Light illumination has been widely used to promote activity and selectivity of traditional thermal catalysts. Nevertheless, the role of light irradiation during catalytic reactions is not well understood. In this work...Light illumination has been widely used to promote activity and selectivity of traditional thermal catalysts. Nevertheless, the role of light irradiation during catalytic reactions is not well understood. In this work, Pt/Al2 O3 prepared by wet impregnation was used for photothermal CO2 hydrogenation, and it showed a photothermal effect. Hence, operando diffuse reflectance infrared Fourier-transform spectroscopy and density functional theory calculations were conducted on Pt/Al2 O3 to gain insights into the reaction mechanism. The results indicated that CO desorption from Pt sites including step sites(Ptstep) or/and terrace site(Ptterrace) is an important step during CO2 hydrogenation to free the active Pt sites. Notably, visible light illumination and temperature affected the CO desorption in different ways. The calculated adsorption energy of CO on Ptstep and Ptterrace sites was-1.24 and-1.43 e V, respectively. Hence, CO is more strongly bound to the Ptstep sites. During heating in the dark, CO preferentially desorbs from the Ptterrace site. However, the additional light irradiation facilitates transfer of CO from the Ptstep to Ptterrace sites and its subsequent desorption from the Ptterrace sites, thus promoting the CO2 hydrogenation.展开更多
No shale-rock physical model has been established in the observation coordinate system.To this end,this paper carried out anisotropic wave velocity tests on shale rock and compared the Thomsen,Daley,and Berryman solut...No shale-rock physical model has been established in the observation coordinate system.To this end,this paper carried out anisotropic wave velocity tests on shale rock and compared the Thomsen,Daley,and Berryman solutions to characterize anisotropic acoustic wave velocity.Finally,the Daley solution was selected.Based on basic rock physical models,such as SCA and DEM methods,and combined with the Daley solution,an anisotropic shale-rock physical model was established in the observation coordinate system and applied in Well B1 in the Luzhou area,Sichuan Basin.Our research conclusions were as follows:1.for the samples from the same core,the P-wave velocities in three directions were in the order VP11>VP45>VP33,shear wave velocity VS11 was the largest,but VS33 and VS45 did not follow the law of Vs33>Vs45 for some samples;2.the Daley solution,which not only considers the accuracy requirements but also has a complete expression of P-,SV-,and SH-waves,is most suitable for characterization of anisotropic wave velocity in this study area;3.the rock physical model constructed in the observation coordinate system has high accuracy,in which the absolute value of the relative error of the P-wave slowness was between 0%and 5.05%(0.55%on average),and that of shear-wave slowness was between 0%and 6.05%(0.59%on average);4.the acoustic waves recorded in Well B1 in the observation coordinate system were very different from those in the constitutive coordinate system.The relative difference of the P-wave was between 6.76%and 30.84%(14.68%on average),and that of the S-wave was between 7.00%and 23.44%(13.99%on average).The acoustic slowness measured in the observation coordinate system,such as in a deviated well or a horizontal well section,must be converted to the constitutive coordinate system before it can be used in subsequent engineering applications;5.the anisotropic shale-rock physical model built in the observation coordinate system proposed in this paper can provide basic data and guidance for subsequent pore pressure prediction,geomechanical modeling,and fracturing stimulation design for deviated and horizontal wells.展开更多
基金supported by the National Natural Science Foundation of China(U1862111,U1232119)Sichuan Provincial International Cooperation Project(2017HH0030)the Innovative Research Team of Sichuan Province(2016TD0011)~~
文摘Light illumination has been widely used to promote activity and selectivity of traditional thermal catalysts. Nevertheless, the role of light irradiation during catalytic reactions is not well understood. In this work, Pt/Al2 O3 prepared by wet impregnation was used for photothermal CO2 hydrogenation, and it showed a photothermal effect. Hence, operando diffuse reflectance infrared Fourier-transform spectroscopy and density functional theory calculations were conducted on Pt/Al2 O3 to gain insights into the reaction mechanism. The results indicated that CO desorption from Pt sites including step sites(Ptstep) or/and terrace site(Ptterrace) is an important step during CO2 hydrogenation to free the active Pt sites. Notably, visible light illumination and temperature affected the CO desorption in different ways. The calculated adsorption energy of CO on Ptstep and Ptterrace sites was-1.24 and-1.43 e V, respectively. Hence, CO is more strongly bound to the Ptstep sites. During heating in the dark, CO preferentially desorbs from the Ptterrace site. However, the additional light irradiation facilitates transfer of CO from the Ptstep to Ptterrace sites and its subsequent desorption from the Ptterrace sites, thus promoting the CO2 hydrogenation.
基金supported by the Post Doctoral Project of Southwest Oil and Gas Field Research on Geomechanics and Effective Fracturing Factors of Deep Shale” (No. 20210302-31)the Scientific Research Project of Southwest Oil and Gas Field Branch “Geological Engineering Integration of Well Block Yang101”。
文摘No shale-rock physical model has been established in the observation coordinate system.To this end,this paper carried out anisotropic wave velocity tests on shale rock and compared the Thomsen,Daley,and Berryman solutions to characterize anisotropic acoustic wave velocity.Finally,the Daley solution was selected.Based on basic rock physical models,such as SCA and DEM methods,and combined with the Daley solution,an anisotropic shale-rock physical model was established in the observation coordinate system and applied in Well B1 in the Luzhou area,Sichuan Basin.Our research conclusions were as follows:1.for the samples from the same core,the P-wave velocities in three directions were in the order VP11>VP45>VP33,shear wave velocity VS11 was the largest,but VS33 and VS45 did not follow the law of Vs33>Vs45 for some samples;2.the Daley solution,which not only considers the accuracy requirements but also has a complete expression of P-,SV-,and SH-waves,is most suitable for characterization of anisotropic wave velocity in this study area;3.the rock physical model constructed in the observation coordinate system has high accuracy,in which the absolute value of the relative error of the P-wave slowness was between 0%and 5.05%(0.55%on average),and that of shear-wave slowness was between 0%and 6.05%(0.59%on average);4.the acoustic waves recorded in Well B1 in the observation coordinate system were very different from those in the constitutive coordinate system.The relative difference of the P-wave was between 6.76%and 30.84%(14.68%on average),and that of the S-wave was between 7.00%and 23.44%(13.99%on average).The acoustic slowness measured in the observation coordinate system,such as in a deviated well or a horizontal well section,must be converted to the constitutive coordinate system before it can be used in subsequent engineering applications;5.the anisotropic shale-rock physical model built in the observation coordinate system proposed in this paper can provide basic data and guidance for subsequent pore pressure prediction,geomechanical modeling,and fracturing stimulation design for deviated and horizontal wells.