The thermodynamic and kinetic mechanisms of Taixi anthracite during its graphitization process were explored.To understand the variation trends of carbon arrangement order,microcrystal size,and graphitization degree a...The thermodynamic and kinetic mechanisms of Taixi anthracite during its graphitization process were explored.To understand the variation trends of carbon arrangement order,microcrystal size,and graphitization degree against temperature during the graphitization process,a series of experiments were performed using Raman spectroscopy and X-ray diffraction(XRD).Subsequently,the influencing factors of the dominant reaction at different temperatures were analyzed using thermodynamics and kinetics.The results showed that the graphitization process of Taixi anthracite can be divided into three stages from the perspective of reaction thermodynamics and kinetics.Temperature played a crucial role in the formation and growth of a graphitic structure.Meanwhile,multivariate mechanisms coexisted in the graphitization process.At ultrahigh temperatures,the defects of synthetic graphite could not be completely eliminated and perfect graphite crystals could not be produced.At low temperatures,the reaction is mainly controlled by dynamics,while at high temperatures,thermodynamics dominates the direction of the reaction.展开更多
Materialization of coal is one of effective and clean pathways for its utilization. The microstructures of coal-based carbon materials have an important influence on their functional applications. Herein, the microstr...Materialization of coal is one of effective and clean pathways for its utilization. The microstructures of coal-based carbon materials have an important influence on their functional applications. Herein, the microstructural evolution of anthracite in the temperature range of 1000–2800 ℃ was systematically investigated to provide a guidance for the microstructural regulation of coal-based carbon materials.The results indicate that the microstructure of anthracite undergoes an important change during carbonization-graphitization process. As the temperature increases, aromatic layers in anthracite gradually transform into disordered graphite microcrystals and further grow into ordered graphite microcrystals, and then ordered graphite microcrystals are laterally linked to form pseudo-graphite phase and eventually transformed into highly ordered graphite-like sheets. In particular, 2000–2200 ℃ is a critical temperature region for the qualitative change of ordered graphite crystallites to pseudo-graphite phase,in which the relevant structural parameters including stacking height, crystallite lateral size and graphitization degree show a rapid increase. Moreover, both aromaticity and graphitization degree have a linear positive correlation with carbonization-graphitization temperature in a specific temperature range.Besides, after initial carbonization, some defect structures in anthracite such as aliphatic carbon and oxygen-containing functional groups are released in the form of gaseous low-molecular volatiles along with an increased pore structure, and the intermediates derived from minerals could facilitate the conversion of sp^(3) amorphous carbon to sp^(2) graphitic carbon. This work provides a valuable reference for the rational design of microstructure of coal-based carbon materials.展开更多
The three-dimensional(3 D) structures of pores directly affect the CH4 flow.Therefore,it is very important to analyze the3 D spatial structure of pores and to simulate the CH4 flow with the connected pores as the carr...The three-dimensional(3 D) structures of pores directly affect the CH4 flow.Therefore,it is very important to analyze the3 D spatial structure of pores and to simulate the CH4 flow with the connected pores as the carrier.The result shows that the equivalent radius of pores and throats are 1-16 μm and 1.03-8.9 μm,respectively,and the throat length is 3.28-231.25 μm.The coordination number of pores concentrates around three,and the intersection point between the connectivity function and the X-axis is 3-4 μm,which indicate the macro-pores have good connectivity.During the single-channel flow,the pressure decreases along the direction of CH4 flow,and the flow velocity of CH4 decreases from the pore center to the wall.Under the dual-channel and the multi-channel flows,the pressure also decreases along the CH4 flow direction,while the velocity increases.The mean flow pressure gradually decreases with the increase of the distance from the inlet slice.The change of mean flow pressure is relatively stable in the direction horizontal to the bedding plane,while it is relatively large in the direction perpendicular to the bedding plane.The mean flow velocity in the direction horizontal to the bedding plane(Y-axis) is the largest,followed by that in the direction horizontal to the bedding plane(X-axis),and the mean flow velocity in the direction perpendicular to the bedding plane is the smallest.展开更多
基金Projects(51704204,51974194,52104097)supported by the National Natural Science Foundation of ChinaProjects(20210302123147,20210302124352)supported by the Basic Research Program of Shanxi Province,China。
基金financially supported by the China Postdoctoral Science Foundation and China National “Twelfth Five-Year” Plan for Science & Technology (No. 2014BAB01B02)Shenhua Ningxia Coal Industry Group for financial support and providing Taixi anthracite samplesthe support of Advanced Analysis & Computation Center of China University of Mining and Technology
文摘The thermodynamic and kinetic mechanisms of Taixi anthracite during its graphitization process were explored.To understand the variation trends of carbon arrangement order,microcrystal size,and graphitization degree against temperature during the graphitization process,a series of experiments were performed using Raman spectroscopy and X-ray diffraction(XRD).Subsequently,the influencing factors of the dominant reaction at different temperatures were analyzed using thermodynamics and kinetics.The results showed that the graphitization process of Taixi anthracite can be divided into three stages from the perspective of reaction thermodynamics and kinetics.Temperature played a crucial role in the formation and growth of a graphitic structure.Meanwhile,multivariate mechanisms coexisted in the graphitization process.At ultrahigh temperatures,the defects of synthetic graphite could not be completely eliminated and perfect graphite crystals could not be produced.At low temperatures,the reaction is mainly controlled by dynamics,while at high temperatures,thermodynamics dominates the direction of the reaction.
基金supported by the National Natural Science Foundation of China(Nos.51974110,52074109 and 52274261)the Key Scientific and Technological Project of Henan Province(No.202102210183)the Coal Green Conversion Outstanding Foreign Scientists Foundation of Henan Province(No.GZS2020012).
文摘Materialization of coal is one of effective and clean pathways for its utilization. The microstructures of coal-based carbon materials have an important influence on their functional applications. Herein, the microstructural evolution of anthracite in the temperature range of 1000–2800 ℃ was systematically investigated to provide a guidance for the microstructural regulation of coal-based carbon materials.The results indicate that the microstructure of anthracite undergoes an important change during carbonization-graphitization process. As the temperature increases, aromatic layers in anthracite gradually transform into disordered graphite microcrystals and further grow into ordered graphite microcrystals, and then ordered graphite microcrystals are laterally linked to form pseudo-graphite phase and eventually transformed into highly ordered graphite-like sheets. In particular, 2000–2200 ℃ is a critical temperature region for the qualitative change of ordered graphite crystallites to pseudo-graphite phase,in which the relevant structural parameters including stacking height, crystallite lateral size and graphitization degree show a rapid increase. Moreover, both aromaticity and graphitization degree have a linear positive correlation with carbonization-graphitization temperature in a specific temperature range.Besides, after initial carbonization, some defect structures in anthracite such as aliphatic carbon and oxygen-containing functional groups are released in the form of gaseous low-molecular volatiles along with an increased pore structure, and the intermediates derived from minerals could facilitate the conversion of sp^(3) amorphous carbon to sp^(2) graphitic carbon. This work provides a valuable reference for the rational design of microstructure of coal-based carbon materials.
基金financially supported by the National Key Research and Development Plan(No.2018YFB0605601)the National Natural Science Foundation of China(No.41972168)。
文摘The three-dimensional(3 D) structures of pores directly affect the CH4 flow.Therefore,it is very important to analyze the3 D spatial structure of pores and to simulate the CH4 flow with the connected pores as the carrier.The result shows that the equivalent radius of pores and throats are 1-16 μm and 1.03-8.9 μm,respectively,and the throat length is 3.28-231.25 μm.The coordination number of pores concentrates around three,and the intersection point between the connectivity function and the X-axis is 3-4 μm,which indicate the macro-pores have good connectivity.During the single-channel flow,the pressure decreases along the direction of CH4 flow,and the flow velocity of CH4 decreases from the pore center to the wall.Under the dual-channel and the multi-channel flows,the pressure also decreases along the CH4 flow direction,while the velocity increases.The mean flow pressure gradually decreases with the increase of the distance from the inlet slice.The change of mean flow pressure is relatively stable in the direction horizontal to the bedding plane,while it is relatively large in the direction perpendicular to the bedding plane.The mean flow velocity in the direction horizontal to the bedding plane(Y-axis) is the largest,followed by that in the direction horizontal to the bedding plane(X-axis),and the mean flow velocity in the direction perpendicular to the bedding plane is the smallest.
