As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the ...As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the relationship between heavy oil composition and potassium storage performance remains unclear.Using heavy oils containing distinct chemical groups as the carbon source,namely fluid catalytic cracking slurry(FCCS),petroleum asphalt(PA)and deoiled asphalt(DOA),three carbon nanosheets(CNS)were prepared through a molten salt method,and used as the anodes for PIBs.The composition of the heavy oil determines the lamellar thicknesses,sp^(3)-C/sp^(2)-C ratio and defect concentration,thereby affecting the potassium storage performance.The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets(CNS-FCCS)that have a smaller layer thickness,larger interlayer spacing(0.372 nm),and increased number of folds than in CNS derived from the other three precursors.These features give it faster charge/ion transfer,more potassium storage sites and better reaction kinetics.CNS-FCCS has a remarkable K^(+)storage capacity(248.7 mAh g^(-1) after 100 cycles at 0.1 A g^(-1)),long cycle lifespan(190.8 mAh g^(-1) after 800 cycles at 1.0 A g^(-1))and excellent rate capability,ranking it among the best materials for this application.This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance,and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.展开更多
The ever-increasing integration of electronic devices has inevit-ably caused electromagnetic interference and heat accumulation problems,and dual-function materials with both a high thermal conductivity and high elect...The ever-increasing integration of electronic devices has inevit-ably caused electromagnetic interference and heat accumulation problems,and dual-function materials with both a high thermal conductivity and high electromagnetic wave absorption(EWA)are regarded as an effective strategy for solving these problems.Carbon materials are widely used as thermal and EWA fillers due to their excellent conductivity and outstanding thermal conduction properties,and have become a research hotspot in the field of high thermal conductivity,microwave absorbing materials in recent years.The status of current research progress on carbon-based high thermal-conduction microwave absorption materials,including carbon fibers,carbon nanotubes,graphene and amorphous carbon,is re-viewed,and the influence of the structure of the materials on their absorption and thermal conductivity properties,such as core-shell structure,three-dimensional network structure,and heteroatom doping,is also elaborated.Feasible solutions for the cur-rent problems with these materials are proposed,with the aim of providing valuable guidance for the future design of carbon-based high thermal conduction microwave absorbing materials.展开更多
Catalytic oxidation desulfurization(CODS)technology has shown great promise for diesel desulfurization by virtue of its low cost,mild reaction conditions,and superior desulfurization performance.Herein,a series of FeM...Catalytic oxidation desulfurization(CODS)technology has shown great promise for diesel desulfurization by virtue of its low cost,mild reaction conditions,and superior desulfurization performance.Herein,a series of FeMoO_(x)/LaTiO_(y)-z samples with diverse Fe/Mo ratios were prepared via a facile citric acid-assisted method.The impact of Fe incorporation on the dispersion and surface elemental states of Mo species,as well as oxygen species content of the synthesized FeMoO_(x)/LaTiO_(y)-z catalysts were systematically characterized using TEM,BET,UV-vis DRS,XPS,XANES,and reaction kinetics,and their CODS performances were examined for 4,6-DMDBT removal.Experimental results demonstrated that Fe/Mo ratio significantly affected the Ti−O bond strength,surface dispersion and electronic structure of Mo O_(2)species on FeMoO_(x)/LaTiO_(y)-z catalysts.FeMoO_(x)/LaTiO_(y)-2 catalyst showed outstanding cycling durability and the best CODS performance with almost 100%removal of 4,6-DMDBT from model oil within 75 min due to its proper MoO3 dispersion,optimal redox property,and the most oxygen vacancy concentration.Nevertheless,further enhancing Fe content led to the increased dispersion of Mo species,while the decrease active Mo species as well as the increase of steric effect for 4,6-DMDBT accessing to the catalytic reactive sites considerably increase the apparent activation energy of FeMoO_(x)/LaTiO_(y)-z(z>2)catalysts during the CODS process,thereby seriously suppressing their CODS performances.Moreover,Radical trapping experiments reveal that the·,generated by the activation of O_(2)at the active sites,catalytic oxidized 4,6-DMDBT to the product of 4,6-DMDBTO_(2),thereby enabling both deep desulfurization and recovery of high-value 4,6-DMDBTO_(2).These findings offer an alternative strategy to achieve ultra deep desulfurization as well as separate and recover high economic value sulfone substances from diesel.展开更多
The kinetics of Athabasca bitumen derived heavy gas oil over NiMo/Al2O3 catalysts were studied in a JQ-II high-pressure microscale hydrotreator unit under different operation conditions, including temperature, pressur...The kinetics of Athabasca bitumen derived heavy gas oil over NiMo/Al2O3 catalysts were studied in a JQ-II high-pressure microscale hydrotreator unit under different operation conditions, including temperature, pressure, H/O ratio and LHSV. The multi-parameter models of hydrodesulfurization and hydrodenitrogenation were proposed. The model parameters verify that the HDS and HDN reactions follow 1.5-order and 1.6-order kinetic rules, respectively. The kinetic activation energies of HDN and HDS over Com, Hom1 and Hom2 show that homemade catalysts exhibit higher activities in HDN than commercial catalyst. Using the multi-parameter kinetic model to predict the contents of sulfur and nitrogen in products is in good agreement with the experimental data.展开更多
Petroleum asphalt,an important by-product of the petrochemical industry,has diverse applications but often suffers from low industrial added value.Because of its low cost,high carbon content,and high polycyclic aromat...Petroleum asphalt,an important by-product of the petrochemical industry,has diverse applications but often suffers from low industrial added value.Because of its low cost,high carbon content,and high polycyclic aromatic hydrocarbon content,appropriate modification can increase its value and expand its energy storage applications.Current research progress on the common preparation methods of petroleum asphalt-based carbon materials,including template-assisted pyrolysis,molten salt treatment,activation,heteroatom doping,and pre-oxidation is reviewed,and its use in supercapacitors and alkali metal ion batteries,is also elaborated.Feasible solutions for the current problems with petroleum asphalt are proposed,with the aim of providing insights into its high value-added utilization.展开更多
The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts hav...The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.展开更多
The geometry and the potential curve of thermal decomposition for 1,1′dimethyl-5,5′-azotetraol (1-DMAT) are calculated by ab initio quantum chemistry method. The structural characteristics and decomposition mechanis...The geometry and the potential curve of thermal decomposition for 1,1′dimethyl-5,5′-azotetraol (1-DMAT) are calculated by ab initio quantum chemistry method. The structural characteristics and decomposition mechanism are carefully studied. It is found that the terrazzo ring satisfies 4n+2 rule and it is a conjugated π-system for 1-DMAT. The azotetrazol has aromatic characteristic and its thermal decomposition can proceed in two steps: ring opening and separation N2. The activation energies of the two steps are 243.5kJ/mol and 64.01kJ/mol, respectively. The ring opening is the rate-controlling step.展开更多
The geometry and the potential curve of thermal decomposition for 2,2′dimethyl-5,5′-azotetraol (2-DMAT) are calculated by ab initio quantum chemistry method. The structural characteristics and decomposition mechanis...The geometry and the potential curve of thermal decomposition for 2,2′dimethyl-5,5′-azotetraol (2-DMAT) are calculated by ab initio quantum chemistry method. The structural characteristics and decomposition mechanism are carefully studied. It is found that the terrazzo ring satisfies 4n+2 rule and it is a conjugated π-systems for 2-DMAT. The azotetrazol has aromaic characteristic and its thermal decomposition can proceed in two steps: ring opening and N2 separation. The activation energies of the two steps are 152.3kJ/mol and 44.67kJ/mol respectively. The ring opening is the rate-controlling step.展开更多
Catalytic pyrolysis of Chinese Daqing atmospheric residue on a commercial fluid catalytic cracking(FCC) catalyst was investigated in a confined fluidized bed reactor.The results show that the commercial FCC catalyst h...Catalytic pyrolysis of Chinese Daqing atmospheric residue on a commercial fluid catalytic cracking(FCC) catalyst was investigated in a confined fluidized bed reactor.The results show that the commercial FCC catalyst has good capability of cracking atmospheric residue to light olefins.The analysis of gas samples shows that the content of total light olefins in cracked gas is above 80%.The analysis of liquid samples shows that the content of aromatics in liquid samples ranges from 60% to 80%,and it increases with the enhancement of reaction temperature.The yield of total light olefins shows a maximum with the increase of reaction temperature,the weight ratios of catalyst-to-oil and steam-to-oil,respectively.The optimal reaction temperature,the weight ratios of catalyst-to-oil and steam-to-oil are about 650℃,15 and 0.75,respectively.展开更多
文摘As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the relationship between heavy oil composition and potassium storage performance remains unclear.Using heavy oils containing distinct chemical groups as the carbon source,namely fluid catalytic cracking slurry(FCCS),petroleum asphalt(PA)and deoiled asphalt(DOA),three carbon nanosheets(CNS)were prepared through a molten salt method,and used as the anodes for PIBs.The composition of the heavy oil determines the lamellar thicknesses,sp^(3)-C/sp^(2)-C ratio and defect concentration,thereby affecting the potassium storage performance.The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets(CNS-FCCS)that have a smaller layer thickness,larger interlayer spacing(0.372 nm),and increased number of folds than in CNS derived from the other three precursors.These features give it faster charge/ion transfer,more potassium storage sites and better reaction kinetics.CNS-FCCS has a remarkable K^(+)storage capacity(248.7 mAh g^(-1) after 100 cycles at 0.1 A g^(-1)),long cycle lifespan(190.8 mAh g^(-1) after 800 cycles at 1.0 A g^(-1))and excellent rate capability,ranking it among the best materials for this application.This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance,and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.
基金financial supports from the National Natural Science Foundation of China(22238012 and 22178384)Science Foundation of China University of Petroleum,Beijing(2462024QNXZ003)。
文摘The ever-increasing integration of electronic devices has inevit-ably caused electromagnetic interference and heat accumulation problems,and dual-function materials with both a high thermal conductivity and high electromagnetic wave absorption(EWA)are regarded as an effective strategy for solving these problems.Carbon materials are widely used as thermal and EWA fillers due to their excellent conductivity and outstanding thermal conduction properties,and have become a research hotspot in the field of high thermal conductivity,microwave absorbing materials in recent years.The status of current research progress on carbon-based high thermal-conduction microwave absorption materials,including carbon fibers,carbon nanotubes,graphene and amorphous carbon,is re-viewed,and the influence of the structure of the materials on their absorption and thermal conductivity properties,such as core-shell structure,three-dimensional network structure,and heteroatom doping,is also elaborated.Feasible solutions for the cur-rent problems with these materials are proposed,with the aim of providing valuable guidance for the future design of carbon-based high thermal conduction microwave absorbing materials.
基金supported by the Natural Science Foundation of Guangdong Province(2024A1515010908,2025A1515011103)Opening Project of Hubei Key Laboratory of Plasma Chemistry and Advanced Materials(2024P11)+2 种基金Postdoctoral Fellowship Program of CPSF(GZC20233104)National Natural Science Foundation of China(22202087)Opening Project of Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing&Finishing(STRZ202418)。
文摘Catalytic oxidation desulfurization(CODS)technology has shown great promise for diesel desulfurization by virtue of its low cost,mild reaction conditions,and superior desulfurization performance.Herein,a series of FeMoO_(x)/LaTiO_(y)-z samples with diverse Fe/Mo ratios were prepared via a facile citric acid-assisted method.The impact of Fe incorporation on the dispersion and surface elemental states of Mo species,as well as oxygen species content of the synthesized FeMoO_(x)/LaTiO_(y)-z catalysts were systematically characterized using TEM,BET,UV-vis DRS,XPS,XANES,and reaction kinetics,and their CODS performances were examined for 4,6-DMDBT removal.Experimental results demonstrated that Fe/Mo ratio significantly affected the Ti−O bond strength,surface dispersion and electronic structure of Mo O_(2)species on FeMoO_(x)/LaTiO_(y)-z catalysts.FeMoO_(x)/LaTiO_(y)-2 catalyst showed outstanding cycling durability and the best CODS performance with almost 100%removal of 4,6-DMDBT from model oil within 75 min due to its proper MoO3 dispersion,optimal redox property,and the most oxygen vacancy concentration.Nevertheless,further enhancing Fe content led to the increased dispersion of Mo species,while the decrease active Mo species as well as the increase of steric effect for 4,6-DMDBT accessing to the catalytic reactive sites considerably increase the apparent activation energy of FeMoO_(x)/LaTiO_(y)-z(z>2)catalysts during the CODS process,thereby seriously suppressing their CODS performances.Moreover,Radical trapping experiments reveal that the·,generated by the activation of O_(2)at the active sites,catalytic oxidized 4,6-DMDBT to the product of 4,6-DMDBTO_(2),thereby enabling both deep desulfurization and recovery of high-value 4,6-DMDBTO_(2).These findings offer an alternative strategy to achieve ultra deep desulfurization as well as separate and recover high economic value sulfone substances from diesel.
基金National Natural Science Foundation of China(20406012) and CNPC program(04A5050102 and 05E7019).
文摘The kinetics of Athabasca bitumen derived heavy gas oil over NiMo/Al2O3 catalysts were studied in a JQ-II high-pressure microscale hydrotreator unit under different operation conditions, including temperature, pressure, H/O ratio and LHSV. The multi-parameter models of hydrodesulfurization and hydrodenitrogenation were proposed. The model parameters verify that the HDS and HDN reactions follow 1.5-order and 1.6-order kinetic rules, respectively. The kinetic activation energies of HDN and HDS over Com, Hom1 and Hom2 show that homemade catalysts exhibit higher activities in HDN than commercial catalyst. Using the multi-parameter kinetic model to predict the contents of sulfur and nitrogen in products is in good agreement with the experimental data.
文摘Petroleum asphalt,an important by-product of the petrochemical industry,has diverse applications but often suffers from low industrial added value.Because of its low cost,high carbon content,and high polycyclic aromatic hydrocarbon content,appropriate modification can increase its value and expand its energy storage applications.Current research progress on the common preparation methods of petroleum asphalt-based carbon materials,including template-assisted pyrolysis,molten salt treatment,activation,heteroatom doping,and pre-oxidation is reviewed,and its use in supercapacitors and alkali metal ion batteries,is also elaborated.Feasible solutions for the current problems with petroleum asphalt are proposed,with the aim of providing insights into its high value-added utilization.
文摘The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.
基金Sponsored by National Basic Research Program of China Through the Grant ( 2004CB217802 )Educational Committee of Beijing(XK114140479)
文摘The geometry and the potential curve of thermal decomposition for 1,1′dimethyl-5,5′-azotetraol (1-DMAT) are calculated by ab initio quantum chemistry method. The structural characteristics and decomposition mechanism are carefully studied. It is found that the terrazzo ring satisfies 4n+2 rule and it is a conjugated π-system for 1-DMAT. The azotetrazol has aromatic characteristic and its thermal decomposition can proceed in two steps: ring opening and separation N2. The activation energies of the two steps are 243.5kJ/mol and 64.01kJ/mol, respectively. The ring opening is the rate-controlling step.
基金Sponsored by National Basic Research Programof China Throughthe Grant(2004CB217802) Educational Committee of Beijing(XK114140479)
文摘The geometry and the potential curve of thermal decomposition for 2,2′dimethyl-5,5′-azotetraol (2-DMAT) are calculated by ab initio quantum chemistry method. The structural characteristics and decomposition mechanism are carefully studied. It is found that the terrazzo ring satisfies 4n+2 rule and it is a conjugated π-systems for 2-DMAT. The azotetrazol has aromaic characteristic and its thermal decomposition can proceed in two steps: ring opening and N2 separation. The activation energies of the two steps are 152.3kJ/mol and 44.67kJ/mol respectively. The ring opening is the rate-controlling step.
基金National Science Fund for Distinguished Young Scholars of China(20525621)Major Research Plan of the Ministry of Education of China(307008).
文摘Catalytic pyrolysis of Chinese Daqing atmospheric residue on a commercial fluid catalytic cracking(FCC) catalyst was investigated in a confined fluidized bed reactor.The results show that the commercial FCC catalyst has good capability of cracking atmospheric residue to light olefins.The analysis of gas samples shows that the content of total light olefins in cracked gas is above 80%.The analysis of liquid samples shows that the content of aromatics in liquid samples ranges from 60% to 80%,and it increases with the enhancement of reaction temperature.The yield of total light olefins shows a maximum with the increase of reaction temperature,the weight ratios of catalyst-to-oil and steam-to-oil,respectively.The optimal reaction temperature,the weight ratios of catalyst-to-oil and steam-to-oil are about 650℃,15 and 0.75,respectively.
