Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further de...Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.展开更多
Pseudo-capacitive negative electrodes remain a major bottleneck in the development of supercapacitor devices with high energy density because the electric double-layer capacitance of the negative electrodes does not m...Pseudo-capacitive negative electrodes remain a major bottleneck in the development of supercapacitor devices with high energy density because the electric double-layer capacitance of the negative electrodes does not match the pseudocapacitance of the corresponding positive electrodes.In the present study,a strategically improved Ni-Co-Mo sulfide is demonstrated to be a promising candidate for high energy density supercapattery devices due to its sustained pseudocapacitive charge storage mechanism.The pseudocapacitive behavior is enhanced when operating under a high current through the addition of a classical Schottky junction next to the electrode-electrolyte interface using atomic layer deposition.The Schottky junction accelerates and decelerates the diffusion of OH-/K+ions during the charging and discharging processes,respectively,to improve the pseudocapacitive behavior.The resulting pseudocapacitive negative electrodes exhibits a specific capacity of 2,114 C g^(-1)at 2 A g^(-1)matches almost that of the positive electrode’s 2,795 C g^(-1)at 3 A g^(-1).As a result,with the equivalent contribution from the positive and negative electrodes,an energy density of 236.1 Wh kg^(-1)is achieved at a power density of 921.9 W kg^(-1)with a total active mass of 15 mg cm-2.This strategy demonstrates the possibility of producing supercapacitors that adapt well to the supercapattery zone of a Ragone plot and that are equal to batteries in terms of energy density,thus,offering a route for further advances in electrochemical energy storage and conversion processes.展开更多
Gas atomization has been studied by using energy method in this paper. It shows that the capillary potential energy of the atomization droplets is supplied by the impingement of the gas on the liquid. The energy crite...Gas atomization has been studied by using energy method in this paper. It shows that the capillary potential energy of the atomization droplets is supplied by the impingement of the gas on the liquid. The energy criterion of the minimum equivalent diameter of the atomization droplets is obtained. The result is comparable to the empirical formulae.[HJ*2/3]展开更多
In view of the difficulty in calculating the atomic structure parameters of high-Z elements,the Hartree–Fock with relativistic corrections(HFR)theory in combination with the ridge regression(RR)algorithm rather than ...In view of the difficulty in calculating the atomic structure parameters of high-Z elements,the Hartree–Fock with relativistic corrections(HFR)theory in combination with the ridge regression(RR)algorithm rather than the Cowan code’s least squares fitting(LSF)method is proposed and applied.By analyzing the energy level structure parameters of the HFR theory and using the fitting experimental energy level extrapolation method,some excited state energy levels of the Yb I(Z=70)atom including the 4f open shell are calculated.The advantages of the ridge regression algorithm are demonstrated by comparing it with Cowan code’s LSF results.In addition,the results obtained by the new method are compared with the experimental results and other theoretical results to demonstrate the reliability and accuracy of our approach.展开更多
Layered backfill is commonly used in mining operations,and its mechanical behavior is strongly influenced by delamination parameters.In this study,13 specimens with different numbers of delamination and delamination a...Layered backfill is commonly used in mining operations,and its mechanical behavior is strongly influenced by delamination parameters.In this study,13 specimens with different numbers of delamination and delamination angle were prepared to investigate the anisotropic mechanical behavior,energy dissipation characteristics and crack development of backfill.P-wave velocity,uniaxial compression,scanning electron microscope(SEM),and acoustic emission(AE)experiments were conducted.The results indicate that:(1)The P-wave velocity has linear and elliptical relationships with the number of delamination surface and delamination angle,respectively;the strength,delamination parameters and P-wave velocity show a high degree of coincidence in terms of their function relationship,which can realize the rapid prediction of strength.(2)The microstructure of the delaminated surface is looser than that of the matrix,leading to a decrease in strength and an increase at the pore-fissure compaction stage.The number and angle of delamination increase linearly with the anisotropy coefficient.(3)The energy evolution in angle-cut backfill can be divided into four stages,with a decrease in the proportion of elastic energy at the initiation stress and peak stress with increasing number of delamination planes and delamination angle.(4)Crack development increases with the number of delamination surface and delamination angle,resulting in a decrease in energy dissipation coefficient and peak AE energy.These findings provide valuable insights for the design of filling materials and processes in mining operations.展开更多
基金support from the Shenzhen Science and Technology Program(No.KQTD20190929173914967,ZDSYS20220527171401003,and JCYJ20200109110416441).
文摘Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.
基金financially supported by the National Research Foundation of Korea(NRF-2022R1A2C2010803)。
文摘Pseudo-capacitive negative electrodes remain a major bottleneck in the development of supercapacitor devices with high energy density because the electric double-layer capacitance of the negative electrodes does not match the pseudocapacitance of the corresponding positive electrodes.In the present study,a strategically improved Ni-Co-Mo sulfide is demonstrated to be a promising candidate for high energy density supercapattery devices due to its sustained pseudocapacitive charge storage mechanism.The pseudocapacitive behavior is enhanced when operating under a high current through the addition of a classical Schottky junction next to the electrode-electrolyte interface using atomic layer deposition.The Schottky junction accelerates and decelerates the diffusion of OH-/K+ions during the charging and discharging processes,respectively,to improve the pseudocapacitive behavior.The resulting pseudocapacitive negative electrodes exhibits a specific capacity of 2,114 C g^(-1)at 2 A g^(-1)matches almost that of the positive electrode’s 2,795 C g^(-1)at 3 A g^(-1).As a result,with the equivalent contribution from the positive and negative electrodes,an energy density of 236.1 Wh kg^(-1)is achieved at a power density of 921.9 W kg^(-1)with a total active mass of 15 mg cm-2.This strategy demonstrates the possibility of producing supercapacitors that adapt well to the supercapattery zone of a Ragone plot and that are equal to batteries in terms of energy density,thus,offering a route for further advances in electrochemical energy storage and conversion processes.
文摘Gas atomization has been studied by using energy method in this paper. It shows that the capillary potential energy of the atomization droplets is supplied by the impingement of the gas on the liquid. The energy criterion of the minimum equivalent diameter of the atomization droplets is obtained. The result is comparable to the empirical formulae.[HJ*2/3]
基金This work was supported by the National Natural Science Foundation of China （No.10676025） and the Research Fund of the Education Bureau of Gansu Province of China （No.3ZS061-A25-029）.
基金the Fundamental Research Funds for the Central Universities(Grant No.10822041A2038).
文摘In view of the difficulty in calculating the atomic structure parameters of high-Z elements,the Hartree–Fock with relativistic corrections(HFR)theory in combination with the ridge regression(RR)algorithm rather than the Cowan code’s least squares fitting(LSF)method is proposed and applied.By analyzing the energy level structure parameters of the HFR theory and using the fitting experimental energy level extrapolation method,some excited state energy levels of the Yb I(Z=70)atom including the 4f open shell are calculated.The advantages of the ridge regression algorithm are demonstrated by comparing it with Cowan code’s LSF results.In addition,the results obtained by the new method are compared with the experimental results and other theoretical results to demonstrate the reliability and accuracy of our approach.
文摘Layered backfill is commonly used in mining operations,and its mechanical behavior is strongly influenced by delamination parameters.In this study,13 specimens with different numbers of delamination and delamination angle were prepared to investigate the anisotropic mechanical behavior,energy dissipation characteristics and crack development of backfill.P-wave velocity,uniaxial compression,scanning electron microscope(SEM),and acoustic emission(AE)experiments were conducted.The results indicate that:(1)The P-wave velocity has linear and elliptical relationships with the number of delamination surface and delamination angle,respectively;the strength,delamination parameters and P-wave velocity show a high degree of coincidence in terms of their function relationship,which can realize the rapid prediction of strength.(2)The microstructure of the delaminated surface is looser than that of the matrix,leading to a decrease in strength and an increase at the pore-fissure compaction stage.The number and angle of delamination increase linearly with the anisotropy coefficient.(3)The energy evolution in angle-cut backfill can be divided into four stages,with a decrease in the proportion of elastic energy at the initiation stress and peak stress with increasing number of delamination planes and delamination angle.(4)Crack development increases with the number of delamination surface and delamination angle,resulting in a decrease in energy dissipation coefficient and peak AE energy.These findings provide valuable insights for the design of filling materials and processes in mining operations.
