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Upgrading pyrolytic carbon-blacks (CBp) from end-of-life tires: Characteristics and modification methodologies

Jiaxue Yu, Junqing Xu, Zhenchen Li, Wenzhi He, Juwen Huang, Junshi Xu, Guangming Li

《环境科学与工程前沿（英文）》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1198-0

摘要： Modification methodologies of upgrading CBp from ELTs were reviewed. Surface microstructures and physiochemical properties of CBp were analyzed. Future perspectives of ELTs pyrolysis industries were suggested. Over 1 billion end-of-life tires (ELTs) are generating annually, and 4 billion ELTs are currently abandoned in landfills and stockpiles worldwide, according to the statistics, leading to the environmental and health risks. To circumvent these issues, pyrolysis, as an attractive thermochemical process, has been addressed to tackle the ELTs’ problem to reduce the risks as well as increase the material recycling. However, due to the lack of systematic characteristic analysis and modification methods, poor quality of CBp limits the improvement of ELTs pyrolysis in industry applications, which plays a crucial role in the economic feasibility of pyrolysis process. In this review, we have summarized the state-of-the-art characteristics and modification methodologies of the upgrading of CBp, to in-depth understand the surface microstructures and physiochemical properties of CBp for the foundation for modification afterwards. By virtue of the proper selection of modification methods and modifying agents, the new generation of multifunctional carbon materials with desired properties can be instead of the traditional materials of CB, promising broader and various application fields.

关键词： Pyrolysis carbon-blacks     CBp     Post-pyrolysis     Demineralization     Surface modification    

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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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Direct pyrolysis to convert biomass to versatile 3D carbon nanotubes/mesoporous carbon architecture:

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 679-690 doi: 10.1007/s11705-022-2266-8

摘要： The massive conversion of resourceful biomass to carbon nanomaterials not only opens a new avenue to effective and economical disposal of biomass, but provides a possibility to produce highly valued functionalized carbon-based electrodes for energy storage and conversion systems. In this work, biomass is applied to a facile and scalable one-step pyrolysis method to prepare three-dimensional (3D) carbon nanotubes/mesoporous carbon architecture, which uses transition metal inorganic salts and melamine as initial precursors. The role of each employed component is investigated, and the electrochemical performance of the attained product is explored. Each component and precise regulation of their dosage is proven to be the key to successful conversion of biomass to the desired carbon nanomaterials. Owing to the unique 3D architecture and integration of individual merits of carbon nanotubes and mesoporous carbon, the as-synthesized carbon nanotubes/mesoporous carbon hybrid exhibits versatile application toward lithium-ion batteries and Zn-air batteries. Apparently, a significant guidance on effective conversion of biomass to functionalized carbon nanomaterials can be shown by this work.

关键词： biomass     direct pyrolysis     3D CNTs/MC hybrid     lithium-ion batteries     Zn-air batteries    

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Catalytic fast pyrolysis of walnut shell for alkylphenols production with nitrogen-doped activated carbon

Shanwei Ma, Hang Li, Guan Zhang, Tahir Iqbal, Kai Li, Qiang Lu

《环境科学与工程前沿（英文）》 2021年 第15卷 第2期 doi: 10.1007/s11783-020-1317-y

摘要： Abstract • N-doped activated carbon was prepared for catalytic pyrolysis of walnut shell. • Alkylphenols were selectively produced from catalytic pyrolysis process. • The alkylphenols yield increased by 8.5 times under the optimal conditions. • Formation mechanism of alkylphenols was proposed. Alkylphenols are a group of valuable phenolic compounds that can be derived from lignocellulosic biomass. In this study, three activated carbons (ACs) were prepared for catalytic fast pyrolysis (CFP) of walnut shell to produce alkylphenols, including nitrogen-doped walnut shell-derived activated carbon (N/WSAC), nitrogen-doped rice husk-derived activated carbon (N/RHAC) and walnut shell-derived activated carbon (WSAC). Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were carried out to reveal the influences of AC type, pyrolytic temperature, and AC-to-walnut shell (AC-to-WS) ratio on the product distributions. Results showed that with nitrogen doping, the N/WSAC possessed stronger capability than WSAC toward the alkylphenols production, and moreover, the N/WSAC also exhibited better effects than N/RHAC to prepare alkylphenols. Under the catalysis of N/WSAC, yields of alkylphenols were significantly increased, especially phenol, cresol and 4-ethylphenol. As the increase of pyrolytic temperature, the alkylphenols yield first increased and then decreased, while high selectivity could be obtained at low pyrolytic temperatures. Such a trend was also observed as the AC-to-WS ratio continuously increased. The alkylphenols production achieved a maximal yield of 44.19 mg/g with the corresponding selectivity of 34.7% at the pyrolytic temperature of 400°C and AC-to-WS ratio of 3, compared with those of only 4.67 mg/g and 6.1% without catalyst. In addition, the possible formation mechanism of alkylphenols was also proposed with the catalysis of N/WSAC.

关键词： Pyrolysis     Walnut shell     Alkylphenols     Nitrogen-doped activated carbon    

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Pyrolysis transformation of ZIF-8 wrapped with polytriazine to nitrogen enriched core-shell polyhedronscarbon for supercapacitor

Nuoya Wang, Xinhua Huang, Lei Zhang, Jinsong Hu, Yimin Chao, Ruikun Zhao

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 944-953 doi: 10.1007/s11705-020-2005-y

摘要： This work presents a simple effective strategy to synthesize -doped and shell-controlled carbon nanocages through a package baking approach. A green approach to synthesize core-shell ZIF-8@PTZ nanoparticles involves zinc contained ZIF-8 core wrapped by a N-enriched polytriazine (PTZ). Synthesized core-shell ZIF-8@PTZ nanoparticles are calcinated to further sublime zinc through PTZ shell and washed by HCl, leaving a porous carbon structure. At the meantime, hollow cavities were introduced into N-doped carbon polyhedrons via the sacrifice of ZIF-8 template (noted as ZIF-8@C/N-x). The electrochemical performance of the ZIF-8@C/N-x as supercapacitor electrode has demonstrated high energy density and specific capacitance, as well as a long-term cycleability showing 92% capacitance retention after 10000 cycles. There is a systematic correlation between micro-/meso-porosity of ZIF-8@C/N-x and their electrochemical performances.

关键词： core-shell     EDLC electrode     microporos nano polygons     nitrogen doped carbon    

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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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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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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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Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1114-1124 doi: 10.1007/s11705-021-2087-1

摘要： Improvement of the low-cost transition metal electrocatalyst used in sluggish oxygen evolution reaction is a significant but challenging problem. In this study, ultrafine Fe-modulated Ni nanoparticles embedded in a porous Ni-doped carbon matrix were produced by the pyrolysis of zirconium metal-organic-frameworks, in which 2,2′-bipyridine-5,5′-dicarboxylate operating as a ligand can coordinate with Ni2+ and Fe3+. This strategy allows formation of Fe-modulated Ni nanoparticles with a uniform dimension of about 2 nm which can be ascribed to the spatial blocking effect of ZrO2. This unique catalyst displays an efficient oxygen evolution reaction electrocatalytic activity with a low overpotential of 372 mV at 10 mA·cm–2 and a small Tafel slope of 84.4 mV·dec–1 in alkaline media. More importantly, it shows superior durability and structural stability after 43 h in a chronoamperometry test. Meanwhile, it shows excellent cycling stability during 4000 cyclic voltammetry cycles. This research offers a new insight into the construction of uniform nanoscale transition metals and their alloys as highly efficient and durable electrocatalysts.

关键词： metal-organic framework     pyrolysis     ultrafine     Fe-modulated Ni nanoparticles     oxygen evolution reaction    

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Effect of / molecular structures on pyrolysis performance and heat sink of decalin isomers

《化学科学与工程前沿（英文）》 2023年 第18卷 第1期 doi: 10.1007/s11705-023-2375-z

摘要： Decalin is considered as an important compound of high-energy-density endothermic fuel, which is an ideal on-board coolant for thermal management of advanced aircraft. However, decalin contains two isomers with a tunable composition, and their effects on the pyrolysis performance, such as the heat sink and coking tendency have not been demonstrated. Herein, we investigated the pyrolysis of decalin isomers, i.e., cis-decalin, trans-decalin and their mixtures (denoted as mix-decalin), in order to clarify the effects of the cis-/trans-structures on the pyrolysis performance of decalin fuels. The pyrolysis results confirmed that conversion of the tested fuels (600–725 °C, 4 MPa) decreased in the order cis-decalin > mix-decalin > trans-decalin. Detailed analyses of the pyrolysis products were used to compare the product distributions from cis-decalin, mix-decalin and trans-decalin, and the yields of some typical components (such as cyclohexene, 1-methylcyclohexene, benzene and toluene) showed significant differences, which could be ascribed to deeper cracking of cis-decalin. Additionally, the heat sinks and coking tendencies of the decalins decreased in the order cis-decalin > mix-decalin > trans-decalin. This work demonstrates the relationship between the cis/trans structures and the pyrolysis performance of decalin, which provides a better understanding of the structure-activity relationships of endothermic hydrocarbon fuels.

关键词： endothermic fuel     decalin     pyrolysis     heat sink     molecular structure    

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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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木质纤维素类生物质热解实现碳中和工业应用的关键问题

张书, 邹侃, 李斌, Hojae Shim, 黄勇

《工程（英文）》 2023年 第29卷 第10期   页码 35-38 doi: 10.1016/j.eng.2023.02.015

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标题 作者 时间 类型 操作

Upgrading pyrolytic carbon-blacks (CBp) from end-of-life tires: Characteristics and modification methodologies

Jiaxue Yu, Junqing Xu, Zhenchen Li, Wenzhi He, Juwen Huang, Junshi Xu, Guangming Li

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

Direct pyrolysis to convert biomass to versatile 3D carbon nanotubes/mesoporous carbon architecture:

期刊论文

Catalytic fast pyrolysis of walnut shell for alkylphenols production with nitrogen-doped activated carbon

Shanwei Ma, Hang Li, Guan Zhang, Tahir Iqbal, Kai Li, Qiang Lu

期刊论文

Pyrolysis transformation of ZIF-8 wrapped with polytriazine to nitrogen enriched core-shell polyhedronscarbon for supercapacitor

Nuoya Wang, Xinhua Huang, Lei Zhang, Jinsong Hu, Yimin Chao, Ruikun Zhao

期刊论文

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

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

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

期刊论文

Ultrafine Fe-modulated Ni nanoparticles embedded within nitrogen-doped carbon from Zr-MOFs-confined conversion

期刊论文

Effect of / molecular structures on pyrolysis performance and heat sink of decalin isomers

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

木质纤维素类生物质热解实现碳中和工业应用的关键问题

张书, 邹侃, 李斌, Hojae Shim, 黄勇

期刊论文