices and another group of encryption matrices, respectively. The embedded matrices are integrated with the FDCM to fulfill the frequency domain encryption, and then the inverse DCT processing is implemented to recover the spatial domain signal. Eventually,under the function of the encryption matrices and the proposed diagonal scrambling algorithm, the final color ciphertext is obtained. The experimental results show that the proposed method can not only ensure efficient encryption but also satisfy various sizes of image encryption. Besides, it has better performance than other similar techniques in statistical feature analysis, such as key space, key sensitivity, anti-differential attack, information entropy, noise attack, etc.展开更多
AIM: To elucidate the mechanisms of mesenteric vasodilation in portal hypertension (PHT), with a focus on endothelin signaling. METHODS: PHT was induced in rats by common bile duct ligation (CBDL). Portal pressure (PP...AIM: To elucidate the mechanisms of mesenteric vasodilation in portal hypertension (PHT), with a focus on endothelin signaling. METHODS: PHT was induced in rats by common bile duct ligation (CBDL). Portal pressure (PP) was measured directly via catheters placed in the portal vein tract. The level of endothelin-1 (ET-1) in the mesenteric circulation was determined by radioimmunoassay, and the expression of the endothelin A receptor (ETAR) and endothelin B receptor (ETBR) was assessed by immunofluorescence and Western blot. Additionally, expression of G protein coupled kinase-2 (GRK2) and β-arrestin 2, which influence endothelin receptor sensitivity, were also studied by Western blot. RESULTS: PP of CBDL rats increased significantly (11.89 ± 1.38 mmHg vs 16.34 ± 1.63 mmHg). ET-1 expression decreased in the mesenteric circulation 2 and 4 wk after CBDL. ET-1 levels in the systemic circulation of CBDL rats were increased at 2 wk and decreased at 4 wk. There was no change in ETAR expression in response to CBDL; however, increased expression of ETBR in the endothelial cells of mesenteric arterioles and capillaries was observed. In sham-operated rats, ETBR was mainly expressed in the CD31+ endothelial cells of the arterioles. With development of PHT, in addition to the endothelial cells, ETBR expression was noticeably detectable in the SMA+ smooth muscle cells of arterioles and in the CD31+ capillaries. Following CBDL, increased expression of GRK2 was also found in mesenteric tissue, though there was no change in the level of β-arrestin 2. CONCLUSION: Decreased levels of ET-1 and increased ETBR expression in the mesenteric circulation following CBDL in rats may underlie mesenteric vasodilation in individuals with PHT. Mechanistically, increased GRK2 expression may lead to desensitization of ETAR, as well as other vasoconstrictors, promoting this vasodilatory effect.展开更多
Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of...Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.展开更多
In order to consider the influence of temperature and underground water movement, an elastoplastic model and a 2D FEM stress fields on the migration of radioactive nuclide with code for analysis of coupled thermo-hyd...In order to consider the influence of temperature and underground water movement, an elastoplastic model and a 2D FEM stress fields on the migration of radioactive nuclide with code for analysis of coupled thermo-hydro-mechanical (THM) processes in saturated and unsaturated porous media were extended and improved through introducing the percolation and migration equation, so that the code can be used for solving the temperature field, flow field, stress field and nuclide concentration field simultaneously. The states of temperatures, pore pressures and nuclide concentrations in the near field of a hypothetical nuclear waste repository were investigated. The influence of the half life of the radioactive nuclide on the temporal change of nuclide concentration was analyzed considering the thermo-hydro-mechanical-migratory coupling. The results show that, at the boundary of the vitrified waste, the concentration of radioactive nuclide with a half life of 10 a falls after a period of rising, with the maximum value of 0.182 mol/m3 and the minimum value of 0.181 mol/m^3 at the end of computation. For a half life of 1 000 a, the concentration of radioactive nuclide always increases with the increase of the time during the computation period; and the maximum value is 1.686 mol/m^3 at the end of the computation. Therefore, under the condition of THM coupling, the concentration of radioactive nuclide with a shorter half life will decrease more quickly with water flow; but for the radioactive nuclide with a longer half life, its concentration will keep at a higher level for a longer time in the migration process.展开更多
In this study, the coupled heave-pitch motion equations of a spar platform were established by considering lst-order and 2nd-order random wave loads and the effects of time-varying displacement volume and transient wa...In this study, the coupled heave-pitch motion equations of a spar platform were established by considering lst-order and 2nd-order random wave loads and the effects of time-varying displacement volume and transient wave elevation. We generated random wave loads based on frequency-domain wave load transfer functions and the Joint North Sea Wave Project (JONSWAP) wave spectrum, designed program codes to solve the motion equations, and then simulated the coupled heave-pitch motion responses of the platform in the time domain. We then calculated and compared the motion responses in different sea conditions and separately investigated the effects of 2nd-order random wave loads and transient wave elevation. The results show that the coupled heave-pitch motion responses of the platform are primarily dominated by wave height and the characteristic wave period, the latter of which has a greater impact. 2nd-order mean wave loads mainly affect the average heave value. The platform's pitch increases after the 2nd-order low frequency wave loads are taken into account. The platform's heave is underestimated if the transient wave elevation term in the motion equations is neglected.展开更多
Cobalt-based oxides,with high abundance,good stability and excellent catalytic performance,are regarded as promising photocatalysts for artificial photosynthetic systems to alleviate foreseeable energy shortages and g...Cobalt-based oxides,with high abundance,good stability and excellent catalytic performance,are regarded as promising photocatalysts for artificial photosynthetic systems to alleviate foreseeable energy shortages and global warming.Herein,for the first time,a series of novel spongy porous CDs@CoOx materials were synthesized to act as an efficient and stable bifunctional photocatalyst for water oxidation and CO2 reduction.Notably,the preparation temperatures visibly influence the morphologies and photocatalytic performances of the CDs@CoOx.Under the optimal conditions,a maximum O2 yield of 40.4% and pretty apparent quantum efficiency(AQE)of 58.6% at 460 nm were obtained over CDs@CoOx-300 for water oxidation.Similarly,the optimized sample CDs@CoOx-300 manifests significant enhancement on the CO2-to-CO conversion with a high selectivity of 89.3% and CO generation rate of 8.1μmol/h,which is superior to most previous cobalt-based catalysts for CO2 reduction.The composite CDs@CoOx-300 not only exposes more active sites but also facilitates electron transport,which results in excellent photocatalytic activity.In addition,the boosted photocatalytic behavior is attributed to the synergistic effect between CoOx and CDs,which was verified by the photocatalytic activity control experiments and electrochemical characterization.The work offers a novel strategy to fabricate a high performance bifunctional photocatalyst for water oxidation and CO2 reduction.展开更多
Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled inte...Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled interface constructed betweenα-MnO2 and Co3O4 is responsible for the enhanced catalytic activity.The resultantα-MnO2@Co3O4 catalyst exhibits excellent catalytic activity at a T90%(temperature required to achieve a toluene conversion of 90%)of approximately 229℃,which is 47 and 28℃ lower than those of the pureα-MnO2 nanowire and Co3O4-b obtained via pyrolysis of ZIF-67,respectively.This activity is attributed to the increase in the number of surface-adsorbed oxygen species,which accelerate the oxygen mobility and enhance the redox pairs of Mn^4+/Mn^3+ and Co^2+/Co^3+.Moreover,the result of in situ diffuse reflectance infrared Fourier transform spectroscopy suggests that the gaseous oxygen could be more easily activated to adsorbed oxygen species on the surface of α-MnO2@Co3O4 than on that of α-MnO2.The catalytic reaction route of toluene oxidation over theα-MnO2@Co3O4 catalyst is as follows:toluene→benzoate species→alkanes containing oxygen functional group→CO2 and H2O.In addition,the α-MnO2@Co3O4 catalyst shows excellent stability and good water resistance for toluene oxidation.Furthermore,the preparation method can be extended to other 1D MnO2 materials.A new strategy for the development of high-performance catalysts of practical significance is provided.展开更多
Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a...Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.展开更多
Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(...Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.展开更多
Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)...Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.展开更多
High qualityβ-Ga_(2)O_(3)single crystal nanobelts with length of 2−3 mm and width from tens of microns to 132μm were synthesized by carbothermal reduction method.Based on the grown nanobelt with the length of 600μm...High qualityβ-Ga_(2)O_(3)single crystal nanobelts with length of 2−3 mm and width from tens of microns to 132μm were synthesized by carbothermal reduction method.Based on the grown nanobelt with the length of 600μm,the dual-Schottky-junctions coupling device(DSCD)was fabricated.Due to the electrically floating Ga_(2)O_(3)nanobelt region coupling with the double Schottky-junctions,the current I_(S2)increases firstly and rapidly reaches into saturation as increase the voltage V_(S2).The saturation current is about 10 pA,which is two orders of magnitude lower than that of a single Schottky-junction.In the case of solar-blind ultraviolet(UV)light irradiation,the photogenerated electrons further aggravate the coupling physical mechanism in device.I_(S2)increases as the intensity of UV light increases.Under the UV light of 1820μW/cm^(2),I_(S2)quickly enters the saturation state.At V_(S2)=10 V,photo-to-dark current ratio(PDCR)of the device reaches more than 104,the external quantum efficiency(EQE)is 1.6×10^(3)%,and the detectivity(D*)is 7.5×10^(12)Jones.In addition,the device has a very short rise and decay times of 25−54 ms under different positive and negative bias.DSCD shows unique electrical and optical control characteristics,which will open a new way for the application of nanobelt-based devices.展开更多
Integrating selective organic synthesis with hydrogen(H_(2))evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes ...Integrating selective organic synthesis with hydrogen(H_(2))evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes towards efficient production of solar fuels and chemicals.In this work,a facile one‐pot oil bath method has been proposed to fabricate a noble metal‐free ultrathin Ni‐doped ZnIn_(2)S_(4)(ZIS/Ni)composite nanosheet for effective solar‐driven selective dehydrocoupling of benzyl alcohol into value‐added C–C coupled hydrobenzoin and H_(2) fuel,which exhibits higher performance than pure ZIS nanosheet.The remarkably improved photoredox activity of ZIS/Ni is mainly attributed to the optimized electron structure featuring narrower band gap and suitable energy band position,which facilitates the ability of light harvesting and photoexcited charge carrier separation and transfer.Furthermore,it has been demonstrated that it is feasible to employ ZIS/Ni for various aromatic alcohols dehydrocoupling to the corresponding C–C coupled products.It is expected that this work can stimulate further interest on the establishment of innovative photocatalytic redox platform coupling clean solar fuels synthesis and selective organic conversion in a sustainable manner.展开更多
The development of highly active,selective,and stable electrocatalysts can facilitate the effective implementation of electrocatalytic CO_(2)conversion into fuels or chemicals for mitigating the energy crisis and clim...The development of highly active,selective,and stable electrocatalysts can facilitate the effective implementation of electrocatalytic CO_(2)conversion into fuels or chemicals for mitigating the energy crisis and climate problems.Therefore,it is necessary to achieve the goal through reasonable material design based on the actuality of the operational active site at the molecular scale.Inspired by the stimulating synergistic effect of coupled heteronuclear metal atoms,a novel Ni-Co atomic pairs configuration(denoted as NiN_(3)?CoN_(3)-NC)active site was theoretically screened out for improving electrochemical CO_(2)reduction reaction(CO_(2)RR).The structure of NiN_(3)?CoN_(3)-NC was finely regulated by adjusting Zn content in the precursors Zn/Co/Ni-zeolite imidazolate frameworks(Zn/Co/Ni-ZIFs)and pyrolysis temperature.The structural features of NiN_(3)?CoN_(3)-NC were systematically confirmed by aberration-corrected HAADF-STEM coupled with 3D atom-overlapping Gaussian-function fitting mapping,XAFS,and XRD.The results of theoretical calculations reveal that the synergistic effect of Ni-Co atomic pairs can effectively promote the*COOH intermediate formation and thus the overall CO_(2)RR kinetic was improved,and also restrained the competitive hydrogen evolution reaction.Due to the attributes of Ni-Co atomic pairs configuration,the developed NiN_(3)?CoN_(3)-NC with superior catalytic activity,selectivity,and durability,with a high turnover frequency of 2265 h^(-1)at-1.1 V(vs.RHE)and maximum Faradaic efficiency of 97.7%for CO production.This work demonstrates the great potential of DACs as highly efficient catalysts for CO_(2)RR,provides a useful strategy to design heteronuclear DACs,exploits the synergistic effect of multiple metal sites to facilitate complex CO_(2)RR catalytic reactions,and inspires more efforts to develop the potential of DACs in various fields.展开更多
As one of the most important ways to reduce the greenhouse gas emission,carbon dioxide(CO2)enhanced gas recovery(CO2-EGR) is attractive since the gas recovery can be enhanced simultaneously with CO2sequestration.B...As one of the most important ways to reduce the greenhouse gas emission,carbon dioxide(CO2)enhanced gas recovery(CO2-EGR) is attractive since the gas recovery can be enhanced simultaneously with CO2sequestration.Based on the existing equation of state(EOS) module of TOUGH2 MP,extEOS7C is developed to calculate the phase partition of H2O-CO2-CH4-NaCl mixtures accurately with consideration of dissolved NaCI and brine properties at high pressure and temperature conditions.Verifications show that it can be applied up to the pressure of 100 MPa and temperature of 150℃.The module was implemented in the linked simulator TOUGH2MP-FLAC3 D for the coupled hydro-mechanical simulations.A simplified three-dimensional(3D)1/4 model(2.2 km×1 km×1 km) which consists of the whole reservoir,caprock and baserock was generated based on the geological conditions of a gas field in the North German Basin.The simulation results show that,under an injection rate of 200,000 t/yr and production rate of 200,000 sm3/d,CO2breakthrough occurred in the case with the initial reservoir pressure of 5 MPa but did not occur in the case of 42 MPa.Under low pressure conditions,the pressure driven horizontal transport is the dominant process;while under high pressure conditions,the density driven vertical flow is dominant.Under the considered conditions,the CO2-EGR caused only small pressure changes.The largest pore pressure increase(2 MPa) and uplift(7 mm) occurred at the caprock bottom induced by only CO2injection.The caprock had still the primary stress state and its integrity was not affected.The formation water salinity and temperature variations of ±20℃ had small influences on the CO2-EGR process.In order to slow down the breakthrough,it is suggested that CO2-EGR should be carried out before the reservoir pressure drops below the critical pressure of CO2.展开更多
The ablation of ultra-high-temperature ceramics(UTHCs)is a complex physicochemical process including mechanical behavior,temperature effect,and chemical reactions.In order to realize the structural optimization and fu...The ablation of ultra-high-temperature ceramics(UTHCs)is a complex physicochemical process including mechanical behavior,temperature effect,and chemical reactions.In order to realize the structural optimization and functional design of ultra-high temperature ceramics,a coupled thermo-chemo-mechanical bond-based peridynamics(PD)model is proposed based on the ZrB_(2) ceramics oxidation kinetics model and coupled thermomechanical bond-based peridynamics.Compared with the traditional coupled thermo-mechanical model,the proposedmodel considers the influenceof chemical reactionprocessonthe ablation resistanceof ceramicmaterials.In order to verify the reliability of the proposed model,the thermo-mechanical coupling model,damage model and oxidation kinetic model are established respectively to investigate the applicability of the proposedmodel proposed in dealing with thermo-mechanical coupling,crack propagation,and chemical reaction,and the results show that the model is reliable.Finally,the coupled thermo-mechanical model and coupled thermo-chemo-mechanical model are used to simulate the crack propagation process of the plate under the thermal shock load,and the results show that the oxide layer plays a good role in preventing heat transfer and protecting the internal materials.Based on the PD fully coupled thermo-mechanical model,this paper innovatively introduces the oxidation kinetic model to analyze the influence of parameter changes caused by oxide layer growth and chemical growth strain on the thermal protection ability of ceramics.The proposed model provides an effective simulation technology for the structural design of UTHCs.展开更多
In this paper, a coupled model was used to estimate the responses of soil moisture and net primary production of vegetation(NPP) to increasing atmospheric CO2 concentration and climate change. The analysis uses three ...In this paper, a coupled model was used to estimate the responses of soil moisture and net primary production of vegetation(NPP) to increasing atmospheric CO2 concentration and climate change. The analysis uses three experiments simulated by the second-generation Earth System Model(CanESM2) of the Canadian Centre for Climate Modelling and Analysis(CCCma), which are part of the phase 5 of the Coupled Model Intercomparison Project(CMIP5). The authors focus on the magnitude and evolution of responses in soil moisture and NPP using simulations modeled by CanESM, in which the individual effects of increasing CO2 concentration and climate change and their combined effect are separately accounted for. When considering only the single effect of climate change, the soil moisture and NPP have a linear trend of 0.03 kg m–2 yr–1 and –0.14 gC m–2 yr–2, respectively. However, such a reduction in the global NPP results from the decrease of NPP at lower latitudes and in the Southern Hemisphere, although increased NPP has been shown in high northern latitudes. The largest negative trend is located in the Amazon basin at –1.79 gC m–2 yr–2. For the individual effect of increasing CO2 concentration, both soil moisture and NPP show increases, with an elevated linear trend of 0.02 kg m–2 yr–1 and 0.84 gC m–2 yr–2, respectively. Most regions show an increasing NPP, except Alaska. For the combined effect of increasing atmospheric CO2 and climate change, the increased soil moisture and NPP exhibit a linear trend of 0.04 kg m–2 yr–1 and 0.83 gC m–2 yr–2 at a global scale. In the Amazon basin, the higher reduction in soil moisture is illustrated by the model, with a linear trend of –0.39 kg m–2 yr–1, for the combined effect. Such a change in soil moisture is caused by a weakened Walker circulation simulated by this coupled model, compared with the single effect of increasing CO2 concentration(experiment M2), and a consequence of the reduction in NPP is also shown in this area, with a linear trend of-0.16 gC m-2 yr-2.展开更多
Dilatancy-controlled gas flow in preferential pathways plays a key role in the safety analysis of radioactive waste repositories.This is particularly the case for bentonite,an often-preferred barrier material.Gas flow...Dilatancy-controlled gas flow in preferential pathways plays a key role in the safety analysis of radioactive waste repositories.This is particularly the case for bentonite,an often-preferred barrier material.Gas flow in preferential pathways is characterized by localization and spontaneous behavior,which is challenging to simulate in numerical models due to strong hydro-mechanical coupling.To analyze a laboratory experiment in the framework of the DECOVALEX-2023 project,this study introduced a new approach of combining continuous modelling methods with spatial material properties derived from material heterogeneities and experimental observations.The proposed model utilized hydro-mechanical spatial distributions,namely Young’s modulus and gas entry pressure,and elastoplasticity combined with a linear swelling model.A conceptual strain-dependent permeability approach simulated dilatancycontrolled gas flow based on hydro-mechanical coupling.To test the effectiveness of the presented approach,a gas injection test in a compacted,saturated bentonite sample was simulated using the opensource code OpenGeoSys 5.8 and compared with experimental observations.The presented methodology is capable of simulating localized gas flow in preferential pathways.The spatial distributions of Young’s modulus and gas entry pressure affect the swelling pressure,relative permeability and,in combination with the strain-dependent permeability model,also the intrinsic permeability.展开更多
In this study, 1D and 2D shallow-water models were coupled to simulate unsteady flow in channel networks and embayment. The 1D model solved the 1D shallow-water equations (St. Venant) using the Preissmann box method a...In this study, 1D and 2D shallow-water models were coupled to simulate unsteady flow in channel networks and embayment. The 1D model solved the 1D shallow-water equations (St. Venant) using the Preissmann box method and targeted long narrow reaches of the river networks, while the 2D model targeted broad channels and embayment and solved the 2D shallow-water equations using a semi-implicit scheme applied to an unstructured grid of triangular cells. The 1D and 2D models were solved simultaneously by building a matrix for the free surface elevation at every 1D junction and 2D cell center. Velocities were then computed explicitly based on the results at the previous time step and the updated water level. The originality of the scheme arose from a novel coupling method. The results showed that the coupled 1D/2D model produced identical results as the full 2D model in classical to benchmark problems with considerable savings in computational effort. Application of the model to the Pearl River Estuary in southern China showed that complex patterns of tidal wave propagation could be efficiently modeled.展开更多
基金the National Key Research and Development Program of China(Grant No.2022YFE0106500)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Grant No.2022076)+1 种基金the National Key Scientific and Technological Infrastructure project“Earth System Numerical Simulation Facility”(EarthLab2023-EL-ZD-00012)。
文摘The atmospheric carbon dioxide(CO_(2))concentration has been increasing rapidly since the Industrial Revolution,which has led to unequivocal global warming and crucial environmental change.It is extremely important to investigate the interactions among atmospheric CO_(2),the physical climate system,and the carbon cycle of the underlying surface for a better understanding of the Earth system.Earth system models are widely used to investigate these interactions via coupled carbon-climate simulations.The Chinese Academy of Sciences Earth System Model version 2(CAS-ESM2.0)has successfully fixed a two-way coupling of atmospheric CO_(2)with the climate and carbon cycle on land and in the ocean.Using CAS-ESM2.0,we conducted a coupled carbon-climate simulation by following the CMIP6 proposal of a historical emissions-driven experiment.This paper examines the modeled CO_(2)by comparison with observed CO_(2)at the sites of Mauna Loa and Barrow,and the Greenhouse Gases Observing Satellite(GOSAT)CO_(2)product.The results showed that CAS-ESM2.0 agrees very well with observations in reproducing the increasing trend of annual CO_(2)during the period 1850-2014,and in capturing the seasonal cycle of CO_(2)at the two baseline sites,as well as over northern high latitudes.These agreements illustrate a good ability of CAS-ESM2.0 in simulating carbon-climate interactions,even though uncertainties remain in the processes involved.This paper reports an important stage of the development of CAS-ESM with the coupling of carbon and climate,which will provide significant scientific support for climate research and China’s goal of carbon neutrality.
基金the National Science Fund for Distinguished Young Scholars(Grant No.52125103)the National Natural Science Foundation of China(Grant Nos.52301232,52071041,12074048,and 12147102)China Postdoctoral Science Foundation(Grant No.2022M720552).
文摘Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).
基金Project supported by the National Natural Science Foundation of China(Grant Nos.62105004 and 52174141)the College Student Innovation and Entrepreneurship Fund Project(Grant No.202210361053)+1 种基金Anhui Mining Machinery and Electrical Equipment Coordination Innovation Center,Anhui University of Science&Technology(Grant No.KSJD202304)the Anhui Province Digital Agricultural Engineering Technology Research Center Open Project(Grant No.AHSZNYGC-ZXKF021)。
文摘A novel color image encryption scheme is developed to enhance the security of encryption without increasing the complexity. Firstly, the plain color image is decomposed into three grayscale plain images, which are converted into the frequency domain coefficient matrices(FDCM) with discrete cosine transform(DCT) operation. After that, a twodimensional(2D) coupled chaotic system is developed and used to generate one group of embedded matrices and another group of encryption matrices, respectively. The embedded matrices are integrated with the FDCM to fulfill the frequency domain encryption, and then the inverse DCT processing is implemented to recover the spatial domain signal. Eventually,under the function of the encryption matrices and the proposed diagonal scrambling algorithm, the final color ciphertext is obtained. The experimental results show that the proposed method can not only ensure efficient encryption but also satisfy various sizes of image encryption. Besides, it has better performance than other similar techniques in statistical feature analysis, such as key space, key sensitivity, anti-differential attack, information entropy, noise attack, etc.
基金Supported by Grant from National Key New Drug Creation Project of China, No. 2009ZX09102
文摘AIM: To elucidate the mechanisms of mesenteric vasodilation in portal hypertension (PHT), with a focus on endothelin signaling. METHODS: PHT was induced in rats by common bile duct ligation (CBDL). Portal pressure (PP) was measured directly via catheters placed in the portal vein tract. The level of endothelin-1 (ET-1) in the mesenteric circulation was determined by radioimmunoassay, and the expression of the endothelin A receptor (ETAR) and endothelin B receptor (ETBR) was assessed by immunofluorescence and Western blot. Additionally, expression of G protein coupled kinase-2 (GRK2) and β-arrestin 2, which influence endothelin receptor sensitivity, were also studied by Western blot. RESULTS: PP of CBDL rats increased significantly (11.89 ± 1.38 mmHg vs 16.34 ± 1.63 mmHg). ET-1 expression decreased in the mesenteric circulation 2 and 4 wk after CBDL. ET-1 levels in the systemic circulation of CBDL rats were increased at 2 wk and decreased at 4 wk. There was no change in ETAR expression in response to CBDL; however, increased expression of ETBR in the endothelial cells of mesenteric arterioles and capillaries was observed. In sham-operated rats, ETBR was mainly expressed in the CD31+ endothelial cells of the arterioles. With development of PHT, in addition to the endothelial cells, ETBR expression was noticeably detectable in the SMA+ smooth muscle cells of arterioles and in the CD31+ capillaries. Following CBDL, increased expression of GRK2 was also found in mesenteric tissue, though there was no change in the level of β-arrestin 2. CONCLUSION: Decreased levels of ET-1 and increased ETBR expression in the mesenteric circulation following CBDL in rats may underlie mesenteric vasodilation in individuals with PHT. Mechanistically, increased GRK2 expression may lead to desensitization of ETAR, as well as other vasoconstrictors, promoting this vasodilatory effect.
基金support from the Tangshan Talent Funding Project(Grant No.A202202007)National Natural Science Foundation of China(Grant Nos.22102136 and 21703065)+2 种基金Natural Science Foundation of Hebei Province(Grant Nos.B2018209267 and E2022209039)Natural Science Foundation of Hubei Province(Grant No.2022CFB1001)Department of Education of Hubei Province(Grant No.Q20221701).
文摘Electrochemical C-C and C-N coupling reactions with the conversion of abundant and inexpensive small molecules,such as CO_(2) and nitrogencontaining species,are considered a promising route for increasing the value of CO_(2) reduction products.The development of high-performance catalysts is the key to the both electrocatalytic reactions.In this review,we present a systematic summary of the reaction systems for electrocatalytic CO_(2) reduction,along with the coupling mechanisms of C-C and C-N bonds over outstanding electrocatalytic materials recently developed.The key intermediate species and reaction pathways related to the coupling as well as the catalyst-structure relationship will be also discussed,aiming to provide insights and guidance for designing efficient CO_(2) reduction systems.
基金Project(2010CB732101) supported by the National Basic Research Program of China Project(SKLQ 008) supported by the Research Fund of State Key Laboratory of Geomechanics and Geotechnical Engineering of China
文摘In order to consider the influence of temperature and underground water movement, an elastoplastic model and a 2D FEM stress fields on the migration of radioactive nuclide with code for analysis of coupled thermo-hydro-mechanical (THM) processes in saturated and unsaturated porous media were extended and improved through introducing the percolation and migration equation, so that the code can be used for solving the temperature field, flow field, stress field and nuclide concentration field simultaneously. The states of temperatures, pore pressures and nuclide concentrations in the near field of a hypothetical nuclear waste repository were investigated. The influence of the half life of the radioactive nuclide on the temporal change of nuclide concentration was analyzed considering the thermo-hydro-mechanical-migratory coupling. The results show that, at the boundary of the vitrified waste, the concentration of radioactive nuclide with a half life of 10 a falls after a period of rising, with the maximum value of 0.182 mol/m3 and the minimum value of 0.181 mol/m^3 at the end of computation. For a half life of 1 000 a, the concentration of radioactive nuclide always increases with the increase of the time during the computation period; and the maximum value is 1.686 mol/m^3 at the end of the computation. Therefore, under the condition of THM coupling, the concentration of radioactive nuclide with a shorter half life will decrease more quickly with water flow; but for the radioactive nuclide with a longer half life, its concentration will keep at a higher level for a longer time in the migration process.
基金Foundation item: Supported by the National Natural Science Foundation of China under Grant No. 51279130 and No. 51239008
文摘In this study, the coupled heave-pitch motion equations of a spar platform were established by considering lst-order and 2nd-order random wave loads and the effects of time-varying displacement volume and transient wave elevation. We generated random wave loads based on frequency-domain wave load transfer functions and the Joint North Sea Wave Project (JONSWAP) wave spectrum, designed program codes to solve the motion equations, and then simulated the coupled heave-pitch motion responses of the platform in the time domain. We then calculated and compared the motion responses in different sea conditions and separately investigated the effects of 2nd-order random wave loads and transient wave elevation. The results show that the coupled heave-pitch motion responses of the platform are primarily dominated by wave height and the characteristic wave period, the latter of which has a greater impact. 2nd-order mean wave loads mainly affect the average heave value. The platform's pitch increases after the 2nd-order low frequency wave loads are taken into account. The platform's heave is underestimated if the transient wave elevation term in the motion equations is neglected.
文摘Cobalt-based oxides,with high abundance,good stability and excellent catalytic performance,are regarded as promising photocatalysts for artificial photosynthetic systems to alleviate foreseeable energy shortages and global warming.Herein,for the first time,a series of novel spongy porous CDs@CoOx materials were synthesized to act as an efficient and stable bifunctional photocatalyst for water oxidation and CO2 reduction.Notably,the preparation temperatures visibly influence the morphologies and photocatalytic performances of the CDs@CoOx.Under the optimal conditions,a maximum O2 yield of 40.4% and pretty apparent quantum efficiency(AQE)of 58.6% at 460 nm were obtained over CDs@CoOx-300 for water oxidation.Similarly,the optimized sample CDs@CoOx-300 manifests significant enhancement on the CO2-to-CO conversion with a high selectivity of 89.3% and CO generation rate of 8.1μmol/h,which is superior to most previous cobalt-based catalysts for CO2 reduction.The composite CDs@CoOx-300 not only exposes more active sites but also facilitates electron transport,which results in excellent photocatalytic activity.In addition,the boosted photocatalytic behavior is attributed to the synergistic effect between CoOx and CDs,which was verified by the photocatalytic activity control experiments and electrochemical characterization.The work offers a novel strategy to fabricate a high performance bifunctional photocatalyst for water oxidation and CO2 reduction.
文摘Herein,a bottom-down design is presented to successfully fabricate ZIF-derived Co3O4,grown in situ on a one-dimensional(1D)α-MnO2 material,denoted as α-MnO2@Co3O4.The synergistic effect derived from the coupled interface constructed betweenα-MnO2 and Co3O4 is responsible for the enhanced catalytic activity.The resultantα-MnO2@Co3O4 catalyst exhibits excellent catalytic activity at a T90%(temperature required to achieve a toluene conversion of 90%)of approximately 229℃,which is 47 and 28℃ lower than those of the pureα-MnO2 nanowire and Co3O4-b obtained via pyrolysis of ZIF-67,respectively.This activity is attributed to the increase in the number of surface-adsorbed oxygen species,which accelerate the oxygen mobility and enhance the redox pairs of Mn^4+/Mn^3+ and Co^2+/Co^3+.Moreover,the result of in situ diffuse reflectance infrared Fourier transform spectroscopy suggests that the gaseous oxygen could be more easily activated to adsorbed oxygen species on the surface of α-MnO2@Co3O4 than on that of α-MnO2.The catalytic reaction route of toluene oxidation over theα-MnO2@Co3O4 catalyst is as follows:toluene→benzoate species→alkanes containing oxygen functional group→CO2 and H2O.In addition,the α-MnO2@Co3O4 catalyst shows excellent stability and good water resistance for toluene oxidation.Furthermore,the preparation method can be extended to other 1D MnO2 materials.A new strategy for the development of high-performance catalysts of practical significance is provided.
基金the National Natural Science Foundation of China(51303083)the National Natural Science Foundation of China for Excellent Young Scholars(51922050)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20191293)the Fundamental Research Funds for the Central Universities(30920021123)。
文摘Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.
基金supported by the National Key R&D Program of China(2022YFA2105900)the National Natural Science Foundation of China(No.22178197)。
文摘Electrochemical reduction of CO_(2)(CO_(2)RR)has become a research hot spot in recent years in the context of carbon neutrality.HCOOH is one of the most promising products obtained by electrochemical reduction of CO_(2) due to its high energy value as estimated by market price per energy unit and wide application in chemical industry.Biomass is the most abundant renewable resource in the natural world.Coupling biomass oxidative conversion with CO_(2)RR driven by renewable electricity would well achieve carbon negativity.In this work,we comprehensively reviewed the current research progress on CO_(2)RR to produce HCOOH and coupled system for conversion of biomass and its derivatives to produce value-added products.Sn-and Bi-based electrocatalysts are discussed for CO_(2)RR with regards to the structure of the catalyst and reaction mechanisms.Electro-oxidation reactions of biomass derived sugars,alcohols,furan aldehydes and even polymeric components of lignocellulose were reviewed as alternatives to replace oxygen evolution reaction(OER)in the conventional electrolysis process.It was recommended that to further improve the efficiency of the coupled system,future work should be focused on the development of more efficient and stable catalysts,careful design of the electrolytic cells for improving the mass transfer and development of environment-friendly processes for recovering the formed formate and biomass oxidation products.
基金supported by the National Natural Science Foundation of China(52072196,52002200,52102106,52202262,22379081,22379080)the Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09)+1 种基金the Natural Science Foundation of Shandong Province(ZR2020QE063,ZR202108180009,ZR2023QE059)the Project funded by China Postdoctoral Science Foundation(2023M741871)。
文摘Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.
基金supported by Natural Science Basic Research Program in Shaanxi Province of China(No.2023-JCYB-574)National Natural Science Foundation of China(No.62204203).
文摘High qualityβ-Ga_(2)O_(3)single crystal nanobelts with length of 2−3 mm and width from tens of microns to 132μm were synthesized by carbothermal reduction method.Based on the grown nanobelt with the length of 600μm,the dual-Schottky-junctions coupling device(DSCD)was fabricated.Due to the electrically floating Ga_(2)O_(3)nanobelt region coupling with the double Schottky-junctions,the current I_(S2)increases firstly and rapidly reaches into saturation as increase the voltage V_(S2).The saturation current is about 10 pA,which is two orders of magnitude lower than that of a single Schottky-junction.In the case of solar-blind ultraviolet(UV)light irradiation,the photogenerated electrons further aggravate the coupling physical mechanism in device.I_(S2)increases as the intensity of UV light increases.Under the UV light of 1820μW/cm^(2),I_(S2)quickly enters the saturation state.At V_(S2)=10 V,photo-to-dark current ratio(PDCR)of the device reaches more than 104,the external quantum efficiency(EQE)is 1.6×10^(3)%,and the detectivity(D*)is 7.5×10^(12)Jones.In addition,the device has a very short rise and decay times of 25−54 ms under different positive and negative bias.DSCD shows unique electrical and optical control characteristics,which will open a new way for the application of nanobelt-based devices.
文摘Integrating selective organic synthesis with hydrogen(H_(2))evolution in one photocatalytic redox reaction system sheds light on the underlying approach for concurrent employment of photogenerated electrons and holes towards efficient production of solar fuels and chemicals.In this work,a facile one‐pot oil bath method has been proposed to fabricate a noble metal‐free ultrathin Ni‐doped ZnIn_(2)S_(4)(ZIS/Ni)composite nanosheet for effective solar‐driven selective dehydrocoupling of benzyl alcohol into value‐added C–C coupled hydrobenzoin and H_(2) fuel,which exhibits higher performance than pure ZIS nanosheet.The remarkably improved photoredox activity of ZIS/Ni is mainly attributed to the optimized electron structure featuring narrower band gap and suitable energy band position,which facilitates the ability of light harvesting and photoexcited charge carrier separation and transfer.Furthermore,it has been demonstrated that it is feasible to employ ZIS/Ni for various aromatic alcohols dehydrocoupling to the corresponding C–C coupled products.It is expected that this work can stimulate further interest on the establishment of innovative photocatalytic redox platform coupling clean solar fuels synthesis and selective organic conversion in a sustainable manner.
基金the support of the Sichuan Science and Technology Program(2023NSFC0098)the Science and Technology Development Fund from Macao SAR(FDCT)(0081/2019/AMJ,0154/2019/A3,006/2022/ALC,and 0111/2022/A2)+2 种基金the Shenzhen-Hong Kong-Macao Science and Technology Research Programme(Type C)(SGDX20210823103803017)the Multi-Year Research Grants(MYRG2022-00026-IAPME)from Research&Development Office at University of Macaothe Frontier Project of Chengdu Tianfu New Area Institute(SWUST,2022ZY017)。
文摘The development of highly active,selective,and stable electrocatalysts can facilitate the effective implementation of electrocatalytic CO_(2)conversion into fuels or chemicals for mitigating the energy crisis and climate problems.Therefore,it is necessary to achieve the goal through reasonable material design based on the actuality of the operational active site at the molecular scale.Inspired by the stimulating synergistic effect of coupled heteronuclear metal atoms,a novel Ni-Co atomic pairs configuration(denoted as NiN_(3)?CoN_(3)-NC)active site was theoretically screened out for improving electrochemical CO_(2)reduction reaction(CO_(2)RR).The structure of NiN_(3)?CoN_(3)-NC was finely regulated by adjusting Zn content in the precursors Zn/Co/Ni-zeolite imidazolate frameworks(Zn/Co/Ni-ZIFs)and pyrolysis temperature.The structural features of NiN_(3)?CoN_(3)-NC were systematically confirmed by aberration-corrected HAADF-STEM coupled with 3D atom-overlapping Gaussian-function fitting mapping,XAFS,and XRD.The results of theoretical calculations reveal that the synergistic effect of Ni-Co atomic pairs can effectively promote the*COOH intermediate formation and thus the overall CO_(2)RR kinetic was improved,and also restrained the competitive hydrogen evolution reaction.Due to the attributes of Ni-Co atomic pairs configuration,the developed NiN_(3)?CoN_(3)-NC with superior catalytic activity,selectivity,and durability,with a high turnover frequency of 2265 h^(-1)at-1.1 V(vs.RHE)and maximum Faradaic efficiency of 97.7%for CO production.This work demonstrates the great potential of DACs as highly efficient catalysts for CO_(2)RR,provides a useful strategy to design heteronuclear DACs,exploits the synergistic effect of multiple metal sites to facilitate complex CO_(2)RR catalytic reactions,and inspires more efforts to develop the potential of DACs in various fields.
基金funded by the National Natural Science Foundation of China(Grant No.NSFC51374147)the German Society for Petroleum and Coal Science and Technology(Grant No.DGMK680-4)
文摘As one of the most important ways to reduce the greenhouse gas emission,carbon dioxide(CO2)enhanced gas recovery(CO2-EGR) is attractive since the gas recovery can be enhanced simultaneously with CO2sequestration.Based on the existing equation of state(EOS) module of TOUGH2 MP,extEOS7C is developed to calculate the phase partition of H2O-CO2-CH4-NaCl mixtures accurately with consideration of dissolved NaCI and brine properties at high pressure and temperature conditions.Verifications show that it can be applied up to the pressure of 100 MPa and temperature of 150℃.The module was implemented in the linked simulator TOUGH2MP-FLAC3 D for the coupled hydro-mechanical simulations.A simplified three-dimensional(3D)1/4 model(2.2 km×1 km×1 km) which consists of the whole reservoir,caprock and baserock was generated based on the geological conditions of a gas field in the North German Basin.The simulation results show that,under an injection rate of 200,000 t/yr and production rate of 200,000 sm3/d,CO2breakthrough occurred in the case with the initial reservoir pressure of 5 MPa but did not occur in the case of 42 MPa.Under low pressure conditions,the pressure driven horizontal transport is the dominant process;while under high pressure conditions,the density driven vertical flow is dominant.Under the considered conditions,the CO2-EGR caused only small pressure changes.The largest pore pressure increase(2 MPa) and uplift(7 mm) occurred at the caprock bottom induced by only CO2injection.The caprock had still the primary stress state and its integrity was not affected.The formation water salinity and temperature variations of ±20℃ had small influences on the CO2-EGR process.In order to slow down the breakthrough,it is suggested that CO2-EGR should be carried out before the reservoir pressure drops below the critical pressure of CO2.
基金support from the National Natural Science Foun-dation of China(11972267).
文摘The ablation of ultra-high-temperature ceramics(UTHCs)is a complex physicochemical process including mechanical behavior,temperature effect,and chemical reactions.In order to realize the structural optimization and functional design of ultra-high temperature ceramics,a coupled thermo-chemo-mechanical bond-based peridynamics(PD)model is proposed based on the ZrB_(2) ceramics oxidation kinetics model and coupled thermomechanical bond-based peridynamics.Compared with the traditional coupled thermo-mechanical model,the proposedmodel considers the influenceof chemical reactionprocessonthe ablation resistanceof ceramicmaterials.In order to verify the reliability of the proposed model,the thermo-mechanical coupling model,damage model and oxidation kinetic model are established respectively to investigate the applicability of the proposedmodel proposed in dealing with thermo-mechanical coupling,crack propagation,and chemical reaction,and the results show that the model is reliable.Finally,the coupled thermo-mechanical model and coupled thermo-chemo-mechanical model are used to simulate the crack propagation process of the plate under the thermal shock load,and the results show that the oxide layer plays a good role in preventing heat transfer and protecting the internal materials.Based on the PD fully coupled thermo-mechanical model,this paper innovatively introduces the oxidation kinetic model to analyze the influence of parameter changes caused by oxide layer growth and chemical growth strain on the thermal protection ability of ceramics.The proposed model provides an effective simulation technology for the structural design of UTHCs.
基金supported by the project of the National Natural Science Foundation of China (Grant Nos. 41275082 and 41305070)the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDA05110103)the Knowledge Innovation Program of the Chinese Academy of Sciences (Grant Nos. KZCX2-EW-QN208 and 7-122158)
文摘In this paper, a coupled model was used to estimate the responses of soil moisture and net primary production of vegetation(NPP) to increasing atmospheric CO2 concentration and climate change. The analysis uses three experiments simulated by the second-generation Earth System Model(CanESM2) of the Canadian Centre for Climate Modelling and Analysis(CCCma), which are part of the phase 5 of the Coupled Model Intercomparison Project(CMIP5). The authors focus on the magnitude and evolution of responses in soil moisture and NPP using simulations modeled by CanESM, in which the individual effects of increasing CO2 concentration and climate change and their combined effect are separately accounted for. When considering only the single effect of climate change, the soil moisture and NPP have a linear trend of 0.03 kg m–2 yr–1 and –0.14 gC m–2 yr–2, respectively. However, such a reduction in the global NPP results from the decrease of NPP at lower latitudes and in the Southern Hemisphere, although increased NPP has been shown in high northern latitudes. The largest negative trend is located in the Amazon basin at –1.79 gC m–2 yr–2. For the individual effect of increasing CO2 concentration, both soil moisture and NPP show increases, with an elevated linear trend of 0.02 kg m–2 yr–1 and 0.84 gC m–2 yr–2, respectively. Most regions show an increasing NPP, except Alaska. For the combined effect of increasing atmospheric CO2 and climate change, the increased soil moisture and NPP exhibit a linear trend of 0.04 kg m–2 yr–1 and 0.83 gC m–2 yr–2 at a global scale. In the Amazon basin, the higher reduction in soil moisture is illustrated by the model, with a linear trend of –0.39 kg m–2 yr–1, for the combined effect. Such a change in soil moisture is caused by a weakened Walker circulation simulated by this coupled model, compared with the single effect of increasing CO2 concentration(experiment M2), and a consequence of the reduction in NPP is also shown in this area, with a linear trend of-0.16 gC m-2 yr-2.
基金This research was conducted within the DECOVALEX-2023 projectDECOVALEX is an international research project comprising participants from industry,government,and academia,focusing on development of understanding,models and codes in complex coupled problems in sub-surface geological and engineering applications.DECOVALEX-2023 is the current phase of the project.The authors appreciate the DECOVALEX-2023 Funding Organisations Andra,BASE,BGE,BGR,CAS,CNSC,COVRA,US DOE,ENRESA,ENSI,JAEA,KAERI,NWMO,RWM,SÚRAO,SSM and Taipower for their financial and technical support of the work described in this paper.The statements made in the paper are,however,solely those of the authors and do not necessarily reflect those of the Funding Organisations.This work was further supported by the German Federal Ministry for Economic Affairs and Climate Action(BMWK).
文摘Dilatancy-controlled gas flow in preferential pathways plays a key role in the safety analysis of radioactive waste repositories.This is particularly the case for bentonite,an often-preferred barrier material.Gas flow in preferential pathways is characterized by localization and spontaneous behavior,which is challenging to simulate in numerical models due to strong hydro-mechanical coupling.To analyze a laboratory experiment in the framework of the DECOVALEX-2023 project,this study introduced a new approach of combining continuous modelling methods with spatial material properties derived from material heterogeneities and experimental observations.The proposed model utilized hydro-mechanical spatial distributions,namely Young’s modulus and gas entry pressure,and elastoplasticity combined with a linear swelling model.A conceptual strain-dependent permeability approach simulated dilatancycontrolled gas flow based on hydro-mechanical coupling.To test the effectiveness of the presented approach,a gas injection test in a compacted,saturated bentonite sample was simulated using the opensource code OpenGeoSys 5.8 and compared with experimental observations.The presented methodology is capable of simulating localized gas flow in preferential pathways.The spatial distributions of Young’s modulus and gas entry pressure affect the swelling pressure,relative permeability and,in combination with the strain-dependent permeability model,also the intrinsic permeability.
基金financially supporrted by the National Key Research and Development Program of China(Grant No.2017YFC1404200)the National Natural Science Foundation of China(Grant Nos.51779150 and 51979040)
文摘In this study, 1D and 2D shallow-water models were coupled to simulate unsteady flow in channel networks and embayment. The 1D model solved the 1D shallow-water equations (St. Venant) using the Preissmann box method and targeted long narrow reaches of the river networks, while the 2D model targeted broad channels and embayment and solved the 2D shallow-water equations using a semi-implicit scheme applied to an unstructured grid of triangular cells. The 1D and 2D models were solved simultaneously by building a matrix for the free surface elevation at every 1D junction and 2D cell center. Velocities were then computed explicitly based on the results at the previous time step and the updated water level. The originality of the scheme arose from a novel coupling method. The results showed that the coupled 1D/2D model produced identical results as the full 2D model in classical to benchmark problems with considerable savings in computational effort. Application of the model to the Pearl River Estuary in southern China showed that complex patterns of tidal wave propagation could be efficiently modeled.