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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 C_5–8 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 C_5–8 n/iso/cyclo-paraffins from a thermodynamic point of view.

关键词： naphtha catalytic pyrolysis reaction pathway equilibrium yield

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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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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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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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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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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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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/C_eff 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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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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Prediction of high-density polyethylene pyrolysis using kinetic parameters based on thermogravimetric

《环境科学与工程前沿（英文）》 2023年第17卷第1期 doi: 10.1007/s11783-023-1606-3

摘要：

● Reducting the sampling frequency can enhance the modelling process.

关键词： HDPE Pyrolysis Kinetics Thermogravimetric ANOVA Artificial neural network

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Hydro-pyrolysis of lignocellulosic biomass over alumina supported Platinum, Mo

Songbo He, Jeffrey Boom, Rolf van der Gaast, K. Seshan

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 155-161 doi: 10.1007/s11705-017-1655-x

摘要： In-line hydro-treatment of bio-oil vapor from fast pyrolysis of lignocellulosic biomass (hydro-pyrolysis of biomass) is studied as a method of upgrading the liquefied bio-oil for a possible precursor to green fuels. The nobel metal (Pt) and non-noble metal catalysts (Mo C and WC) were compared at 500 °C and atmospheric pressure which are same as the reaction conditions for fast pyrolysis of biomass. Results indicated that under the pyrolysis conditions, the major components, such as acids and carbonyls, of the fast pyrolysis bio-oil can be completely and partially hydrogenated to form hydrocarbons, an ideal fossil fuel blend, in the hydro-treated bio-oil. The carbide catalysts perform equally well as the Pt catalyst regarding to the aliphatic and aromatic hydrocarbon formation (ca. 60%), showing the feasibility of using the cheap non-noble catalysts for hydro-pyrolysis of biomass.

关键词： bio-oil pyrolysis hydro-deoxygenation (HDO) non-noble metal catalysts hydro-treatment

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Particle formation of hydroxyapatite precursor containing two components in a spray pyrolysis process

W. Widiyastuti, Adhi Setiawan, Sugeng Winardi, Tantular Nurtono, Heru Setyawan

《化学科学与工程前沿（英文）》 2014年第8卷第1期页码 104-113 doi: 10.1007/s11705-014-1406-1

摘要： The particle formation mechanism of hydroxyapatite precursor containing two components, Ca(OOCCH ) and (NH ) HPO with a ratio of Ca/P= 1.67, in a spray pyrolysis process has been studied by computational fluid dynamics (CFD) simulation on the transfer of heat and mass from droplets to the surrounding media. The focus included the evaporation of the solvent in the droplets, a second evaporation due to crust formation, the decomposition reaction of each component of the precursor, and a solid-state reaction that included the kinetic parameters of the precursor regarding its two components that formed the hydroxyapatite product. The rate of evaporation and the reacted fraction of the precursor both increased with temperature. The predicted average size of the hydroxyapatite particles agreed well with the experimental results. Therefore, the selected models were also suitable for predicting the average size of particles that contain two components in the precursor solution.

关键词： droplet hydroxyapatite particle CFD tubular furnace spray pyrolysis

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Fabrication of N-doped carbon nanobelts from a polypyrrole tube by confined pyrolysis for supercapacitors

Wei Wang, Haijun Lv, Juan Du, Aibing Chen

《化学科学与工程前沿（英文）》 2021年第15卷第5期页码 1312-1321 doi: 10.1007/s11705-020-2033-7

摘要： In this present work, N-doped carbon nanobelts (N-CNBs) were prepared by a confined-pyrolysis approach and the N-CNBs were derived from a polypyrrole (Ppy) tube coated with a compact silica layer. The silica layer provided a confined space for the Ppy pyrolysis, thereby hindering the rapid overflow of pyrolysis gas, which is the activator for the formation of carbonaceous materials. At the same time, the confined environment can activate the carbon shell to create a thin wall and strip the carbon tube into belt morphology. This process of confined pyrolysis realizes self-activation during the pyrolysis of Ppy to obtain the carbon nanobelts without adding any additional activator, which reduces pollution and preparation cost. In addition, this approach is simple to operate and avoids the disadvantages of other methods that consume time and materials. The as-prepared N-CNB shows cross-linked nanobelt morphology and a rich porous structure with a large specific surface area. As supercapacitor electrode materials, the N-CNB can present abundant active sites, and exhibits a specific capacitance of 246 F·g , and excellent ability with 95.44% retention after 10000 cycles. This indicates that the N-CNB is an ideal candidate as a supercapacitor electrode material.

关键词： carbon nanobelts polypyrrole N-doped confined pyrolysis supercapacitor

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Preparation and characterization of novel carbon molecular sieve membrane/PSSF composite by pyrolysis

Ying Yan, Peng Huang, Huiping Zhang

《化学科学与工程前沿（英文）》 2019年第13卷第4期页码 772-783 doi: 10.1007/s11705-019-1827-y

摘要： Carbon molecular sieve membrane (CMSM)/paper-like stainless steel fibers (PSSF) has been manufactured by pyrolyzing poly (furfuryl alcohol) (PFA) coated on the metal fibers. PFA was synthesized using oxalic acid dihydrate as a catalyst and coated on microfibers by dip coating method. For the purpose of investigating the effects of final carbonization temperature, the composites were carbonized between 400°C and 800°C under flowing nitrogen. The morphology and microstructure were examined by X-ray diffraction, Fourier transforms infrared spectroscopy, scanning electron microscopy, thermogravimetric analysis, N adsorption and desorption, Raman spectra and X-ray photoelectron spectra. The consequences of characterization showed that the CMSM containing mesopores of 3.9 nm were manufactured. The specific surface area of the CMSM/PSSF fabricated in different pyrolysis temperature varies from 26.5 to 169.1 m ∙g and pore volume varies from 0.06 to 0.23 cm ∙g . When pyrolysis temperature exceeds 600°C, the specific surface, pore diameter and pore volume decreased as carbonization temperature increased. Besides, the degree of graphitization in carbon matrix increased with rising pyrolysis temperature. Toluene adsorption experiments on different structured fixed bed that was padded by CMSM/PSSF and granular activated carbon (GAC) were conducted. For the sake of comparison, adsorption test was also performed on fixed bed packed with GAC. The experimental results indicated that the rate constant ′ was dramatically increased as the proportion of CMCM/PSSF composites increased on the basis of Yoon-Nelson model, which suggested that structured fixed bed padded with CMSM/PSSF composite offered higher adsorption rate and mass transfer efficiency.

关键词： carbon molecular sieve membrane stainless steel fibers pyrolysis structured fixed bed toluene

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Effect of temperature on Lu’an bituminous char structure evolution in pyrolysis and combustion

Yandi ZHANG, Yinhe LIU, Xiaoli DUAN, Yao ZHOU, Xiaoqian LIU, Shijin XU

《能源前沿（英文）》 2021年第15卷第1期页码 14-25 doi: 10.1007/s11708-020-0805-x

摘要： In the process of pyrolysis and combustion of coal particles, coal structure evolution will be affected by the ash behavior, which will further affect the char reactivity, especially in the ash melting temperature zone. Lu’an bituminous char and ash samples were prepared at the N and air atmospheres respectively across ash melting temperature. A scanning electron microscope (SEM) was used to observe the morphology of char and ash. The specific surface area (SSA) analyzer and thermogravimetric analyzer were respectively adopted to obtain the pore structure characteristics of the coal chars and combustion parameters. Besides, an X-ray diffractometer (XRD) was applied to investigate the graphitization degree of coal chars prepared at different pyrolysis temperatures. The SEM results indicated that the number density and physical dimension of ash spheres exuded from the char particles both gradually increased with the increasing temperature, thus the coalescence of ash spheres could be observed obviously above 1100°C. Some flocculent materials appeared on the surface of the char particles at 1300°C, and it could be speculated that -Si N was generated in the pyrolysis process under N . The SSA of the chars decreased with the increasing pyrolysis temperature. Inside the char particles, the micropore area and its proportion in the SSA also declined as the pyrolysis temperature increased. Furthermore, the constantly increasing pyrolysis temperature also caused the reactivity of char decrease, which is consistent with the results obtained by XRD. The higher combustion temperature resulted in the lower porosity and more fragments of the ash.

关键词： bituminous char pyrolysis ash structure evolution reactivity

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标题作者时间类型操作

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

期刊论文

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

期刊论文

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

期刊论文

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

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

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

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

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

Liaoyuan Mao, Yanxin Li, Z. Conrad Zhang

期刊论文

Prediction of high-density polyethylene pyrolysis using kinetic parameters based on thermogravimetric

期刊论文

Hydro-pyrolysis of lignocellulosic biomass over alumina supported Platinum, Mo

Songbo He, Jeffrey Boom, Rolf van der Gaast, K. Seshan

期刊论文

Particle formation of hydroxyapatite precursor containing two components in a spray pyrolysis process

W. Widiyastuti, Adhi Setiawan, Sugeng Winardi, Tantular Nurtono, Heru Setyawan

期刊论文

Fabrication of N-doped carbon nanobelts from a polypyrrole tube by confined pyrolysis for supercapacitors

Wei Wang, Haijun Lv, Juan Du, Aibing Chen

期刊论文

Preparation and characterization of novel carbon molecular sieve membrane/PSSF composite by pyrolysis

Ying Yan, Peng Huang, Huiping Zhang

期刊论文

Effect of temperature on Lu’an bituminous char structure evolution in pyrolysis and combustion

Yandi ZHANG, Yinhe LIU, Xiaoli DUAN, Yao ZHOU, Xiaoqian LIU, Shijin XU

期刊论文

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