Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with th...Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with the continuous development of material systems and modification strategies,researchers have gradually found that D-band center theory is usually effective for large metal particle systems,but for small metal particle systems or semiconductors,such as single atom systems,the opposite conclusion to the D-band center theory is often obtained.To solve the issue above,here we propose a bonding and anti-bonding orbitals stable electron intensity difference(BASED)theory for surface chemistry.The newly-proposed BASED theory can not only successfully explain the abnormal phenomena of D-band center theory,but also exhibits a higher accuracy for prediction of adsorption energy and bond length of intermediates on active sites.Importantly,a new phenomenon of the spin transition state in the adsorption process is observed based on the BASED theory,where the active center atom usually yields an unstable high spin transition state to enhance its adsorption capability in the adsorption process of intermediates when their distance is about 2.5Å.In short,the BASED theory can be considered as a general principle to understand catalytic mechanism of intermediates on surfaces.展开更多
Stochastic seismic inversion is the combination of geostatistics and seismic inversion technology which integrates information from seismic records, well logs, and geostatistics into a posterior probability density fu...Stochastic seismic inversion is the combination of geostatistics and seismic inversion technology which integrates information from seismic records, well logs, and geostatistics into a posterior probability density function （PDF） of subsurface models. The Markov chain Monte Carlo （MCMC） method is used to sample the posterior PDF and the subsurface model characteristics can be inferred by analyzing a set of the posterior PDF samples. In this paper, we first introduce the stochastic seismic inversion theory, discuss and analyze the four key parameters： seismic data signal-to-noise ratio （S/N）, variogram, the posterior PDF sample number, and well density, and propose the optimum selection of these parameters. The analysis results show that seismic data S/N adjusts the compromise between the influence of the seismic data and geostatistics on the inversion results, the variogram controls the smoothness of the inversion results, the posterior PDF sample number determines the reliability of the statistical characteristics derived from the samples, and well density influences the inversion uncertainty. Finally, the comparison between the stochastic seismic inversion and the deterministic model based seismic inversion indicates that the stochastic seismic inversion can provide more reliable information of the subsurface character.展开更多
The formations and transformations of the chemical bonds of reactants and intermediates on cata- lyst surfaces occur in conjunction with the evolution of heat during catalytic reactions. Measure- ment of this evolved ...The formations and transformations of the chemical bonds of reactants and intermediates on cata- lyst surfaces occur in conjunction with the evolution of heat during catalytic reactions. Measure- ment of this evolved heat is helpful in terms of understanding the nature of the interactions be- tween the catalyst and the adsorbed species, and provides insights into the reactivity of the catalyst. Although various techniques have previously been applied to assessments of evolved heat, direct measurements using a Tian-Calvet microcalorimeter are currently the most reliable method for this purpose. In this review, we summarize the relationship between the adsorption/reaction energetics determined by microcalorimetry and the reactivities of supported catalysts, and examine the im- portant role of microcalorimetry in understanding catalytic performance from the energetic point of view.展开更多
文摘Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with the continuous development of material systems and modification strategies,researchers have gradually found that D-band center theory is usually effective for large metal particle systems,but for small metal particle systems or semiconductors,such as single atom systems,the opposite conclusion to the D-band center theory is often obtained.To solve the issue above,here we propose a bonding and anti-bonding orbitals stable electron intensity difference(BASED)theory for surface chemistry.The newly-proposed BASED theory can not only successfully explain the abnormal phenomena of D-band center theory,but also exhibits a higher accuracy for prediction of adsorption energy and bond length of intermediates on active sites.Importantly,a new phenomenon of the spin transition state in the adsorption process is observed based on the BASED theory,where the active center atom usually yields an unstable high spin transition state to enhance its adsorption capability in the adsorption process of intermediates when their distance is about 2.5Å.In short,the BASED theory can be considered as a general principle to understand catalytic mechanism of intermediates on surfaces.
基金supported by the National Major Science and Technology Project of China on Development of Big Oil-Gas Fields and Coalbed Methane (No. 2008ZX05010-002)
文摘Stochastic seismic inversion is the combination of geostatistics and seismic inversion technology which integrates information from seismic records, well logs, and geostatistics into a posterior probability density function （PDF） of subsurface models. The Markov chain Monte Carlo （MCMC） method is used to sample the posterior PDF and the subsurface model characteristics can be inferred by analyzing a set of the posterior PDF samples. In this paper, we first introduce the stochastic seismic inversion theory, discuss and analyze the four key parameters： seismic data signal-to-noise ratio （S/N）, variogram, the posterior PDF sample number, and well density, and propose the optimum selection of these parameters. The analysis results show that seismic data S/N adjusts the compromise between the influence of the seismic data and geostatistics on the inversion results, the variogram controls the smoothness of the inversion results, the posterior PDF sample number determines the reliability of the statistical characteristics derived from the samples, and well density influences the inversion uncertainty. Finally, the comparison between the stochastic seismic inversion and the deterministic model based seismic inversion indicates that the stochastic seismic inversion can provide more reliable information of the subsurface character.
基金supported by the National Natural Science Foundation of China (21573232, 21576251, 21676269)National Key Projects for Funda-mental Research and Development of China (2016YFA0202801)Department of Science and Technology of Liaoning province under contract of 2015020086–101~~
文摘The formations and transformations of the chemical bonds of reactants and intermediates on cata- lyst surfaces occur in conjunction with the evolution of heat during catalytic reactions. Measure- ment of this evolved heat is helpful in terms of understanding the nature of the interactions be- tween the catalyst and the adsorbed species, and provides insights into the reactivity of the catalyst. Although various techniques have previously been applied to assessments of evolved heat, direct measurements using a Tian-Calvet microcalorimeter are currently the most reliable method for this purpose. In this review, we summarize the relationship between the adsorption/reaction energetics determined by microcalorimetry and the reactivities of supported catalysts, and examine the im- portant role of microcalorimetry in understanding catalytic performance from the energetic point of view.
