Nowadays,the efficient and cleaner utilization of coal have attracted wide attention due to the rich coal and rare oil/gas resources structure in China.Coal chemical looping gasification(CCLG)is a promising coal utili...Nowadays,the efficient and cleaner utilization of coal have attracted wide attention due to the rich coal and rare oil/gas resources structure in China.Coal chemical looping gasification(CCLG)is a promising coal utilization technology to achieve energy conservation and emission reduction targets for highly pure synthesis gas.As a downstream product of synthesis gas,methyl methacrylate(MMA),is widely used as raw material for synthesizing polymethyl methacrylate and resin products with excellent properties.So this paper proposes a novel system integrating MMA production and CCLG(CCLG-MMA)processes aiming at"energy saving and low emission",in which the synthesis gas produced by CCLG and purified by dry methane reforming(DMR)reaction and Rectisol process reacts with ethylene for synthesizing MMA.Firstly,the reaction mechanism of CCLG is investigated by using Reactive force field(ReaxFF)MD simulation based on atomic models of char and oxygen carrier(Fe_(2)O_(3))for obtaining optimum reaction temperature of fuel reactor(FR).Secondly,the steady-state simulation of CCLG-MMA system is carried out to verify the feasibility of MMA production.The amount of CO_(2)emitted by CCLG process and DMR reaction is 0.0028(kg CO_(2))^(-1)·(kg MMA)^(-1).The total energy consumption of the CCLG-MMA system is 45521 kJ·(kg MMA)^(-1),among which the consumption of MMA production part is 25293 k(·kg MMA)^(-1).The results show that the CCLG-MMA system meets CO_(2)emission standard and has lower energy consumption compared to conventional MMA production process.Finally,one control scheme is designed to verify the stability of CCLG-MMA system.The CCLG-MMA integration strategy aims to obtain highly pure MMA from multi-scale simulation perspectives,so this is an optimal design regarding all factors influencing cleaner MMA production.展开更多
ReaxFF molecular dynamic simulation combined with experimental verification was performed to understand the overall reaction mechanism,especially the primary and secondary reactions involving in tar formation of sub-b...ReaxFF molecular dynamic simulation combined with experimental verification was performed to understand the overall reaction mechanism,especially the primary and secondary reactions involving in tar formation of sub-bituminous coal pyrolysis.Quantitative relationship at atomic level is clarified between bond breakage of functional groups and products generation,revealing that the amount and order in forming each product are subject to the number of corresponding functional groups and their bond energies respectively.The primary breakage of-C-O-and-C-C-bridge-bonds present in initial coal macromolecular generates molecular of heavy tar,whereas heavy tar can be converted into light tar through cracking side chain of aromatic rings and cyclic hydrocarbons at increased pyrolysis temperatures.At very high temperatures the cracking of short-chain hydrocarbons and residual atoms connecting to aromatic rings further occurs to generate light tar and gas.The remaining aromatic-ring fragments of heavy tar are likely cross-linked to form char.Furthermore,the simultaneous evolution tendency of tar yield and tar quality under different pyrolysis temperatures and heating rates is obtained at molecular level.For obtaining high yield and quality of tar,appropriately high temperature as well as suitable heating rate are needed to compromise the high yield of primary tar and high quality of secondarily upgraded products.展开更多
Lubrication failure accompanying with blackening phenomenon significantly reduces the long-running operational reliability of porous polymide(PPI)lubricated with poly-α-olefin(PAO)oil.Here,the effects of lubrication ...Lubrication failure accompanying with blackening phenomenon significantly reduces the long-running operational reliability of porous polymide(PPI)lubricated with poly-α-olefin(PAO)oil.Here,the effects of lubrication condition and counter-surface chemistry on the blackening failure of PAO impregnated PPI were studied through the comparison of the tribological tests against GCr15 steel ball and Al_(2)O_(3)ceramic ball with and without PAO oil lubrication.Black products were found to be formed on the PAO impregnated PPI surface slid against steel ball or Al_(2)O_(3)ball added with iron nano-particles,but be absent under the conditions without iron or PAO oil.Further analysis indicated that the iron-catalyzed splitting of PAO oil into small molecule alkanes and following the formation of black organic matter should be mainly responsible for the blackening phenomenon.Molecular dynamic(MD)simulations demonstrated that the iron facilitated the separation of hydrogen atom and the following broken of C–C bonds in PAO molecules,final resulting in the splitting of PAO oil.展开更多
基金supported by the National Natural Science Foundation of China(21576143)Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2020-KF-13)。
文摘Nowadays,the efficient and cleaner utilization of coal have attracted wide attention due to the rich coal and rare oil/gas resources structure in China.Coal chemical looping gasification(CCLG)is a promising coal utilization technology to achieve energy conservation and emission reduction targets for highly pure synthesis gas.As a downstream product of synthesis gas,methyl methacrylate(MMA),is widely used as raw material for synthesizing polymethyl methacrylate and resin products with excellent properties.So this paper proposes a novel system integrating MMA production and CCLG(CCLG-MMA)processes aiming at"energy saving and low emission",in which the synthesis gas produced by CCLG and purified by dry methane reforming(DMR)reaction and Rectisol process reacts with ethylene for synthesizing MMA.Firstly,the reaction mechanism of CCLG is investigated by using Reactive force field(ReaxFF)MD simulation based on atomic models of char and oxygen carrier(Fe_(2)O_(3))for obtaining optimum reaction temperature of fuel reactor(FR).Secondly,the steady-state simulation of CCLG-MMA system is carried out to verify the feasibility of MMA production.The amount of CO_(2)emitted by CCLG process and DMR reaction is 0.0028(kg CO_(2))^(-1)·(kg MMA)^(-1).The total energy consumption of the CCLG-MMA system is 45521 kJ·(kg MMA)^(-1),among which the consumption of MMA production part is 25293 k(·kg MMA)^(-1).The results show that the CCLG-MMA system meets CO_(2)emission standard and has lower energy consumption compared to conventional MMA production process.Finally,one control scheme is designed to verify the stability of CCLG-MMA system.The CCLG-MMA integration strategy aims to obtain highly pure MMA from multi-scale simulation perspectives,so this is an optimal design regarding all factors influencing cleaner MMA production.
基金financially supported by the National Natural Science Foundation of China(Grant No.U1908201)the National Key Research and Development Program of China(Grant No.2018YFC0808500).
文摘ReaxFF molecular dynamic simulation combined with experimental verification was performed to understand the overall reaction mechanism,especially the primary and secondary reactions involving in tar formation of sub-bituminous coal pyrolysis.Quantitative relationship at atomic level is clarified between bond breakage of functional groups and products generation,revealing that the amount and order in forming each product are subject to the number of corresponding functional groups and their bond energies respectively.The primary breakage of-C-O-and-C-C-bridge-bonds present in initial coal macromolecular generates molecular of heavy tar,whereas heavy tar can be converted into light tar through cracking side chain of aromatic rings and cyclic hydrocarbons at increased pyrolysis temperatures.At very high temperatures the cracking of short-chain hydrocarbons and residual atoms connecting to aromatic rings further occurs to generate light tar and gas.The remaining aromatic-ring fragments of heavy tar are likely cross-linked to form char.Furthermore,the simultaneous evolution tendency of tar yield and tar quality under different pyrolysis temperatures and heating rates is obtained at molecular level.For obtaining high yield and quality of tar,appropriately high temperature as well as suitable heating rate are needed to compromise the high yield of primary tar and high quality of secondarily upgraded products.
基金supported by the National Natural Science Foundation of China(Nos.52350411 and 52122507)the National Key R&D Program of China(No.2023YFB3405500)+1 种基金Sichuan Science and Technology Program(Nos.2023NSFSC1988 and 23NSFTD0030)the Independent Project of State Key Laboratory of Traction Power(No.2023TPL-T04).
文摘Lubrication failure accompanying with blackening phenomenon significantly reduces the long-running operational reliability of porous polymide(PPI)lubricated with poly-α-olefin(PAO)oil.Here,the effects of lubrication condition and counter-surface chemistry on the blackening failure of PAO impregnated PPI were studied through the comparison of the tribological tests against GCr15 steel ball and Al_(2)O_(3)ceramic ball with and without PAO oil lubrication.Black products were found to be formed on the PAO impregnated PPI surface slid against steel ball or Al_(2)O_(3)ball added with iron nano-particles,but be absent under the conditions without iron or PAO oil.Further analysis indicated that the iron-catalyzed splitting of PAO oil into small molecule alkanes and following the formation of black organic matter should be mainly responsible for the blackening phenomenon.Molecular dynamic(MD)simulations demonstrated that the iron facilitated the separation of hydrogen atom and the following broken of C–C bonds in PAO molecules,final resulting in the splitting of PAO oil.
