Nanosize cerium-zirconium solid solution(CZO)with a special fluorite structure has received an increasing research interest due to their remarkable advantages such as excellent oxygen storage capacity and great flexib...Nanosize cerium-zirconium solid solution(CZO)with a special fluorite structure has received an increasing research interest due to their remarkable advantages such as excellent oxygen storage capacity and great flexibility in their composition and structure.By partial metal(including rare earth,transition,alkaline earth or other metal)doping into CZO,the physicochemical properties of these catalytic materials can be controllable adjusted for the study of specific reactions.To date,nanosize CZO has been prepared by co-precipitation,sol-gel,surfactant-assisted approach,solution combustion,micro-emulsion,high energy mechanical milling,etc.The advent of these methodologies has prompted researchers to construct well-defined networks with customized micromorphology and functionalities.In this review,we describe not only the basic structure and synthetic strategies of CZO,but also their relevant applications in environmental catalysis,such as the purification for CO,nitrogen oxides(NOx),volatile organic compounds(VOC),soot,hydrocarbon(HC),CO2 and solid particulate matters(PM),and some reaction mechanisms are also summarized.展开更多
Photocatalytic hydrogen(H2)evolution via water spilling over semiconductors has been considered to be one of the most promising strategies for sustainable energy supply in the future to provide non-pollution and renew...Photocatalytic hydrogen(H2)evolution via water spilling over semiconductors has been considered to be one of the most promising strategies for sustainable energy supply in the future to provide non-pollution and renewable energy.The key to efficient conversion of solar-chemical energy is the design of an efficient structure for high charge separation and transportation.Therefore,cocatalysts are necessary in boosting photocatalytic H2 evolution.To date,semiconductor photocatalysts have been modified by various cocatalysts due to the extended light harvest,enhanced charge carrier separation efficiency and improved stability.This review focuses on recent developments of cocatalysts in photocatalytic H2 evolution,the roles and mechanism of the cocatalysts are discussed in detail.The cocatalysts can be divided into the following categories:metal/alloy cocatalysts,metal phosphides cocatalysts,metal oxide/hydroxide cocatalysts,carbon-based cocatalysts,dual cocatalysts,Z-scheme cocatalysts and MOFs cocatalysts.The future research and forecast for photocatalytic hydrogen generation are also suggested.展开更多
Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission elec...Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray scattering elemental mapping, X-ray diffraction, Raman and X-ray photoelectron spectroscopy, and temperature-programmed reduction of H2. Further, their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction. K substitution into the LaNiO3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion. Amongst various catalysts, La0.95K0.05NiO3 exhibited the highest activity in soot combustion (with its T50 and CO2 S values being 338 °C and 98.2%, respectively), which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst. K-substitution improves the valence state of Ni and increases the number of oxygen vacancies, thereby leading to increased density of surface-active oxygen species. The active oxygen species play a vital role in catalyzing the elimination of soot. The perovskite-type La1?xKxNiO3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.展开更多
The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/...The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi(CN/BMO/Bi)hollow microsphere was successfully fabricated through solvothermal and in situ reduction methods.The results revealed that the optimal ternary 0.4 CN/BMO/9 Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B(RhB)degradation with nine times that of pure BMO.The DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4 CN/BMO/9 Bi is a z-scheme structure.Quenching experiments also provided solid evidence that the·O^2-(at-0.33 eV)is the main species during dye degradation,and the conduction band of g-C3N4 is only the reaction site,demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2 MoO 6/Bi is through an indirect z-scheme structure.Thus,the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping,resulting in better optical absorption ability and a lower combination rate of photogenerated charge carriers.The findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.展开更多
The electronic metal-support interaction(EMSI)is one of most intriguing phenomena in heterogeneous catalysis.In this work,this subtle effect is clearly demonstrated by density functional theory(DFT)calculations of sin...The electronic metal-support interaction(EMSI)is one of most intriguing phenomena in heterogeneous catalysis.In this work,this subtle effect is clearly demonstrated by density functional theory(DFT)calculations of single Pt atom supported on vacancies in a boron nitride nanosheet.Moreover,the relation between the EMSI and the performance of Pt in propane direct dehydrogenation(PDH)is investigated in detail.The charge state and partial density of states of single Pt atom show distinct features at different anchoring positions,such as boron and nitrogen vacancies(Bvac and Nvac,respectively).Single Pt atom become positively and negatively charged on Bvac and Nvac,respectively.Therefore,the electronic structure of Pt can be adjusted by rational deposition on the support.Moreover,Pt atoms in different charge states have been shown to have different catalytic abilities in PDH.The DFT calculations reveal that Pt atoms on Bvac(Pt-Bvac)have much higher reactivity towards reactant/product adsorption and C–H bond activation than Pt supported on Nvac(Pt-Nvac),with larger adsorption energy and lower barrier along the reaction pathway.However,the high reactivity of Pt-Bvac also hinders propene desorption,which could lead to unwanted deep dehydrogenation.Therefore,the results obtained herein suggest that a balanced reactivity for C–H activation in propane and propene desorption is required to achieve optimum yields.Based on this descriptor,a single Pt atom on a nitrogen vacancy is considered an effective catalyst for PDH.Furthermore,the deep dehydrogenation of the formed propene is significantly suppressed,owing to the large barrier on Pt-Nvac.The current work demonstrates that the catalytic properties of supported single Pt atoms can be tuned by rationally depositing them on a boron nitride nanosheet and highlights the great potential of single-atom catalysis in the PDH reaction.展开更多
A series of quaternary ammonium ionic liquids(ILs)were synthesized and employed as catalysts for the production of poly(isosorbide carbonate)(PIC)from diphenyl carbonate and isosorbide via a melt polycondensation proc...A series of quaternary ammonium ionic liquids(ILs)were synthesized and employed as catalysts for the production of poly(isosorbide carbonate)(PIC)from diphenyl carbonate and isosorbide via a melt polycondensation process.The relationship between the anions of the ILs and the catalytic activities was investigated,and the readily‐prepared IL tetraethylammonium imidazolate(TEAI)was found to exhibit the highest catalytic activity.After optimizing the reaction conditions,a PIC with a weight‐average molecular weight(Mw)of25600g/mol was obtained,in conjunction with an isosorbide conversion of92%.As a means of modifying the molecular flexibility and thermal properties of the PIC,poly(aliphatic diol‐co‐isosorbide carbonate)s(PAIC)s were successfully synthesized,again using TEAI,and polymers with Mw values ranging from29000to112000g/mol were obtained.13C NMR analyses determined that the PAIC specimens had random microstructures,while differential scanning calorimetry demonstrated that each of the PAICs were amorphous and had glass transition temperatures ranging from50to115°C.Thermogravimetric analyses found Td‐5%values ranging from316to332°C for these polymers.Based on these data,it is evident that the incorporation of linear or cyclohexane‐based diol repeating units changed the thermal properties of the PIC.展开更多
PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution o...PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g^–1 h^–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g^–1 h^–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.展开更多
Nanocatalysts consisting of three‐dimensionally ordered macroporous(3DOM)TiO2‐supported ultrafine Pd nanoparticles(Pd/3DOM‐TiO2‐GBMR)were readily fabricated by gas bubbling‐assisted membrane reduction(GBMR)method...Nanocatalysts consisting of three‐dimensionally ordered macroporous(3DOM)TiO2‐supported ultrafine Pd nanoparticles(Pd/3DOM‐TiO2‐GBMR)were readily fabricated by gas bubbling‐assisted membrane reduction(GBMR)method.These catalysts had a well‐defined and highly ordered macroporous nanostructure with an average pore size of 280 nm.In addition,ultrafine hemispherical Pd nanoparticles(NPs)with a mean particle size of 1.1 nm were found to be well dispersed over the surface of the 3DOM‐TiO2 support and deposited on the inner walls of the material.The nanostructure of the 3DOM‐TiO2 support ensured efficient contact between soot particles and the catalyst.The large interface area between the ultrafine Pd NPs and the TiO2 also increased the density of sites for O2 activation as a result of the strong metal(Pd)‐support(TiO2)interaction(SMSI).A Pd/3DOM‐TiO2‐GBMR catalyst with ultrafine Pd NPs(1.1 nm)exhibited higher catalytic activity during diesel soot combustion compared with that obtained from a specimen having relatively large Pd NPs(5.0 nm).The T10,T50 and T90 values obtained from the former were 295,370 and 415°C.Both the activity and nanostructure of the Pd/3DOM‐TiO2‐GBMR catalyst were stable over five replicate soot oxidation trials.These results suggest that nanocatalysts having a 3DOM structure together with ultrafine Pd NPs can decrease the amount of Pd required,and that this approach has potential practical applications in the catalytic combustion of diesel soot particles.展开更多
Efficient composite semiconductor photocatalysts are highly desirable for the visible-light-driven degradation of organic pollutants. In this study, Bi24O31Cl10 photocatalyst was prepared via a hydrothermal method and...Efficient composite semiconductor photocatalysts are highly desirable for the visible-light-driven degradation of organic pollutants. In this study, Bi24O31Cl10 photocatalyst was prepared via a hydrothermal method and modified with Pt nanoparticles (NPs) through a facile deposition procedure. The composite photocatalyst was characterized by X-ray diffraction, transmission electronic microscopy, X-ray photoelectron spectroscopy, UV-vis diffusion reflectance spectroscopy, photoluminescence spectroscopy, and electron spin resonance. The 1.0 wt% Pt/Bi24O31Cl10 photocatalyst showed the highest activity for the degradation of methyl orange under visible light (source: 300 W Xe lamp coupled with a UV-cutoff filter), and the photocatalytic degradation efficiency improved about 2.2 times compared to that of pure Bi24O31Cl10. The composite photocatalyst could maintain most of its activity after four runs of the photocatalytic experimental cycle. This study could provide a novel insight for the modification of other desirable semiconductor materials to achieve high photocatalytic activities.展开更多
The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal...The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal‐organic frameworks(MOFs)are considered to be potential photocatalytic materials.Herein,monodisperse,small size,non‐precious metal transition metal phosphide Ni2P is encapsulated into a typical MOF(UiO‐66‐NH2)as a hybrid core‐shell cocatalyst to modify Zn_(0.5)Cd_(0.5)S for photocatalytic hydrogen production.Ni2P is wrapped in UiO‐66‐NH_(2)via an in situ solvothermal method,and Zn_(0.5)Cd_(0.5)S sulfide is decorated with a core‐shell Ni_(2)P@UiO‐66‐NH_(2)cocatalyst to obtain ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite materials.Photoelectric and chemical characterization confirms that the ternary composites have good kinetic hydrogen production performance.The hydrogen production rate of 10%10 mg Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S reaches 40.91 mmol·g^(–1)·h^(–1)with an apparent quantum efficiency at 420 nm of 13.57%.The addition of 10 mg Ni_(2)P@UiO‐66‐NH_(2)increases the surface area of the ternary material,providing abundant reaction sites and forming an efficient charge transfer channel,which is conducive to efficient hydrogen production by the ternary photocatalysts.It is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic reaction.This study provides a new perspective for the construction of high‐performance photocatalytic materials.展开更多
In this paper, we propose a hybrid PML (H-PML) combining the normal absorption factor of convolutional PML (C-PML) with tangential absorption factor of Mutiaxial PML (M-PML). The H-PML boundary conditions can be...In this paper, we propose a hybrid PML (H-PML) combining the normal absorption factor of convolutional PML (C-PML) with tangential absorption factor of Mutiaxial PML (M-PML). The H-PML boundary conditions can better suppress the numerical instability in some extreme models, and the computational speed of finite-element method and the dynamic range are greatly increased using this HPML. We use the finite-element method with a hybrid PML to model the acoustic reflection of the interface when wireline and well logging while drilling (LWD), in a formation with a reflector outside the borehole. The simulation results suggests that the PS- and SP- reflected waves arrive at the same time when the inclination between the well and the outer interface is zero, and the difference in arrival times increases with increasing dip angle. When there are fractures outside the well, the reflection signal is clearer in the subsequent reflection waves and may be used to identify the fractured zone. The difference between the dominant wavelength and the model scale shows that LWD reflection logging data are of higher resolution and quality than wireline acoustic reflection logging.展开更多
Conventional time-space domain and frequency-space domain prediction filtering methods assume that seismic data consists of two parts, signal and random noise. That is, the so-called additive noise model. However, whe...Conventional time-space domain and frequency-space domain prediction filtering methods assume that seismic data consists of two parts, signal and random noise. That is, the so-called additive noise model. However, when estimating random noise, it is assumed that random noise can be predicted from the seismic data by convolving with a prediction error filter. That is, the source-noise model. Model inconsistencies, before and after denoising, compromise the noise attenuation and signal-preservation performances of prediction filtering methods. Therefore, this study presents an inversion-based time-space domain random noise attenuation method to overcome the model inconsistencies. In this method, a prediction error filter (PEF), is first estimated from seismic data; the filter characterizes the predictability of the seismic data and adaptively describes the seismic data's space structure. After calculating PEF, it can be applied as a regularized constraint in the inversion process for seismic signal from noisy data. Unlike conventional random noise attenuation methods, the proposed method solves a seismic data inversion problem using regularization constraint; this overcomes the model inconsistency of the prediction filtering method. The proposed method was tested on both synthetic and real seismic data, and results from the prediction filtering method and the proposed method are compared. The testing demonstrated that the proposed method suppresses noise effectively and provides better signal-preservation performance.展开更多
A series of catalysts consisting of three‐dimensionally ordered macroporous(3DOM)x‐CeO2/Al2O3‐supported Au nanoparticles(x=2,10,20,and40wt%)were successfully synthesized using a reduction‐deposition method.These c...A series of catalysts consisting of three‐dimensionally ordered macroporous(3DOM)x‐CeO2/Al2O3‐supported Au nanoparticles(x=2,10,20,and40wt%)were successfully synthesized using a reduction‐deposition method.These catalysts were characterized using scanning electron microscopy,the Brunauer‐Emmett‐Teller method,X‐ray diffraction,transmission electron microscopy,ultraviolet‐visible spectroscopy,and temperature‐programmed reduction by H2.Au nanoparticles of mean particle size5nm were well dispersed and supported on the inner walls of uniform macropores.The3DOM structure improved the contact efficiency between soot and the catalyst.An Al‐Ce‐O solid solution was formed in the multilayer support,i.e.,x‐CeO2/Al2O3,by the incorporation of Al3+ions into the CeO2lattice,which resulted in the creation of extrinsic oxygen vacancies.Strong interactions between the metal(Au)and the support(Ce)increased the amount of active oxygen species,and this promoted soot oxidation.The catalytic performance in soot combustion was evaluated using a temperature‐programmed oxidation technique.The presence of CeO2nanolayers in the3DOM Au/x‐CeO2/Al2O3catalysts clearly improved the catalytic activities in soot oxidation.Among the prepared catalysts,3DOM Au/20%CeO2/Al2O3showed high catalytic activity and stability in diesel soot oxidation.展开更多
The quality factor(or Q value)is an important parameter for characterizing the inelastic properties of rock.Achieving a Q value estimation with high accuracy and stability is still challenging.In this study,a new meth...The quality factor(or Q value)is an important parameter for characterizing the inelastic properties of rock.Achieving a Q value estimation with high accuracy and stability is still challenging.In this study,a new method for estimating ultrasonic attenuation using a spectral ratio based on an S transform(SR-ST)is presented to improve the stability and accuracy of Q estimation.The variable window of ST is used to solve the time window problem.We add two window factors to the Gaussian window function in the ST.The window factors can adjust the scale of the Gaussian window function to the ultrasonic signal,which reduces the calculation error attributed to the conventional Gaussian window function.Meanwhile,the frequency bandwidth selection rules for the linear regression of the amplitude ratio are given to further improve stability and accuracy.First,the feasibility and influencing factors of the SR-ST method are studied through numerical testing and standard sample experiments.Second,artificial samples with different Q values are used to study the adaptability and stability of the SR-ST method.Finally,a further comparison between the new method and the conventional spectral ratio method(SR)is conducted using rock field samples,again addressing stability and accuracy.The experimental results show that this method will yield an error of approximately 36%using the conventional Gaussian window function.This problem can be solved by adding the time window factors to the Gaussian window function.The frequency bandwidth selection rules and mean slope value of the amplitude ratio used in the SR-ST method can ensure that the maximum error of different Q values estimation(Q>15)is less than 10%.展开更多
The construction of a shale rock physics model and the selection of an appropriate brittleness index (B/) are two significant steps that can influence the accuracy of brittleness prediction. On one hand, the existin...The construction of a shale rock physics model and the selection of an appropriate brittleness index (B/) are two significant steps that can influence the accuracy of brittleness prediction. On one hand, the existing models of kerogen-rich shale are controversial, so a reasonable rock physics model needs to be built. On the other hand, several types of equations already exist for predicting the BI whose feasibility needs to be carefully considered. This study constructed a kerogen-rich rock physics model by performing the self- consistent approximation and the differential effective medium theory to model intercoupled clay and kerogen mixtures. The feasibility of our model was confirmed by comparison with classical models, showing better accuracy. Templates were constructed based on our model to link physical properties and the BL Different equations for the BI had different sensitivities, making them suitable for different types of formations. Equations based on Young's Modulus were sensitive to variations in lithology, while those using Lame's Coefficients were sensitive to porosity and pore fluids. Physical information must be considered to improve brittleness prediction.展开更多
Edge reflections are inevitable in numerical modeling of seismic wavefields, and they are usually attenuated by absorbing boundary conditions. However, the commonly used perfectly matched layer (PML) boundary condit...Edge reflections are inevitable in numerical modeling of seismic wavefields, and they are usually attenuated by absorbing boundary conditions. However, the commonly used perfectly matched layer (PML) boundary condition requires special treatment for the absorbing zone, and in three-dimensional (3D) modeling, it has to split each variable into three corresponding variables, which increases the computing time and memory storage. In contrast, the hybrid absorbing boundary condition (HABC) has the advantages such as ease of implementation, less computation time, and near-perfect absorption; it is thus able to enhance the computational efficiency of 3D elastic wave modeling. In this study, a HABC is developed from two-dimensional (2D) modeling into 3D modeling based on the I st Higdon one way wave equations, and a HABC is proposed that is suitable for a 3D elastic wave numerical simulation. Numerical simulation results for a homogenous model and a complex model indicate that the proposed HABC method is more effective and has better absorption than the traditional PML method.展开更多
Photocatalysis is considered a prospective way to alleviate the energy crisis and environmental pollution.It is therefore extremely important to design highly efficient photocatalysts for catalytic systems.In recent y...Photocatalysis is considered a prospective way to alleviate the energy crisis and environmental pollution.It is therefore extremely important to design highly efficient photocatalysts for catalytic systems.In recent years,hollow‐structured materials have attracted considerable interest for application in energy conversion fields owing to their large specific surface areas,improved light absorption,and shortened charge carrier transfer path.Because they contain inner and outer surfaces,hollow‐structured materials can provide a superior platform for the deposition of other components.A number of hollow‐structured hierarchical systems have been designed and fabricated in recent decades.It is important to rationally design and construct complex hierarchical structures.In this review,general preparation approaches for hollow‐structured materials are presented,followed by a summary of the recent synthesis methods and mechanisms of typical hollow‐structured materials for applications in the photocatalytic field.Complex hollow‐structured hierarchical photocatalysts are classified into two types,hollow cocatalyst‐based and hollow host photocatalyst‐based,and the design principle and analysis of the photocatalytic reaction mechanism for photocatalytic H2 evolution and CO_(2) reduction are also introduced.The effects of hollow‐structured materials have also been investigated.This review provides a reference for the rational construction of advanced,highly efficient photocatalytic materials.展开更多
The corrosion behavior of electrodeposited Ni with normal and bimodal grain size distribution was investigated.The microstructure of samples was researched by SEM,EBSD,TEM and XRD.The corrosion behavior was studied by...The corrosion behavior of electrodeposited Ni with normal and bimodal grain size distribution was investigated.The microstructure of samples was researched by SEM,EBSD,TEM and XRD.The corrosion behavior was studied by potentiodynamic tests and electrochemical impedance.Nanocrystalline Ni with(100)and(111)textures was prepared by an electrodeposition method.The Ni samples with different grain size distributions and twins were then obtained by heat treatment of nanocrystalline Ni at different temperatures.The effect of grain size on corrosion behavior of the sample depends on the ability of the environment to passivate.In the case where passive film forms on the sample surface,the corrosion resistance of the sample increases with decreasing grain size.Conversely,the corrosion resistance decreases with decreasing grain size when there is no passivation.The corrosion behavior of samples with bimodal grain size distribution obeys the rule of mixture.展开更多
基金financially supported by the National Natural Science Foundation of China (21673290, U1662103)~~
文摘Nanosize cerium-zirconium solid solution(CZO)with a special fluorite structure has received an increasing research interest due to their remarkable advantages such as excellent oxygen storage capacity and great flexibility in their composition and structure.By partial metal(including rare earth,transition,alkaline earth or other metal)doping into CZO,the physicochemical properties of these catalytic materials can be controllable adjusted for the study of specific reactions.To date,nanosize CZO has been prepared by co-precipitation,sol-gel,surfactant-assisted approach,solution combustion,micro-emulsion,high energy mechanical milling,etc.The advent of these methodologies has prompted researchers to construct well-defined networks with customized micromorphology and functionalities.In this review,we describe not only the basic structure and synthetic strategies of CZO,but also their relevant applications in environmental catalysis,such as the purification for CO,nitrogen oxides(NOx),volatile organic compounds(VOC),soot,hydrocarbon(HC),CO2 and solid particulate matters(PM),and some reaction mechanisms are also summarized.
基金financially supported by the National Natural Science Foundation of China(51572295,21273285 and 21003157)Beijing Nova Program(2008B76)Science Foundation of China University of Petroleum,Beijing(KYJJ2012-06-20 and 2462016YXBS05)~~
文摘Photocatalytic hydrogen(H2)evolution via water spilling over semiconductors has been considered to be one of the most promising strategies for sustainable energy supply in the future to provide non-pollution and renewable energy.The key to efficient conversion of solar-chemical energy is the design of an efficient structure for high charge separation and transportation.Therefore,cocatalysts are necessary in boosting photocatalytic H2 evolution.To date,semiconductor photocatalysts have been modified by various cocatalysts due to the extended light harvest,enhanced charge carrier separation efficiency and improved stability.This review focuses on recent developments of cocatalysts in photocatalytic H2 evolution,the roles and mechanism of the cocatalysts are discussed in detail.The cocatalysts can be divided into the following categories:metal/alloy cocatalysts,metal phosphides cocatalysts,metal oxide/hydroxide cocatalysts,carbon-based cocatalysts,dual cocatalysts,Z-scheme cocatalysts and MOFs cocatalysts.The future research and forecast for photocatalytic hydrogen generation are also suggested.
基金supported by the National Natural Science Foundation of China(21673142)National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2017A05)+1 种基金PetroChina Innovation Foundation(2018D-5007-0505)Science Foundation of China University of Petroleum,Beijing(242017QNXZ02,2462018BJC005)~~
文摘Three-dimensional ordered macroporous (3DOM) La1?xKxNiO3 perovskite-type catalysts were successfully prepared by a colloidal crystal template method and characterized by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray scattering elemental mapping, X-ray diffraction, Raman and X-ray photoelectron spectroscopy, and temperature-programmed reduction of H2. Further, their catalytic activity in soot combustion was determined by temperature-programmed oxidation reaction. K substitution into the LaNiO3 lattice led to remarkably improved catalytic activity of this catalyst in soot combustion. Amongst various catalysts, La0.95K0.05NiO3 exhibited the highest activity in soot combustion (with its T50 and CO2 S values being 338 °C and 98.2%, respectively), which is comparable to the catalytic activities of Pt-based catalysts under the condition of poor contact between the soot and the catalyst. K-substitution improves the valence state of Ni and increases the number of oxygen vacancies, thereby leading to increased density of surface-active oxygen species. The active oxygen species play a vital role in catalyzing the elimination of soot. The perovskite-type La1?xKxNiO3 nanocatalysts with 3DOM structure without noble metals have potential for practical applications in the catalytic combustion of diesel soot particles.
基金financially supported by the Science Foundation of China University of Petroleum,Beijing(2462017YJRC048,2462018BJC005)the National Natural Science Foundation of China(51802351)~~
文摘The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation rate.In this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi(CN/BMO/Bi)hollow microsphere was successfully fabricated through solvothermal and in situ reduction methods.The results revealed that the optimal ternary 0.4 CN/BMO/9 Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B(RhB)degradation with nine times that of pure BMO.The DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4 CN/BMO/9 Bi is a z-scheme structure.Quenching experiments also provided solid evidence that the·O^2-(at-0.33 eV)is the main species during dye degradation,and the conduction band of g-C3N4 is only the reaction site,demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2 MoO 6/Bi is through an indirect z-scheme structure.Thus,the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping,resulting in better optical absorption ability and a lower combination rate of photogenerated charge carriers.The findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.
基金supported by the National Science Foundation of China(91545117)the Natural Science Foundation of Liaoning Province(201602676)+1 种基金the Fundamental Research Funds for Colleges and Universities in Liaoning Province(LQN201703)the Startup Foundation for Doctors of Shenyang Normal University(BS201620)~~
文摘The electronic metal-support interaction(EMSI)is one of most intriguing phenomena in heterogeneous catalysis.In this work,this subtle effect is clearly demonstrated by density functional theory(DFT)calculations of single Pt atom supported on vacancies in a boron nitride nanosheet.Moreover,the relation between the EMSI and the performance of Pt in propane direct dehydrogenation(PDH)is investigated in detail.The charge state and partial density of states of single Pt atom show distinct features at different anchoring positions,such as boron and nitrogen vacancies(Bvac and Nvac,respectively).Single Pt atom become positively and negatively charged on Bvac and Nvac,respectively.Therefore,the electronic structure of Pt can be adjusted by rational deposition on the support.Moreover,Pt atoms in different charge states have been shown to have different catalytic abilities in PDH.The DFT calculations reveal that Pt atoms on Bvac(Pt-Bvac)have much higher reactivity towards reactant/product adsorption and C–H bond activation than Pt supported on Nvac(Pt-Nvac),with larger adsorption energy and lower barrier along the reaction pathway.However,the high reactivity of Pt-Bvac also hinders propene desorption,which could lead to unwanted deep dehydrogenation.Therefore,the results obtained herein suggest that a balanced reactivity for C–H activation in propane and propene desorption is required to achieve optimum yields.Based on this descriptor,a single Pt atom on a nitrogen vacancy is considered an effective catalyst for PDH.Furthermore,the deep dehydrogenation of the formed propene is significantly suppressed,owing to the large barrier on Pt-Nvac.The current work demonstrates that the catalytic properties of supported single Pt atoms can be tuned by rationally depositing them on a boron nitride nanosheet and highlights the great potential of single-atom catalysis in the PDH reaction.
基金supported by the National Key Projects for Fundamental Research and Development of China(2016YFB0600903)the National Natural Science Foundation of China(91434107,21506226,21476245)the Key Research Program of Frontier Sciences of Chinese Academy of Sciences(QYZDY-SSW-JSC011)~~
文摘A series of quaternary ammonium ionic liquids(ILs)were synthesized and employed as catalysts for the production of poly(isosorbide carbonate)(PIC)from diphenyl carbonate and isosorbide via a melt polycondensation process.The relationship between the anions of the ILs and the catalytic activities was investigated,and the readily‐prepared IL tetraethylammonium imidazolate(TEAI)was found to exhibit the highest catalytic activity.After optimizing the reaction conditions,a PIC with a weight‐average molecular weight(Mw)of25600g/mol was obtained,in conjunction with an isosorbide conversion of92%.As a means of modifying the molecular flexibility and thermal properties of the PIC,poly(aliphatic diol‐co‐isosorbide carbonate)s(PAIC)s were successfully synthesized,again using TEAI,and polymers with Mw values ranging from29000to112000g/mol were obtained.13C NMR analyses determined that the PAIC specimens had random microstructures,while differential scanning calorimetry demonstrated that each of the PAICs were amorphous and had glass transition temperatures ranging from50to115°C.Thermogravimetric analyses found Td‐5%values ranging from316to332°C for these polymers.Based on these data,it is evident that the incorporation of linear or cyclohexane‐based diol repeating units changed the thermal properties of the PIC.
基金supported by the National Natural Science Foundation of China(51572295,21273285,21003157)the Beijing Nova Program(2008B76)the Science Foundation of China University of Petroleum Beijing(KYJJ2012-06-20 and 2462016YXBS05)~~
文摘PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g^–1 h^–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g^–1 h^–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.
基金supported by the National Natural Science Foundation of China(21673142,21477164)the National High Technology Research and Development Program of China(863 Program,2015AA030903)~~
文摘Nanocatalysts consisting of three‐dimensionally ordered macroporous(3DOM)TiO2‐supported ultrafine Pd nanoparticles(Pd/3DOM‐TiO2‐GBMR)were readily fabricated by gas bubbling‐assisted membrane reduction(GBMR)method.These catalysts had a well‐defined and highly ordered macroporous nanostructure with an average pore size of 280 nm.In addition,ultrafine hemispherical Pd nanoparticles(NPs)with a mean particle size of 1.1 nm were found to be well dispersed over the surface of the 3DOM‐TiO2 support and deposited on the inner walls of the material.The nanostructure of the 3DOM‐TiO2 support ensured efficient contact between soot particles and the catalyst.The large interface area between the ultrafine Pd NPs and the TiO2 also increased the density of sites for O2 activation as a result of the strong metal(Pd)‐support(TiO2)interaction(SMSI).A Pd/3DOM‐TiO2‐GBMR catalyst with ultrafine Pd NPs(1.1 nm)exhibited higher catalytic activity during diesel soot combustion compared with that obtained from a specimen having relatively large Pd NPs(5.0 nm).The T10,T50 and T90 values obtained from the former were 295,370 and 415°C.Both the activity and nanostructure of the Pd/3DOM‐TiO2‐GBMR catalyst were stable over five replicate soot oxidation trials.These results suggest that nanocatalysts having a 3DOM structure together with ultrafine Pd NPs can decrease the amount of Pd required,and that this approach has potential practical applications in the catalytic combustion of diesel soot particles.
基金supported by the National Natural Science Foundation of China(51572295,21273285 and 21003157)Beijing Nova Program(2008B76)Science Foundation of China University of Petroleum Beijing(KYJJ2012-06-20 and 2462016YXBS05)~~
文摘Efficient composite semiconductor photocatalysts are highly desirable for the visible-light-driven degradation of organic pollutants. In this study, Bi24O31Cl10 photocatalyst was prepared via a hydrothermal method and modified with Pt nanoparticles (NPs) through a facile deposition procedure. The composite photocatalyst was characterized by X-ray diffraction, transmission electronic microscopy, X-ray photoelectron spectroscopy, UV-vis diffusion reflectance spectroscopy, photoluminescence spectroscopy, and electron spin resonance. The 1.0 wt% Pt/Bi24O31Cl10 photocatalyst showed the highest activity for the degradation of methyl orange under visible light (source: 300 W Xe lamp coupled with a UV-cutoff filter), and the photocatalytic degradation efficiency improved about 2.2 times compared to that of pure Bi24O31Cl10. The composite photocatalyst could maintain most of its activity after four runs of the photocatalytic experimental cycle. This study could provide a novel insight for the modification of other desirable semiconductor materials to achieve high photocatalytic activities.
文摘The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen energy.Metal‐organic frameworks(MOFs)are considered to be potential photocatalytic materials.Herein,monodisperse,small size,non‐precious metal transition metal phosphide Ni2P is encapsulated into a typical MOF(UiO‐66‐NH2)as a hybrid core‐shell cocatalyst to modify Zn_(0.5)Cd_(0.5)S for photocatalytic hydrogen production.Ni2P is wrapped in UiO‐66‐NH_(2)via an in situ solvothermal method,and Zn_(0.5)Cd_(0.5)S sulfide is decorated with a core‐shell Ni_(2)P@UiO‐66‐NH_(2)cocatalyst to obtain ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite materials.Photoelectric and chemical characterization confirms that the ternary composites have good kinetic hydrogen production performance.The hydrogen production rate of 10%10 mg Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S reaches 40.91 mmol·g^(–1)·h^(–1)with an apparent quantum efficiency at 420 nm of 13.57%.The addition of 10 mg Ni_(2)P@UiO‐66‐NH_(2)increases the surface area of the ternary material,providing abundant reaction sites and forming an efficient charge transfer channel,which is conducive to efficient hydrogen production by the ternary photocatalysts.It is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic reaction.This study provides a new perspective for the construction of high‐performance photocatalytic materials.
基金supported by the National Natural Science Foundation of China(No.41204094)Science Foundation of China University of Petroleum,Beijing(No.2462015YQ0506)
文摘In this paper, we propose a hybrid PML (H-PML) combining the normal absorption factor of convolutional PML (C-PML) with tangential absorption factor of Mutiaxial PML (M-PML). The H-PML boundary conditions can better suppress the numerical instability in some extreme models, and the computational speed of finite-element method and the dynamic range are greatly increased using this HPML. We use the finite-element method with a hybrid PML to model the acoustic reflection of the interface when wireline and well logging while drilling (LWD), in a formation with a reflector outside the borehole. The simulation results suggests that the PS- and SP- reflected waves arrive at the same time when the inclination between the well and the outer interface is zero, and the difference in arrival times increases with increasing dip angle. When there are fractures outside the well, the reflection signal is clearer in the subsequent reflection waves and may be used to identify the fractured zone. The difference between the dominant wavelength and the model scale shows that LWD reflection logging data are of higher resolution and quality than wireline acoustic reflection logging.
基金supported by the National Natural Science Foundation of China(No.41474109)the China National Petroleum Corporation under grant number 2016A-33
文摘Conventional time-space domain and frequency-space domain prediction filtering methods assume that seismic data consists of two parts, signal and random noise. That is, the so-called additive noise model. However, when estimating random noise, it is assumed that random noise can be predicted from the seismic data by convolving with a prediction error filter. That is, the source-noise model. Model inconsistencies, before and after denoising, compromise the noise attenuation and signal-preservation performances of prediction filtering methods. Therefore, this study presents an inversion-based time-space domain random noise attenuation method to overcome the model inconsistencies. In this method, a prediction error filter (PEF), is first estimated from seismic data; the filter characterizes the predictability of the seismic data and adaptively describes the seismic data's space structure. After calculating PEF, it can be applied as a regularized constraint in the inversion process for seismic signal from noisy data. Unlike conventional random noise attenuation methods, the proposed method solves a seismic data inversion problem using regularization constraint; this overcomes the model inconsistency of the prediction filtering method. The proposed method was tested on both synthetic and real seismic data, and results from the prediction filtering method and the proposed method are compared. The testing demonstrated that the proposed method suppresses noise effectively and provides better signal-preservation performance.
基金supported by the National High Technology Research and Development Program of China(863 Program,2015AA034603)the National Natural Science Foundation of China(21477146,21673142 and 21303263)+2 种基金the Beijing Nova Program(Z141109001814072)the Specialized Research Fund for the Doctoral Program of Higher Education(20130007120011)the Science Foundation of China University of Petroleum-Beijing(YJRC-2013-13,2462013BJRC003)~~
文摘A series of catalysts consisting of three‐dimensionally ordered macroporous(3DOM)x‐CeO2/Al2O3‐supported Au nanoparticles(x=2,10,20,and40wt%)were successfully synthesized using a reduction‐deposition method.These catalysts were characterized using scanning electron microscopy,the Brunauer‐Emmett‐Teller method,X‐ray diffraction,transmission electron microscopy,ultraviolet‐visible spectroscopy,and temperature‐programmed reduction by H2.Au nanoparticles of mean particle size5nm were well dispersed and supported on the inner walls of uniform macropores.The3DOM structure improved the contact efficiency between soot and the catalyst.An Al‐Ce‐O solid solution was formed in the multilayer support,i.e.,x‐CeO2/Al2O3,by the incorporation of Al3+ions into the CeO2lattice,which resulted in the creation of extrinsic oxygen vacancies.Strong interactions between the metal(Au)and the support(Ce)increased the amount of active oxygen species,and this promoted soot oxidation.The catalytic performance in soot combustion was evaluated using a temperature‐programmed oxidation technique.The presence of CeO2nanolayers in the3DOM Au/x‐CeO2/Al2O3catalysts clearly improved the catalytic activities in soot oxidation.Among the prepared catalysts,3DOM Au/20%CeO2/Al2O3showed high catalytic activity and stability in diesel soot oxidation.
基金supported by the Special Fund of the Institute of Geophysics,China Earthquake Administration(Nos.DQJB19B02 and DQJB17T04)
文摘The quality factor(or Q value)is an important parameter for characterizing the inelastic properties of rock.Achieving a Q value estimation with high accuracy and stability is still challenging.In this study,a new method for estimating ultrasonic attenuation using a spectral ratio based on an S transform(SR-ST)is presented to improve the stability and accuracy of Q estimation.The variable window of ST is used to solve the time window problem.We add two window factors to the Gaussian window function in the ST.The window factors can adjust the scale of the Gaussian window function to the ultrasonic signal,which reduces the calculation error attributed to the conventional Gaussian window function.Meanwhile,the frequency bandwidth selection rules for the linear regression of the amplitude ratio are given to further improve stability and accuracy.First,the feasibility and influencing factors of the SR-ST method are studied through numerical testing and standard sample experiments.Second,artificial samples with different Q values are used to study the adaptability and stability of the SR-ST method.Finally,a further comparison between the new method and the conventional spectral ratio method(SR)is conducted using rock field samples,again addressing stability and accuracy.The experimental results show that this method will yield an error of approximately 36%using the conventional Gaussian window function.This problem can be solved by adding the time window factors to the Gaussian window function.The frequency bandwidth selection rules and mean slope value of the amplitude ratio used in the SR-ST method can ensure that the maximum error of different Q values estimation(Q>15)is less than 10%.
基金supported by the NSFC and Sinopec Joint Key Project(No.U1663207)National Science and Technology Major Project(No.2017ZX05049-002)National 973 Program(No.2014CB239104)
文摘The construction of a shale rock physics model and the selection of an appropriate brittleness index (B/) are two significant steps that can influence the accuracy of brittleness prediction. On one hand, the existing models of kerogen-rich shale are controversial, so a reasonable rock physics model needs to be built. On the other hand, several types of equations already exist for predicting the BI whose feasibility needs to be carefully considered. This study constructed a kerogen-rich rock physics model by performing the self- consistent approximation and the differential effective medium theory to model intercoupled clay and kerogen mixtures. The feasibility of our model was confirmed by comparison with classical models, showing better accuracy. Templates were constructed based on our model to link physical properties and the BL Different equations for the BI had different sensitivities, making them suitable for different types of formations. Equations based on Young's Modulus were sensitive to variations in lithology, while those using Lame's Coefficients were sensitive to porosity and pore fluids. Physical information must be considered to improve brittleness prediction.
基金supported by the National Natural Science Foundation of China(No.41474110)
文摘Edge reflections are inevitable in numerical modeling of seismic wavefields, and they are usually attenuated by absorbing boundary conditions. However, the commonly used perfectly matched layer (PML) boundary condition requires special treatment for the absorbing zone, and in three-dimensional (3D) modeling, it has to split each variable into three corresponding variables, which increases the computing time and memory storage. In contrast, the hybrid absorbing boundary condition (HABC) has the advantages such as ease of implementation, less computation time, and near-perfect absorption; it is thus able to enhance the computational efficiency of 3D elastic wave modeling. In this study, a HABC is developed from two-dimensional (2D) modeling into 3D modeling based on the I st Higdon one way wave equations, and a HABC is proposed that is suitable for a 3D elastic wave numerical simulation. Numerical simulation results for a homogenous model and a complex model indicate that the proposed HABC method is more effective and has better absorption than the traditional PML method.
文摘Photocatalysis is considered a prospective way to alleviate the energy crisis and environmental pollution.It is therefore extremely important to design highly efficient photocatalysts for catalytic systems.In recent years,hollow‐structured materials have attracted considerable interest for application in energy conversion fields owing to their large specific surface areas,improved light absorption,and shortened charge carrier transfer path.Because they contain inner and outer surfaces,hollow‐structured materials can provide a superior platform for the deposition of other components.A number of hollow‐structured hierarchical systems have been designed and fabricated in recent decades.It is important to rationally design and construct complex hierarchical structures.In this review,general preparation approaches for hollow‐structured materials are presented,followed by a summary of the recent synthesis methods and mechanisms of typical hollow‐structured materials for applications in the photocatalytic field.Complex hollow‐structured hierarchical photocatalysts are classified into two types,hollow cocatalyst‐based and hollow host photocatalyst‐based,and the design principle and analysis of the photocatalytic reaction mechanism for photocatalytic H2 evolution and CO_(2) reduction are also introduced.The effects of hollow‐structured materials have also been investigated.This review provides a reference for the rational construction of advanced,highly efficient photocatalytic materials.
基金Projects(51571211,51731010,51471028) supported by the National Natural Science Foundation of ChinaProject(DP160105066) supported by Australian Research Council
文摘The corrosion behavior of electrodeposited Ni with normal and bimodal grain size distribution was investigated.The microstructure of samples was researched by SEM,EBSD,TEM and XRD.The corrosion behavior was studied by potentiodynamic tests and electrochemical impedance.Nanocrystalline Ni with(100)and(111)textures was prepared by an electrodeposition method.The Ni samples with different grain size distributions and twins were then obtained by heat treatment of nanocrystalline Ni at different temperatures.The effect of grain size on corrosion behavior of the sample depends on the ability of the environment to passivate.In the case where passive film forms on the sample surface,the corrosion resistance of the sample increases with decreasing grain size.Conversely,the corrosion resistance decreases with decreasing grain size when there is no passivation.The corrosion behavior of samples with bimodal grain size distribution obeys the rule of mixture.