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Theoretical study on the mechanism of sulfur migration to gas in the pyrolysis of benzothiophene

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 334-346 doi: 10.1007/s11705-022-2209-4

摘要： The release and control of sulfur species in the pyrolysis of fossil fuels and solid wastes have attracted attention worldwide. Particularly, thiophene derivatives are important intermediates for the sulfur gas release from organic sulfur, but the underlying migration mechanisms remain unclear. Herein, the mechanism of sulfur migration during the release of sulfur-containing radicals in benzothiophene pyrolysis was explored through quantum chemistry modeling. The C1-to-C2 H-transfer has the lowest energy barrier of 269.9 kJ·mol–1 and the highest rate constant at low temperatures, while the elevated temperature is beneficial for C−S bond homolysis. 2-Ethynylbenzenethiol is the key intermediate for the formation of S and SH radicals with the overall energy barriers of 408.0 and 498.7 kJ·mol–1 in favorable pathways. The generation of CS radicals is relatively difficult because of the high energy barrier (551.8 kJ·mol–1). However, it can be significantly promoted by high temperatures, where the rate constant exceeds that for S radical generation above 930 °C. Consequently, the strong competitiveness of S and SH radicals results in abundant H2S during benzothiophene pyrolysis, and the high temperature is more beneficial for CS2 generation from CS radicals. This study lays a foundation for elucidating sulfur migration mechanisms and furthering the development of pyrolysis techniques.

关键词： benzothiophene     sulfur migration     pyrolysis     density functional theory    

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Catalytic hydrodeoxygenation of pyrolysis bio-oil to jet fuel: A review

《能源前沿（英文）》 doi: 10.1007/s11708-024-0924-8

摘要： Bio-oil from biomass pyrolysis cannot directly substitute traditional fuel due to compositional deficiencies. Catalytic hydrodeoxygenation (HDO) is the critical and efficient step to upgrade crude bio-oil to high-quality bio-jet fuel by lowering the oxygen content and increasing the heating value. However, the hydrocracking reaction tends to reduce the liquid yield and increase the gas yield, causing carbon loss and producing hydrocarbons with a short carbon-chain. To obtain high-yield bio-jet fuel, the elucidation of the conversion process of biomass catalytic HDO is important in providing guidance for metal catalyst design and optimization of reaction conditions. Considering the complexity of crude bio-oil, this review aimed to investigate the catalytic HDO pathways with model compounds that present typical bio-oil components. First, it provided a comprehensive summary of the impact of physical and electronic structures of both noble and non-noble metals that include monometallic and bimetallic supported catalysts on regulating the conversion pathways and resulting product selectivity. The subsequent first principle calculations further corroborated reaction pathways of model compounds in atom-level on different catalyst surfaces with the experiments above and illustrated the favored C–O/C=O scission orders thermodynamically and kinetically. Then, it discussed hydrogenation effects of different H-donors (such as hydrogen and methane) and catalysts deactivation for economical and industrial consideration. Based on the descriptions above and recent researches, it also elaborated on catalytic HDO of biomass and bio-oil with multi-functional catalysts. Finally, it presented the challenges and future prospective of biomass catalytic HDO.

关键词： biomass pyrolysis oil     bio-jet fuel     catalytic hydrodeoxygenation (HDO)     metal catalyst     reaction pathways    

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Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1700-1712 doi: 10.1007/s11705-022-2207-6

摘要： The chain length and hydrocarbon type significantly affect the production of light olefins during the catalytic pyrolysis of naphtha. Herein, for a better catalyst design and operation parameters optimization, the reaction pathways and equilibrium yields for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins were analyzed thermodynamically. The results revealed that the thermodynamically favorable reaction pathways for n/iso-paraffins and cyclo-paraffins were the protolytic and hydrogen transfer cracking pathways, respectively. However, the formation of light paraffin severely limits the maximum selectivity toward light olefins. The dehydrogenation cracking pathway of n/iso-paraffins and the protolytic cracking pathway of cyclo-paraffins demonstrated significantly improved selectivity for light olefins. The results are thus useful as a direction for future catalyst improvements, facilitating superior reaction pathways to enhance light olefins. In addition, the equilibrium yield of light olefins increased with increasing the chain length, and the introduction of cyclo-paraffin inhibits the formation of light olefins. High temperatures and low pressures favor the formation of ethylene, and moderate temperatures and low pressures favor the formation of propylene. n-Hexane and cyclohexane mixtures gave maximum ethylene and propylene yield of approximately 49.90% and 55.77%, respectively. This work provides theoretical guidance for the development of superior catalysts and the selection of proper operation parameters for the catalytic pyrolysis of C5–8 n/iso/cyclo-paraffins from a thermodynamic point of view.

关键词： naphtha     catalytic pyrolysis     reaction pathway     equilibrium yield    

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Mechanism insight into the formation of HS from thiophene pyrolysis: A theoretical study

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1404-8

摘要：

• Possible formation pathways of H2S were revealed in thiophene pyrolysis.

关键词： Density functional theory     Waste rubber     Thiophene     H2S     Pyrolysis    

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Catalytic hydrodeoxygenation of pyrolysis bio-oil to jet fuel: A review

《能源前沿（英文）》 doi: 10.1007/s11708-024-0943-7

摘要： Bio-oil from biomass pyrolysis cannot directly substitute traditional fuel due to compositional deficiencies. Catalytic hydrodeoxygenation (HDO) is the critical and efficient step to upgrade crude bio-oil to high-quality bio-jet fuel by lowering the oxygen content and increasing the heating value. However, the hydrocracking reaction tends to reduce the liquid yield and increase the gas yield, causing carbon loss and producing hydrocarbons with a short carbon-chain. To obtain high-yield bio-jet fuel, the elucidation of the conversion process of biomass catalytic HDO is important in providing guidance for metal catalyst design and optimization of reaction conditions. Considering the complexity of crude bio-oil, this review aimed to investigate the catalytic HDO pathways with model compounds that present typical bio-oil components. First, it provided a comprehensive summary of the impact of physical and electronic structures of both noble and non-noble metals that include monometallic and bimetallic supported catalysts on regulating the conversion pathways and resulting product selectivity. The subsequent first principle calculations further corroborated reaction pathways of model compounds in atom-level on different catalyst surfaces with the experiments above and illustrated the favored C–O/C=O scission orders thermodynamically and kinetically. Then, it discussed hydrogenation effects of different H-donors (such as hydrogen and methane) and catalysts deactivation for economical and industrial consideration. Based on the descriptions above and recent researches, it also elaborated on catalytic HDO of biomass and bio-oil with multi-functional catalysts. Finally, it presented the challenges and future prospective of biomass catalytic HDO.

关键词： biomass pyrolysis oil     bio-jet fuel     catalytic hydrodeoxygenation (HDO)     metal catalyst     reaction pathways    

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Continuous flow pyrolysis of virgin and waste polyolefins: a comparative study, process optimization

《化学科学与工程前沿（英文）》 2024年 第18卷 第6期 doi: 10.1007/s11705-024-2429-x

摘要： Under optimal process conditions, pyrolysis of polyolefins can yield ca. 90 wt % of liquid product, i.e., combination of light oil fraction and heavier wax. In this work, the experimental findings reported in a selected group of publications concerning the non-catalytic pyrolysis of polyolefins were collected, reviewed, and compared with the ones obtained in a continuously operated bench-scale pyrolysis reactor. Optimized process parameters were used for the pyrolysis of waste and virgin counterparts of high-density polyethylene, low-density polyethylene, polypropylene and a defined mixture of those (i.e., 25:25:50 wt %, respectively). To mitigate temperature drops and enhance heat transfer, an increased feed intake is employed to create a hot melt plastic pool. With 1.5 g·min–1 feed intake, 1.1 L·min–1 nitrogen flow rate, and a moderate pyrolysis temperature of 450 °C, the formation of light hydrocarbons was favored, while wax formation was limited for polypropylene-rich mixtures. Pyrolysis of virgin plastics yielded more liquid (maximum 73.3 wt %) than that of waste plastics (maximum 66 wt %). Blending polyethylenes with polypropylene favored the production of liquids and increased the formation of gasoline-range hydrocarbons. Gas products were mainly composed of C3 hydrocarbons, and no hydrogen production was detected due to moderate pyrolysis temperature.

关键词： waste plastics     polyolefins     chemical recycling     pyrolysis     alternative fuels     waste-to-energy    

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Self-catalytic pyrolysis thermodynamics of waste printed circuit boards with co-existing metals

《环境科学与工程前沿（英文）》 2022年 第16卷 第11期 doi: 10.1007/s11783-022-1581-0

摘要：

● The co-existing metals in WPCBs has positive catalytic influence in pyrolysis.

关键词： Waste printed circuit board     Catalyst     Pyrolysis     Kinetics    

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Kinetic study of the effect of thermal hysteresis on pyrolysis of vacuum residue

《化学科学与工程前沿（英文）》 2024年 第18卷 第12期 doi: 10.1007/s11705-024-2496-z

摘要： Investigating the thermal hysteresis and its effect on the kinetic behaviors and reaction model of vacuum residue pyrolysis is of significant importance in industry and scientific research. Effects of heating rate and heating transfer resistance on the pyrolysis process were examined with the thermogravimetric analysis. The kinetic characteristics of the vacuum residue pyrolysis were estimated using the iso-conversional method and integral master-plots method based on a three-stage reaction model through the deconvolution of Fraser-Suzuki function. Results showed that the reaction order models for the first and second stages were associated with the evaporation of vapor, while the nucleation and growth models for the third stage were linked to char formation. During the pyrolysis, the thermal hysteresis led to an increase in the reaction order in the first stage, which resulted in a delayed release of generated hydrocarbons due to high heating rate and enhanced heat transfer resistance. The reaction in the last stage primarily involved coking, where the presence of an inert solid acted as a nucleating agent, facilitating char formation and reducing the activation energy. The optimization results suggest that the obtained three-stage reaction model and kinetic triplets have the potential to effectively describe the active pyrolysis behavior of vacuum residue under high thermal hysteresis.

关键词： vacuum residue     pyrolysis     thermogravimetric analysis     thermal hysteresis     kinetic mechanism    

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Microwave-assisted pyrolysis of plastics for aviation oil production: energy and economic analyses

《化学科学与工程前沿（英文）》 2024年 第18卷 第7期   页码 81-81 doi: 10.1007/s11705-024-2436-y

摘要： Microwave-assisted pyrolysis is an effective method for recycling plastic wastes into oils that can be used for aviation fuels. In this study, energy and economic analyses of aviation oil production from microwave-assisted pyrolysis of polystyrene were performed. The total energy efficiency, recovered energy efficiency, unitary cost, unitary energy economic cost, relative cost difference, and energy economic factor were detailed. And the effects of microwave power, pyrolysis temperature, microwave absorbent loading, and microwave absorbent type on these parameters were covered. It was found that pyrolysis temperature has the most significant effect on the unitary cost and unitary energy economic cost of aviation oil, and-microwave absorbent type has a significant influence on energy economic factor during the whole microwave-assisted pyrolysis process. The optimum reaction conditions at the tonnage system for pyrolysis of 1 t polystyrene were microwave power of 650 W, pyrolysis temperature of 460 °C, and silicon carbide (microwave absorbent) at a loading of 2 t (twice than feedstock loading). At these optimal conditions, the total energy efficiency, recovered energy efficiency, unitary cost, unitary energy economic cost, relative cost difference, and energy economic factor were 62.78%, 96.51%, 3.21 × 104 yuan·t–1, 779 yuan·GJ–1, 1.49, and 71.02%, respectively.

关键词： energy analysis     economic analysis     microwave-assisted pyrolysis     polystyrene     aviation oil    

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Co-pyrolysis of sludge and kaolin/zeolite in a rotary kiln: Analysis of stabilizing heavy metals

《环境科学与工程前沿（英文）》 2022年 第16卷 第7期 doi: 10.1007/s11783-021-1488-1

摘要：

• Adding kaolin/zeolite promotes the formation of stable heavy metals.

关键词： Co-pyrolysis     Sewage sludge     Heavy metals     Rotary kiln     Immobilization mechanism    

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Synergistic effects and kinetics analysis for co-pyrolysis of vacuum residue and plastics

《化学科学与工程前沿（英文）》 2024年 第18卷 第5期 doi: 10.1007/s11705-024-2414-4

摘要： This study utilized a thermogravimetric analyzer to assess the thermal decomposition behaviors and kinetics properties of vacuum residue (VR) and low-density polyethylene (LDPE) polymers. The kinetic parameters were calculated using the Friedman technique. To demonstrate the interactive effects between LDPE and VR during the co-pyrolysis process, the disparity in mass loss and mass loss rate between the experimental and calculated values was computed. The co-pyrolysis curves obtained through estimation and experimentation exhibited significant deviations, which were influenced by temperature and mixing ratio. A negative synergistic interaction was observed between LDPE and VR, although this inhibitory effect could be mitigated or eliminated by reducing the LDPE ratio in the mixture and increasing the co-pyrolysis temperature. The co-pyrolysis process resulted in a reduction in carbon residue, which could be attributed to the interaction between LDPE and the heavy fractions, particularly resin and asphaltene, present in VR. These findings align with the pyrolysis behaviors exhibited by the four VR fractions. Furthermore, it was observed that the co-pyrolysis process exhibited lower activation energy as the VR ratio increased, indicating a continuous enhancement in the reactivity of the mixed samples during co-pyrolysis.

关键词： co-pyrolysis     heavy residual oil     polyethylene     thermogravimetric analysis     synergistic effects    

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Co-pyrolysis of oil sludge with hydrogen-rich plastics in a vertical stirring reactor: Kinetic analysis

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11783-022-1570-3

摘要：

● Collaborative treatment of plastics and OS was established to improve oil quality.

关键词： Oily sludge     Pyrolysis     Polyethylene     H/Ceff ratio     Oil quality    

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Mass and heat balance calculations and economic evaluation of an innovative biomass pyrolysis project

Quanyuan WEI, Yongshui QU, Tianwei TAN

《化学科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 355-361 doi: 10.1007/s11705-010-0567-9

摘要： Biomass can be converted into flammable gas, charcoal, wood vinegar, wood tar oil and noncombustible materials with thermo-chemical pyrolysis reactions. Many factors influence these processes, such as the properties of the raw materials, and temperature control and these will affect the products that are produced. Based on the data from a straw pyrolysis demonstration project, the mass and heat balance of the biomass pyrolysis process were analyzed. The statistical product and service solutions (SPSS) statistical method was used to analyze the data which were monitored on-site. A cost-benefit analysis was then used to study the viability of commercializing the project. The analysis included net present value, internal rate of return and investment payback period. These results showed that the straw pyrolysis project has little risk, and will produce remarkable economic benefits.

关键词： mass balance     heat balance     biomass pyrolysis     economic benefit    

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Fast and catalytic pyrolysis of xylan: Effects of temperature and M/HZSM-5 (M= Fe, Zn) catalysts on pyrolytic

Xifeng ZHU, Qiang LU, Wenzhi LI, Dong ZHANG,

《能源前沿（英文）》 2010年 第4卷 第3期   页码 424-429 doi: 10.1007/s11708-010-0015-z

摘要： Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) was employed to achieve fast pyrolysis of xylan and on-line analysis of pyrolysis vapors. Tests were conducted to investigate the effects of temperature on pyrolytic products, and to reveal the effect of HZSM-5 and M/HZSM-5 (M= Fe, Zn) zeolites on pyrolysis vapors. The results showed that the total yield of pyrolytic products first increased and then decreased with the increase of temperature from 350°C to 900°C. The pyrolytic products were complex, and the most abundant products included hydroxyacetaldehyde, acetic acid, 1-hydroxy-2-propanone, 1-hydroxy-2-butanone and furfural. Catalytic cracking of pyrolysis vapors with HZSM-5 and M/HZSM-5 (M= Fe, Zn) catalysts significantly altered the product distribution. Oxygen-containing compounds were reduced considerably, and meanwhile, a lot of hydrocarbons, mainly toluene and xylenes, were formed. M/HZSM-5 catalysts were more effective than HZSM-5 in reducing the oxygen-containing compounds, and therefore, they helped to produce higher contents of hydrocarbons than HZSM-5.

关键词： xylan     fast pyrolysis     catalytic pyrolysis     Py-GC/MS     HZSM-5    

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Upgrading of derived pyrolysis vapors for the production of biofuels from corncobs

Liaoyuan Mao, Yanxin Li, Z. Conrad Zhang

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 50-58 doi: 10.1007/s11705-017-1685-4

摘要： A bubbling fluidized bed pyrolyzer was integrated with an honeycomb as a catalytic upgrading zone for the conversion of biomass to liquid fuels. In the upgrading zone, zeolite coated ceramic honeycomb (ZCCH) catalysts consisting of ZSM-5 (Si/Al=25) were stacked and N or recycled non-condensable gas was used as a carrier gas. Ground corncob particles were fast pyrolyzed in the bubbling bed using fine sand particles as a heat carrier and the resulting pyrolysis vapors were passed on-line over the catalytic upgrading zone. The influence of carrier gas, temperature, and weight hourly space velocity (WHSV) of catalyst on the oil product properties, distribution and mass balance were studied. Using ZCCH effectively increased the hydrocarbon yield and the heating value of the dry oil, especially in the presence of the recycled noncondensable gas. Even a low usage of zeolite catalyst at WSHV of 180 h was effective in upgrading the pyrolysis oil and other light olefins. The highest hydrocarbon (≥C2) and liquid aromatics yields reached to 14.23 and 4.17 wt-%, respectively. The undesirable products including light oxygenates, furans dramatically decreased in the presence of the ZCCH catalyst.

关键词： corncob     monolith     upgrading     pyrolysis    

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标题 作者 时间 类型 操作

Theoretical study on the mechanism of sulfur migration to gas in the pyrolysis of benzothiophene

期刊论文

Catalytic hydrodeoxygenation of pyrolysis bio-oil to jet fuel: A review

期刊论文

Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

期刊论文

Mechanism insight into the formation of HS from thiophene pyrolysis: A theoretical study

期刊论文

Catalytic hydrodeoxygenation of pyrolysis bio-oil to jet fuel: A review

期刊论文

Continuous flow pyrolysis of virgin and waste polyolefins: a comparative study, process optimization

期刊论文

Self-catalytic pyrolysis thermodynamics of waste printed circuit boards with co-existing metals

期刊论文

Kinetic study of the effect of thermal hysteresis on pyrolysis of vacuum residue

期刊论文

Microwave-assisted pyrolysis of plastics for aviation oil production: energy and economic analyses

期刊论文

Co-pyrolysis of sludge and kaolin/zeolite in a rotary kiln: Analysis of stabilizing heavy metals

期刊论文

Synergistic effects and kinetics analysis for co-pyrolysis of vacuum residue and plastics

期刊论文

Co-pyrolysis of oil sludge with hydrogen-rich plastics in a vertical stirring reactor: Kinetic analysis

期刊论文

Mass and heat balance calculations and economic evaluation of an innovative biomass pyrolysis project

Quanyuan WEI, Yongshui QU, Tianwei TAN

期刊论文

Fast and catalytic pyrolysis of xylan: Effects of temperature and M/HZSM-5 (M= Fe, Zn) catalysts on pyrolytic

Xifeng ZHU, Qiang LU, Wenzhi LI, Dong ZHANG,

期刊论文

Upgrading of derived pyrolysis vapors for the production of biofuels from corncobs

Liaoyuan Mao, Yanxin Li, Z. Conrad Zhang

期刊论文