Understanding the pore water conversion characteristics during hydrate formation in porous media is important to study the accumulation mechanism of marine gas hydrate.In this study,low-field NMR was used to study the...Understanding the pore water conversion characteristics during hydrate formation in porous media is important to study the accumulation mechanism of marine gas hydrate.In this study,low-field NMR was used to study the pore water conversion characteristics during methane hydrate formation in unsaturated sand samples.Results show that the signal intensity of T_(2) distribution isn’t affected by sediment type and pore pressure,but is affected by temperature.The increase in the pressure of hydrogen-containing gas can cause the increase in the signal intensity of T_(2) distribution.The heterogeneity of pore structure is aggravated due to the hydrate formation in porous media.The water conversion rate fluctuates during the hydrate formation.The sand size affects the water conversion ratio and rate by affecting the specific surface of sand in unsaturated porous media.For the fine sand sample,the large specific surface causes a large gas-water contact area resulting in a higher water conversion rate,but causes a large water-sand contact area resulting in a low water conversion ratio(C_(w)=96.2%).The clay can reduce the water conversion rate and ratio,especially montmorillonite(C_(w)=95.8%).The crystal layer of montmorillonite affects the pore water conversion characteristics by hindering the conversion of interlayer water.展开更多
Metal single-atom catalysts(SACs) have emerged as a focal point of research, captivating the scientific community due to their distinctive electronic properties and unparalleled catalytic prowess in the realm of heter...Metal single-atom catalysts(SACs) have emerged as a focal point of research, captivating the scientific community due to their distinctive electronic properties and unparalleled catalytic prowess in the realm of heterogeneous catalysis. However, their significance transcends their role as mere active sites. Recent investigations have illuminated the multifaceted capabilities of metal single atoms as catalyst promoters and precursors, paving the way for the engineering of highly efficient heterogeneous catalysts. Single-atom promoters not only enhance the stabilization of active metals and tailor the support material, but regulate the reactive interfacial structure, eventually tuning the catalytic performance. Furthermore, SACs were also used as catalyst precursors to design new catalyst active sites. During the pretreatment or catalytic reaction, the structure of the metal single sites is changed significantly and transformed into the new and more active state, which improve the adsorption and reactive ability of reactants or intermediates. In this critical review, we comment the recent development of metal SACs used as catalyst promoters/precursors in engineering heterogeneous catalysts, including thermal catalysis and electrocatalysis. Furthermore, the dynamic evolution of the SACs during the pretreatment or catalytic reaction is also discussed. Finally, we provide our insight to potentially guide the future development on this emerging field.展开更多
基金the financial support of the National Natural Science Foundation of China(41876051 and 41872136)the China Postdoctoral Science Foundation(2021M701815)the Postdoctoral Innovative Talents Support Program in Shandong Province(SDBX2021015).
文摘Understanding the pore water conversion characteristics during hydrate formation in porous media is important to study the accumulation mechanism of marine gas hydrate.In this study,low-field NMR was used to study the pore water conversion characteristics during methane hydrate formation in unsaturated sand samples.Results show that the signal intensity of T_(2) distribution isn’t affected by sediment type and pore pressure,but is affected by temperature.The increase in the pressure of hydrogen-containing gas can cause the increase in the signal intensity of T_(2) distribution.The heterogeneity of pore structure is aggravated due to the hydrate formation in porous media.The water conversion rate fluctuates during the hydrate formation.The sand size affects the water conversion ratio and rate by affecting the specific surface of sand in unsaturated porous media.For the fine sand sample,the large specific surface causes a large gas-water contact area resulting in a higher water conversion rate,but causes a large water-sand contact area resulting in a low water conversion ratio(C_(w)=96.2%).The clay can reduce the water conversion rate and ratio,especially montmorillonite(C_(w)=95.8%).The crystal layer of montmorillonite affects the pore water conversion characteristics by hindering the conversion of interlayer water.
基金financially supported by the National High-Level Young Talents ProgramNational Natural Science Foundation of China (22372138, 22072118 and 22121001)+2 种基金Funds from State Key Laboratory for Physical Chemistry of Solid Surfaces of Xiamen University are also acknowledgedPart fund was supported by the Fundamental Research Funds for the Central Universities (20720220008)by Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM)(HRTP-[2022]-3)。
文摘Metal single-atom catalysts(SACs) have emerged as a focal point of research, captivating the scientific community due to their distinctive electronic properties and unparalleled catalytic prowess in the realm of heterogeneous catalysis. However, their significance transcends their role as mere active sites. Recent investigations have illuminated the multifaceted capabilities of metal single atoms as catalyst promoters and precursors, paving the way for the engineering of highly efficient heterogeneous catalysts. Single-atom promoters not only enhance the stabilization of active metals and tailor the support material, but regulate the reactive interfacial structure, eventually tuning the catalytic performance. Furthermore, SACs were also used as catalyst precursors to design new catalyst active sites. During the pretreatment or catalytic reaction, the structure of the metal single sites is changed significantly and transformed into the new and more active state, which improve the adsorption and reactive ability of reactants or intermediates. In this critical review, we comment the recent development of metal SACs used as catalyst promoters/precursors in engineering heterogeneous catalysts, including thermal catalysis and electrocatalysis. Furthermore, the dynamic evolution of the SACs during the pretreatment or catalytic reaction is also discussed. Finally, we provide our insight to potentially guide the future development on this emerging field.