Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))aroun...Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))around the oxygen vacancies.The origin of the enhanced catalytic activity of ZrO_(2)with defective tetrahedral Zr sites was examined by direct comparison with its pristine counterpart in the current study.Electronic-structure analysis revealed that electrons from oxygen removal were localized within vacancies on the defective surface,which directly attacked the C-H bond in propane.The involvement of localized electrons activates the C-H bond via back-donation to the antibonding orbital on the defective surface;conversely,charge is transferred from propane to the pristine surfaces.The barrier for the first C-H bond activation is clearly significantly reduced on the defective surfaces compared to that on the pristine surfaces,which verifies the superior activity of Zr_(cus).Notably,however,the desorption of both propene and hydrogen molecules from Zr_(cus)is more difficult due to strong binding.The calculated turnover frequency(TOF)for propene formation demonstrates that the pristine surfaces exhibit better catalytic performance at lower temperatures,whereas the defective surfaces have a larger TOF at high temperatures.However,the rate-determining step and reaction order on the defective surface differ from those on the pristine surface,which corroborates that the catalysts follow different mechanisms.A further optimization strategy was proposed to address the remaining bottlenecks in propane dehydrogenation on zirconium oxide.展开更多
Low-frequency vibroseis acquisition has become a routine operation in land seismic surveys,given the advantages of low-frequency signals in characterizing geological structures and enhancing the imaging of deep explor...Low-frequency vibroseis acquisition has become a routine operation in land seismic surveys,given the advantages of low-frequency signals in characterizing geological structures and enhancing the imaging of deep exploration targets.The two key points of low-frequency sweep design techniques include controlling the distortion and improving the output energy during the low-frequency stage.However,the vibrators are limited by the maximum fl ow provided by the hydraulic systems at the low-frequency stage,causing diffi culty in satisfying exploration energy requirements.Initially,a theoretical analysis of the low-frequency acquisition performance of vibrators is conducted.A theoretical maximum output force below 10 Hz is obtained by guiding through theoretical formulas and combining actual vibrator parameters.Then,the signal is optimized according to the surface characteristics of the operation area.Finally,detailed application quality control and operational procedures are established.The new low-frequency sweep design method has overcome the maximum flow limitations of the hydraulic system,increased the low-frequency energy,and achieved broadband acquisition.The designed signal has been tested and applied on various types of ground surfaces in the Middle East desert region,yielding good performance.The proposed low-frequency sweep design method holds considerable value for the application of conventional vibroseis in low-frequency acquisition.展开更多
Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare ...Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare sub-nanometric Pt clusters(~0.8 nm)encapsulated within the defects of CeO_(2)nanorods via an in-situ defect engineering methodology.The as-prepared Pt@d-CeO_(2)catalyst significantly boosts the activity and stability in the water-gas shift(WGS)reaction compared to other analogs.Based on controlled experiments and complementary(in-situ)spectroscopic studies,a reversible encapsulation induced by active site transformation between the Pt^(2+)-terminal hydroxyl and Pt^(δ+)-O vacancy species at the interface is revealed,which enables to evoke the enhanced performance.Our findings not only offer practical guidance for the design of high-efficiency catalysts but also bring a new understanding of the exceptional performance of WGS in a holistic view,which shows a great application potential in materials and catalysis.展开更多
The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts hav...The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.展开更多
The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulati...The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulations of ethane dehydrogenation over Co@BEA zeolite at different temperatures.AIMD simulations showed that a sharp decrease in free energy barrier as temperature increased.Our analysis of the temperature dependence of activation free energies uncovered an unusual entropic effect accompanying the reaction.The unique spatial structures around the Co active site at different temperatures influenced both the extent of charge transfer in the transition state and the arrangement of 3d orbital energy levels.We provided explanations consistent with the principles of thermodynamics and statistical physics.The insights gained at the atomic level have offered a fresh interpretation of the intricate long-range interplay between local chemical reactions and extensive chemical environments.展开更多
Petroleum asphalt,an important by-product of the petrochemical industry,has diverse applications but often suffers from low industrial added value.Because of its low cost,high carbon content,and high polycyclic aromat...Petroleum asphalt,an important by-product of the petrochemical industry,has diverse applications but often suffers from low industrial added value.Because of its low cost,high carbon content,and high polycyclic aromatic hydrocarbon content,appropriate modification can increase its value and expand its energy storage applications.Current research progress on the common preparation methods of petroleum asphalt-based carbon materials,including template-assisted pyrolysis,molten salt treatment,activation,heteroatom doping,and pre-oxidation is reviewed,and its use in supercapacitors and alkali metal ion batteries,is also elaborated.Feasible solutions for the current problems with petroleum asphalt are proposed,with the aim of providing insights into its high value-added utilization.展开更多
Wavelet estimation is an important part of high-resolution seismic data processing.However,itis difficult to preserve the lateral continuity of geological structures and eff ectively recover weak geologicalbodies usin...Wavelet estimation is an important part of high-resolution seismic data processing.However,itis difficult to preserve the lateral continuity of geological structures and eff ectively recover weak geologicalbodies using conventional deterministic wavelet inversion methods,which are based on the joint inversionof wells with seismic data.In this study,starting from a single well,on the basis of the theory of single-welland multi-trace convolution,we propose a steady-state seismic wavelet extraction method for synchronizedinversion using spatial multi-well and multi-well-side seismic data.The proposed method uses a spatiallyvariable weighting function and wavelet invariant constraint conditions with particle swarm optimization toextract the optimal spatial seismic wavelet from multi-well and multi-well-side seismic data to improve thespatial adaptability of the extracted wavelet and inversion stability.The simulated data demonstrate that thewavelet extracted using the proposed method is very stable and accurate.Even at a low signal-to-noise ratio,the proposed method can extract satisfactory seismic wavelets that refl ect lateral changes in structures andweak eff ective geological bodies.The processing results for the field data show that the deconvolution resultsimprove the vertical resolution and distinguish between weak oil and water thin layers and that the horizontaldistribution characteristics are consistent with the log response characteristics.展开更多
Digital radiographic(DR)testing equipment has been widely promoted and applied in the inspection of circumferential welds in oil and gas pipelines.In order to establish a comprehensive quality control system for digit...Digital radiographic(DR)testing equipment has been widely promoted and applied in the inspection of circumferential welds in oil and gas pipelines.In order to establish a comprehensive quality control system for digital radiographic testing and fully evaluate the integrated system inspection ability of equipment,personnel,and processes,a scientific and standardized evaluation method to the system is very necessary.Here investigates the precedents of relevant non-destructive testing evaluation methods at home and abroad,considers the testing characteristics of DR equipment,develops a complete set of DR testing system evaluation procedures.It deeply studies the adaptability methods of program processes from defect production to slicing processing and data statistical calculation for digital radiographic testing evaluation.To check the repeatability and reliability of the detectable system,five process welds with 200 real metallographic defects were fabricated in the laboratory.From the detected results,the DR system has good repeatability in image quality,and the detectable defect size reaches 0.85 mm under achieving 90%detection probability at a confidence level of 95%,the error of detected defect length is±2 mm,and the error of detected defect localization is±5 mm.The qualitative and quantitative detection of defects are accurate and reliable.The test further confirmed the reliable detection ability of the DR detection system,and fully validated the scientific and practical evaluation method designed.The research on the evaluation test method can serve as an important link in the quality control system for the on-site application of digital ray equipment in long-distance pipelines.The designed program,test,and evaluation content can serve as an important basis for the formulation of relevant specifications or standards.展开更多
文摘Recent studies have revealed the extraordinary performance of zirconium oxide in propane dehydrogenation,which is attributed to the excellent reactivity of the coordinatively unsaturated zirconium sites(Zr_(cus))around the oxygen vacancies.The origin of the enhanced catalytic activity of ZrO_(2)with defective tetrahedral Zr sites was examined by direct comparison with its pristine counterpart in the current study.Electronic-structure analysis revealed that electrons from oxygen removal were localized within vacancies on the defective surface,which directly attacked the C-H bond in propane.The involvement of localized electrons activates the C-H bond via back-donation to the antibonding orbital on the defective surface;conversely,charge is transferred from propane to the pristine surfaces.The barrier for the first C-H bond activation is clearly significantly reduced on the defective surfaces compared to that on the pristine surfaces,which verifies the superior activity of Zr_(cus).Notably,however,the desorption of both propene and hydrogen molecules from Zr_(cus)is more difficult due to strong binding.The calculated turnover frequency(TOF)for propene formation demonstrates that the pristine surfaces exhibit better catalytic performance at lower temperatures,whereas the defective surfaces have a larger TOF at high temperatures.However,the rate-determining step and reaction order on the defective surface differ from those on the pristine surface,which corroborates that the catalysts follow different mechanisms.A further optimization strategy was proposed to address the remaining bottlenecks in propane dehydrogenation on zirconium oxide.
基金The authors would like to express their sincere appreciation to the research project of CNPC Geophysical Key Lab(2022DQ0604-4)National Natural Science Foundation of China(Grant No.42074141).
文摘Low-frequency vibroseis acquisition has become a routine operation in land seismic surveys,given the advantages of low-frequency signals in characterizing geological structures and enhancing the imaging of deep exploration targets.The two key points of low-frequency sweep design techniques include controlling the distortion and improving the output energy during the low-frequency stage.However,the vibrators are limited by the maximum fl ow provided by the hydraulic systems at the low-frequency stage,causing diffi culty in satisfying exploration energy requirements.Initially,a theoretical analysis of the low-frequency acquisition performance of vibrators is conducted.A theoretical maximum output force below 10 Hz is obtained by guiding through theoretical formulas and combining actual vibrator parameters.Then,the signal is optimized according to the surface characteristics of the operation area.Finally,detailed application quality control and operational procedures are established.The new low-frequency sweep design method has overcome the maximum flow limitations of the hydraulic system,increased the low-frequency energy,and achieved broadband acquisition.The designed signal has been tested and applied on various types of ground surfaces in the Middle East desert region,yielding good performance.The proposed low-frequency sweep design method holds considerable value for the application of conventional vibroseis in low-frequency acquisition.
文摘Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare sub-nanometric Pt clusters(~0.8 nm)encapsulated within the defects of CeO_(2)nanorods via an in-situ defect engineering methodology.The as-prepared Pt@d-CeO_(2)catalyst significantly boosts the activity and stability in the water-gas shift(WGS)reaction compared to other analogs.Based on controlled experiments and complementary(in-situ)spectroscopic studies,a reversible encapsulation induced by active site transformation between the Pt^(2+)-terminal hydroxyl and Pt^(δ+)-O vacancy species at the interface is revealed,which enables to evoke the enhanced performance.Our findings not only offer practical guidance for the design of high-efficiency catalysts but also bring a new understanding of the exceptional performance of WGS in a holistic view,which shows a great application potential in materials and catalysis.
文摘The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.
文摘The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulations of ethane dehydrogenation over Co@BEA zeolite at different temperatures.AIMD simulations showed that a sharp decrease in free energy barrier as temperature increased.Our analysis of the temperature dependence of activation free energies uncovered an unusual entropic effect accompanying the reaction.The unique spatial structures around the Co active site at different temperatures influenced both the extent of charge transfer in the transition state and the arrangement of 3d orbital energy levels.We provided explanations consistent with the principles of thermodynamics and statistical physics.The insights gained at the atomic level have offered a fresh interpretation of the intricate long-range interplay between local chemical reactions and extensive chemical environments.
文摘Petroleum asphalt,an important by-product of the petrochemical industry,has diverse applications but often suffers from low industrial added value.Because of its low cost,high carbon content,and high polycyclic aromatic hydrocarbon content,appropriate modification can increase its value and expand its energy storage applications.Current research progress on the common preparation methods of petroleum asphalt-based carbon materials,including template-assisted pyrolysis,molten salt treatment,activation,heteroatom doping,and pre-oxidation is reviewed,and its use in supercapacitors and alkali metal ion batteries,is also elaborated.Feasible solutions for the current problems with petroleum asphalt are proposed,with the aim of providing insights into its high value-added utilization.
文摘Wavelet estimation is an important part of high-resolution seismic data processing.However,itis difficult to preserve the lateral continuity of geological structures and eff ectively recover weak geologicalbodies using conventional deterministic wavelet inversion methods,which are based on the joint inversionof wells with seismic data.In this study,starting from a single well,on the basis of the theory of single-welland multi-trace convolution,we propose a steady-state seismic wavelet extraction method for synchronizedinversion using spatial multi-well and multi-well-side seismic data.The proposed method uses a spatiallyvariable weighting function and wavelet invariant constraint conditions with particle swarm optimization toextract the optimal spatial seismic wavelet from multi-well and multi-well-side seismic data to improve thespatial adaptability of the extracted wavelet and inversion stability.The simulated data demonstrate that thewavelet extracted using the proposed method is very stable and accurate.Even at a low signal-to-noise ratio,the proposed method can extract satisfactory seismic wavelets that refl ect lateral changes in structures andweak eff ective geological bodies.The processing results for the field data show that the deconvolution resultsimprove the vertical resolution and distinguish between weak oil and water thin layers and that the horizontaldistribution characteristics are consistent with the log response characteristics.
文摘Digital radiographic(DR)testing equipment has been widely promoted and applied in the inspection of circumferential welds in oil and gas pipelines.In order to establish a comprehensive quality control system for digital radiographic testing and fully evaluate the integrated system inspection ability of equipment,personnel,and processes,a scientific and standardized evaluation method to the system is very necessary.Here investigates the precedents of relevant non-destructive testing evaluation methods at home and abroad,considers the testing characteristics of DR equipment,develops a complete set of DR testing system evaluation procedures.It deeply studies the adaptability methods of program processes from defect production to slicing processing and data statistical calculation for digital radiographic testing evaluation.To check the repeatability and reliability of the detectable system,five process welds with 200 real metallographic defects were fabricated in the laboratory.From the detected results,the DR system has good repeatability in image quality,and the detectable defect size reaches 0.85 mm under achieving 90%detection probability at a confidence level of 95%,the error of detected defect length is±2 mm,and the error of detected defect localization is±5 mm.The qualitative and quantitative detection of defects are accurate and reliable.The test further confirmed the reliable detection ability of the DR detection system,and fully validated the scientific and practical evaluation method designed.The research on the evaluation test method can serve as an important link in the quality control system for the on-site application of digital ray equipment in long-distance pipelines.The designed program,test,and evaluation content can serve as an important basis for the formulation of relevant specifications or standards.
