The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/...The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/Co3O4 nanoparticles coupled with N-doped carbon hybrids(Ni/Co3O4@NC) were synthesized via a facile impregnation-calcination method as efficient electrocatalysts for OER in alkaline media. Notably, the impregnation of the polymer with Ni and Co ions in the first step ensured the homogeneous distribution of metals, thus guaranteeing the subsequent in situ calcination reaction, which produced well-dispersed Ni and Co3O4 nanoparticles. Moreover, the N-doped carbon matrix formed at high temperatures could effectively prevent the aggregation and coalescence, and regulate the electronic configuration of active species. Benefiting from the synergistic effect between the Ni, Co3O4, and NC species, the obtained Ni/Co3O4@NC hybrids exhibited enhanced OER activities and remarkable stability in an alkaline solution with a smaller overpotential of 350 m V to afford 10 m A cm-2, lower Tafel slope of 52.27 m V dec-1, smaller charge-transfer resistance, and higher double-layer capacitance of 25.53 m F cm-2 compared to those of unary Co3O4@NC or Ni@NC metal hybrids. Therefore, this paper presents a facile strategy for designing other heteroatom-doped oxides coupled with ideal carbon materials as electrocatalysts for the OER.展开更多
Metal doping for active sites exhibits remarkable potential for improving the hydrogen evolution reaction(HER).Multi-doping and the use of a conductive substrate can further modulate catalytic performance.Herein,Nb-Co...Metal doping for active sites exhibits remarkable potential for improving the hydrogen evolution reaction(HER).Multi-doping and the use of a conductive substrate can further modulate catalytic performance.Herein,Nb-CoSe well dispersed in N-doped carbon nanospheres(NCs,Nb-CoSe@NC)was synthesized to serve as a conductive substrate and facilitated good dispersion of active sites for the HER.Nb doping can also change the electronic structure of CoSe,which facilitates the activity for the HER.In order to further improve the conductivity and intrinsic activity of Nb-CoSe@NC,dual,nonmetal doping was realized through gas sulfurization to prepare hierarchical Nb-CoSeS@NC.The prepared Nb-CoSeS@NC,with a core-shell structure,exhibited a low overpotential of 115 mV at 10 mA cm–2,which is smaller than that of the most doped catalysts.In addition,NCs not only improved the dispersion and conductivity of the catalyst but also prevented metal corrosion in an electrolyte,thus facilitating the long-term stability of Nb-CoSeS@NC.Moreover,the synergistic effect of the multi-doping of Nb,S,and Se was explained.This work provides a promising,multi-doping strategy for the large-scale application of transition-metal-based electrocatalysts for the HER.展开更多
The fi rst arrival waveform inversion(FAWI)has a strong nonlinearity due to the objective function using L2 parametrization.When the initial velocity is not accurate,the inversion can easily fall into local minima.In ...The fi rst arrival waveform inversion(FAWI)has a strong nonlinearity due to the objective function using L2 parametrization.When the initial velocity is not accurate,the inversion can easily fall into local minima.In the full waveform inversion method,adding a cross-correlation function to the objective function can eff ectively reduce the nonlinearity of the inversion process.In this paper,the nonlinearity of this process is reduced by introducing the correlation objective function into the FAWI and by deriving the corresponding gradient formula.We then combine the first-arrival wave travel-time tomography with the FAWI to form a set of inversion processes.This paper uses the limited memory Broyden-Fletcher-Goldfarb-Shanno(L-BFGS)algorithm to improve the computational effi ciency of inversion and solve the problem of the low effi ciency of the FAWI method.The overthrust model and fi eld data test show that the method used in this paper can eff ectively reduce the nonlinearity of inversion and improve the inversion calculation effi ciency at the same time.展开更多
To meet the current energy needs of society,the highly efficient and continuous production of clean energy is required.One of the key issues facing the green hydrogen evolution is the construction of efficient,low-cos...To meet the current energy needs of society,the highly efficient and continuous production of clean energy is required.One of the key issues facing the green hydrogen evolution is the construction of efficient,low-cost electrocatalysts.Prussian blue(PB),Prussian blue analogs(PBAs),and their derivatives have tunable metal centers and have attracted significant interest as novel photo-and electrochemical catalysts.In this review,recent research progress into PB/PBA-based hollow structures,substrate-supported nanostructures,and their derivatives for green water splitting is discussed and summarized.First,several remarkable examples of nanostructured PB/PBAs supported on substrates(copper foil,carbon cloth,and nickel foam)and hollow structures(such as single-shelled hollow boxes,open hollow cages,and intricate hollow structures(multi-shell and yolk-shell))are discussed in detail,including their synthesis and formation mechanisms.Subsequently,the applications of PB/PBA derivatives((hydr)oxides,phosphides,chalcogenides,and carbides)for water splitting are discussed.Finally,the limitations in this research area and the most urgent challenges are summarized.We hope that this review will stimulate more researchers to develop technologies based on these intricate PB/PBA structures and their derivatives for highly efficient,green water splitting.展开更多
A rod-like NiCo2O4 modified glassy carbon electrode was fabricated and used for non-enzymatic glucose sensing. The NiCo2O4 was prepared by a facile hydrothermal reaction and subsequently treated in a commercial microw...A rod-like NiCo2O4 modified glassy carbon electrode was fabricated and used for non-enzymatic glucose sensing. The NiCo2O4 was prepared by a facile hydrothermal reaction and subsequently treated in a commercial microwave oven to eliminate the residual water introduced during the hydrothermal procedure. Structural analysis showed that there was no significant structural alteration before and after microwave treatment. The elimination of water residuals was confirmed by the stoichiometric ratio change by using element analysis. The microwave treated NiCo2O4 (M-NiCo2O4) showed excellent performance as a glucose sensor (sensitivity 431.29 μA·mmol/L-1·cm-2). The sensing performance decreases dramatically by soaking the M-NiCo2O4 in water. This result indicates that the introduction of residual water during hydrothermal process strongly affects the electrochemical performance and microwave pre-treatment is crucial for better sensory performance.展开更多
The full-waveform inversion method is a high-precision inversion method based on the minimization of the misfit between the synthetic seismograms and the observed data.However,this method suffers from cycle skipping i...The full-waveform inversion method is a high-precision inversion method based on the minimization of the misfit between the synthetic seismograms and the observed data.However,this method suffers from cycle skipping in the time domain or phase wrapping in the frequency because of the inaccurate initial velocity or the lack of low-frequency information.furthermore,the object scale of inversion is affected by the observation system and wavelet bandwidth,the inversion for large-scale structures is a strongly nonlinear problem that is considerably difficult to solve.In this study,we modify the unwrapping algorithm to obtain accurate unwrapped instantaneous phase,then using this phase conducts the inversion for reducing the strong nonlinearity.The normal instantaneous phases are measured as modulo 2π,leading the loss of true phase information.The path integral algorithm can be used to unwrap the instantaneous phase of the seismograms having time series and onedimensional(1 D)signal characteristics.However,the unwrapped phase is easily affected by the numerical simulation and phase calculations,resulting in the low resolution of inversion parameters.To increase the noise resistance and ensure the inversion accuracy,we present an improved unwrapping method by adding an envelope into the path integral unwrapping algorithm for restricting the phase mutation points,getting accurate instantaneous phase.The objective function constructed by unwrapping instantaneous phase is less affected by the local minimum,thereby making it suitable for full-waveform inversion.Further,the corresponding instantaneous phase inversion formulas are provided.Using the improved algorithm,we can invert the low-wavenumber components of the underneath structure and ensure the accuracy of the inverted velocity.Finally,the numerical tests of the 2 D Marmousi model and 3 D SEG/EAGE salt model prove the accuracy of the proposed algorithm and the ability to restore largescale low-wavenumber structures,respectively.展开更多
文摘The most energy-inefficient step in the oxygen evolution reaction(OER), which involves a complicated four-electron transfer process, limits the efficiency of the electrochemical water splitting. Here, well-defined Ni/Co3O4 nanoparticles coupled with N-doped carbon hybrids(Ni/Co3O4@NC) were synthesized via a facile impregnation-calcination method as efficient electrocatalysts for OER in alkaline media. Notably, the impregnation of the polymer with Ni and Co ions in the first step ensured the homogeneous distribution of metals, thus guaranteeing the subsequent in situ calcination reaction, which produced well-dispersed Ni and Co3O4 nanoparticles. Moreover, the N-doped carbon matrix formed at high temperatures could effectively prevent the aggregation and coalescence, and regulate the electronic configuration of active species. Benefiting from the synergistic effect between the Ni, Co3O4, and NC species, the obtained Ni/Co3O4@NC hybrids exhibited enhanced OER activities and remarkable stability in an alkaline solution with a smaller overpotential of 350 m V to afford 10 m A cm-2, lower Tafel slope of 52.27 m V dec-1, smaller charge-transfer resistance, and higher double-layer capacitance of 25.53 m F cm-2 compared to those of unary Co3O4@NC or Ni@NC metal hybrids. Therefore, this paper presents a facile strategy for designing other heteroatom-doped oxides coupled with ideal carbon materials as electrocatalysts for the OER.
文摘Metal doping for active sites exhibits remarkable potential for improving the hydrogen evolution reaction(HER).Multi-doping and the use of a conductive substrate can further modulate catalytic performance.Herein,Nb-CoSe well dispersed in N-doped carbon nanospheres(NCs,Nb-CoSe@NC)was synthesized to serve as a conductive substrate and facilitated good dispersion of active sites for the HER.Nb doping can also change the electronic structure of CoSe,which facilitates the activity for the HER.In order to further improve the conductivity and intrinsic activity of Nb-CoSe@NC,dual,nonmetal doping was realized through gas sulfurization to prepare hierarchical Nb-CoSeS@NC.The prepared Nb-CoSeS@NC,with a core-shell structure,exhibited a low overpotential of 115 mV at 10 mA cm–2,which is smaller than that of the most doped catalysts.In addition,NCs not only improved the dispersion and conductivity of the catalyst but also prevented metal corrosion in an electrolyte,thus facilitating the long-term stability of Nb-CoSeS@NC.Moreover,the synergistic effect of the multi-doping of Nb,S,and Se was explained.This work provides a promising,multi-doping strategy for the large-scale application of transition-metal-based electrocatalysts for the HER.
基金supported by the Major Scientific and Technological Project of PetroChina (ZD2019-183-003)Project of National Natural Science Foundation of China (42074133)+1 种基金the Fundamental Research Funds for the Central Universities (19CX02056A)Project of State Key Laboratory of Shale Oil and Gas Enrichment Mechanisms and Effective Development (33550000-21-FW0399-0009)
文摘The fi rst arrival waveform inversion(FAWI)has a strong nonlinearity due to the objective function using L2 parametrization.When the initial velocity is not accurate,the inversion can easily fall into local minima.In the full waveform inversion method,adding a cross-correlation function to the objective function can eff ectively reduce the nonlinearity of the inversion process.In this paper,the nonlinearity of this process is reduced by introducing the correlation objective function into the FAWI and by deriving the corresponding gradient formula.We then combine the first-arrival wave travel-time tomography with the FAWI to form a set of inversion processes.This paper uses the limited memory Broyden-Fletcher-Goldfarb-Shanno(L-BFGS)algorithm to improve the computational effi ciency of inversion and solve the problem of the low effi ciency of the FAWI method.The overthrust model and fi eld data test show that the method used in this paper can eff ectively reduce the nonlinearity of inversion and improve the inversion calculation effi ciency at the same time.
文摘To meet the current energy needs of society,the highly efficient and continuous production of clean energy is required.One of the key issues facing the green hydrogen evolution is the construction of efficient,low-cost electrocatalysts.Prussian blue(PB),Prussian blue analogs(PBAs),and their derivatives have tunable metal centers and have attracted significant interest as novel photo-and electrochemical catalysts.In this review,recent research progress into PB/PBA-based hollow structures,substrate-supported nanostructures,and their derivatives for green water splitting is discussed and summarized.First,several remarkable examples of nanostructured PB/PBAs supported on substrates(copper foil,carbon cloth,and nickel foam)and hollow structures(such as single-shelled hollow boxes,open hollow cages,and intricate hollow structures(multi-shell and yolk-shell))are discussed in detail,including their synthesis and formation mechanisms.Subsequently,the applications of PB/PBA derivatives((hydr)oxides,phosphides,chalcogenides,and carbides)for water splitting are discussed.Finally,the limitations in this research area and the most urgent challenges are summarized.We hope that this review will stimulate more researchers to develop technologies based on these intricate PB/PBA structures and their derivatives for highly efficient,green water splitting.
基金supported by the Shandong Provincial Natural Science Foundation,China(No.ZR2017QB015)the National Natural Science Foundation of China(No.21773309)China University of Petroleum Student’s Platform for Innovation and Entrepreneurship Training Program(No.20161449)
文摘A rod-like NiCo2O4 modified glassy carbon electrode was fabricated and used for non-enzymatic glucose sensing. The NiCo2O4 was prepared by a facile hydrothermal reaction and subsequently treated in a commercial microwave oven to eliminate the residual water introduced during the hydrothermal procedure. Structural analysis showed that there was no significant structural alteration before and after microwave treatment. The elimination of water residuals was confirmed by the stoichiometric ratio change by using element analysis. The microwave treated NiCo2O4 (M-NiCo2O4) showed excellent performance as a glucose sensor (sensitivity 431.29 μA·mmol/L-1·cm-2). The sensing performance decreases dramatically by soaking the M-NiCo2O4 in water. This result indicates that the introduction of residual water during hydrothermal process strongly affects the electrochemical performance and microwave pre-treatment is crucial for better sensory performance.
基金supported by the National Science and Technology major projects of China(No.2017ZX05032-003-002)Shandong Key Research and Development Plan Project(No.2018GHY115016)China University of Petroleum(East China)Independent Innovation Research Project(No.18CX06023A)。
文摘The full-waveform inversion method is a high-precision inversion method based on the minimization of the misfit between the synthetic seismograms and the observed data.However,this method suffers from cycle skipping in the time domain or phase wrapping in the frequency because of the inaccurate initial velocity or the lack of low-frequency information.furthermore,the object scale of inversion is affected by the observation system and wavelet bandwidth,the inversion for large-scale structures is a strongly nonlinear problem that is considerably difficult to solve.In this study,we modify the unwrapping algorithm to obtain accurate unwrapped instantaneous phase,then using this phase conducts the inversion for reducing the strong nonlinearity.The normal instantaneous phases are measured as modulo 2π,leading the loss of true phase information.The path integral algorithm can be used to unwrap the instantaneous phase of the seismograms having time series and onedimensional(1 D)signal characteristics.However,the unwrapped phase is easily affected by the numerical simulation and phase calculations,resulting in the low resolution of inversion parameters.To increase the noise resistance and ensure the inversion accuracy,we present an improved unwrapping method by adding an envelope into the path integral unwrapping algorithm for restricting the phase mutation points,getting accurate instantaneous phase.The objective function constructed by unwrapping instantaneous phase is less affected by the local minimum,thereby making it suitable for full-waveform inversion.Further,the corresponding instantaneous phase inversion formulas are provided.Using the improved algorithm,we can invert the low-wavenumber components of the underneath structure and ensure the accuracy of the inverted velocity.Finally,the numerical tests of the 2 D Marmousi model and 3 D SEG/EAGE salt model prove the accuracy of the proposed algorithm and the ability to restore largescale low-wavenumber structures,respectively.
