JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2024
·Vol. 99
·期 7
·1626-1636
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IF 2.8
Haonnan Qiao,Yaqi Feng,Changsen Zhang
Background Catalytic co-pyrolysis of biomass with waste plastics can produce high-quality chemicals, making it a potential alternative to fossil fuels. The production of aromatic-rich oil was achieved in this work by the catalytic co-pyrolysis of pine sawdust and low-density polyethylene (LDPE) using a series of biochar (BC) made using different preparation methods. Zinc chloride (ZnCl 2 ) was employed to activate the BC during the preparation process, owing to its optimal activity for the co-pyrolysis intermediates. The study compared the effects of BCs activated using different treatment methods on the yield and fractions of pine sawdust and LDPE co-pyrolysis in a fast pyrolysis tube furnace at 650 °C. Results The study indicates that the ZnCl 2 BC, prepared from pine sawdust by fast pyrolysis (F-AC), exhibited the best aromatic catalytic activity. The selectivity to aromatic hydrocarbons was 72.53%, and the content of BTEX (benzene, toluene, ethylbenzene, and xylene) was 32.17%. Conclusion The Diels–Alder reaction and aromatization were made more effective due to the Zn sites and large pore structure in F-AC. Using Fourier transform infrared, scanning electron microscopy and X-ray photoelectron spectroscopy analysis, it was found that F-AC contained more oxygen (O)-containing groups in abundance, which improved its adsorption capacity for reaction intermediates. At the same time, the porous structure and high SSA of BC provided a region for the reaction intermediate to interact with the active center containing O-containing groups. This enhanced the synergy between biomass and plastics and raised the selectivity of aromatic hydrocarbons. It provides a reference for the application of carbon-based materials in the co-pyrolysis of biomass and waste plastics. © 2024 Society of Chemical Industry (SCI).
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
·
IF 5.8
Shan Cheng,Yi Fu,Hong Tian,Yi Cheng,Jiawei Wang,Jiang Zhu,Linxi Guo,Xuan Huang
The selectivity and catalytic mechanism of HZSM-5 in the pyrolysis of lignin model compounds at 600 °C were investigated using Py-GC/MS and density functional theory (DFT). The findings indicate that HZSM-5 elevated the relative content of aromatic hydrocarbons in the pyrolysis products of phenol, vanillin, and syringol by 12.3 %, 11.7 %, and 7.5 %, respectively. Meanwhile, the relative content of oxygen-containing products, including aldehydes and acids, was reduced by 15.7–52.0 %. Throughout the pyrolysis of lignin model compounds, various side chain reactions take place, such as dissociation, decarbonylation, isomerization rearrangement, alkylation, and aromatization. The selective catalytic decomposition mechanism of HZSM-5 on oxygen-containing functional groups involves both the physical selection imparted by the pore size structure and the selection of acid sites that form hydrogen bonds with hydroxyl, carbonyl, and methoxy groups. This mechanism was corroborated by DFT calculations, which showed that the energy barriers for the removal of most oxygen-containing functional groups were lowered by 1.7–72.4 kJ/mol. These results provide an in-depth understanding of the catalytic pyrolysis of lignin and pave the way for future research on the high-value utilization of waste lignin.
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NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 35
·15512-15523
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IF 2.7
Sen Fu,Hanxu Guo,Hong Yuan
A nano-ZSM-5 zeolite having a hierarchical pore structure was synthesized using L-lysine as a mesopore template and growth inhibitor. The effects of the L-lysine/Si and Si/Al molar ratios on the morphology and pore structure of the zeolite were studied. The products were characterized by scanning electron microscopy, transmission electron microscopy and N2-Brunauer–Emmett–Teller surface area analysis. These assessments showed that the particle size of the ZSM-5 zeolite could be reduced to 60 nm with a surface area as high as 395 m2 g−1 and a high density of mesopores. These zeolites were applied to the catalytic pyrolysis of oleic acid in a fixed-bed reactor to generate benzene, toluene and xylenes (BTX). At a reaction temperature of 500 °C, the catalyst having L-lysine/Si and Si/Al ratios of 0.4 and 30, respectively, gave a BTX yield of 27.4 wt%. This yield decreased with increases in the Si/Al ratio whereas varying the L-lysine/Si ratio did not produce a specific trend. The spent catalyst was characterized by thermogravimetric analysis and exhibited superior anti-coking ability and longer catalytic lifetime compared with a standard ZSM-5 zeolite.
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高影响因子
MOLECULES
·
2024
·Vol. 29
·期 14
·3417
·
IF 4.2
Pengfei Zhu,Zhaoxia Hu,Shouwen Chen
The development of economical catalysts that exhibit both high activity and durability for chlorinated volatile organic compounds (CVOCs) elimination remains a challenge. The oxidizing and acidic sites play a crucial role in the oxidation process of CVOCs; herein, praseodymium (Pr) was introduced into CrOx catalysts via in situ pyrolysis of MIL-101(Cr). With the decomposition of the ligand, a mixed micro-mesoporous structure was formed within the M-Cr catalyst, thereby reducing the contact resistance between catalyst active sites and the 1,2-dichloroethane molecule. Moreover, the synergistic interaction between chromium and praseodymium facilitates Oβspecies and acidic sites, significantly enhancing the low-temperature catalytic performance and durability of the M-PrCr catalyst for 1,2-dichloroethane (1,2-DCE) oxidation. The M-30PrCr catalyst possess enhanced active oxygen sites and acid sites, thereby exhibiting the highest catalytic activity and stability. This study may provide a novel and promising strategy for practical applications in the elimination of 1,2-DCE.
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PubMed
高影响因子
FLAVOUR AND FRAGRANCE JOURNAL
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2025
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IF 2
Xi Jiang,Jian Wu,Lucan Zhao,Jun Wang,Weiqiang Xiao,Zhen Chen,Jian Jiang,Miao Liang,Jiaqi Wang,Junsong Zhang
Different types of tobacco should exhibit significant differences in pyrolysis behaviour and pyrolytic aroma components distribution due to their intrinsic microstructures and chemical composition features but rarely be compared. Herein, the pyrolysis characteristics of three types of tobacco (oriental tobacco, burley tobacco and flue-cured tobacco) were studied by using thermogravimetric technique combined with thermal analysis kinetics method. The weight loss processes of each tobacco sample can be divided into four stages, namely dehydration, decomposition of volatile components, decomposition of hemicellulose and cellulose, and decomposition of lignin and carbonisation. Different types of tobacco exhibited various pyrolysis characteristic parameters in terms of T i , T f , DTG max , and CPI, indicating an obvious difference in the thermal decomposition characteristics of tobacco. And then a stepwise heating strategy was designed to in-depth investigate the pyrolysis characteristics and release behaviour of aroma components at different thermal weight loss stages by using the self-built infrared tube furnace combined with Cambridge filter capture system. The weight loss stages II and III would generate most of the aroma components for each type of tobacco. The release amount of oxygen heterocyclic and ketone compounds exhibited the order of flue-cured tobacco (558.90 μg·g −1 ) > burley tobacco (423.44 μg·g −1 ) > oriental tobacco (291.55 μg·g −1 ) during the four stages. The release amount of nitrogen heterocyclic compounds exhibited the order of burley tobacco>flue-cured tobacco>oriental tobacco, while the organic acids exhibited the opposite order. Furthermore, the physicochemical properties of biochar generated from different types of tobacco were characterised and compared by elemental analysis, Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). This study may provide guidelines for the rational utilisation of different types of tobacco leaves in related products.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
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2025
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IF 3.8
Jianning Zhang,Yanpei Dang,Tianhao Li,Yangzhong Zhao,Liantai Duan,Ke Chen,Xiao Zhang,Hengli Duan,Wensheng Yan,Sihua Feng,Gang Shao,Zhaoju Yu,Qing Huang,Yujie Song
Silicon boron carbonitride (SiBCN) ceramics have garnered significant attention due to their exceptional high-temperature stability, resistance to creep, and favorable electrical properties. However, the ceramicization mechanism of covalently bonded boron atoms in polyborosilazane (PBSN), which is crucial in determining the structural and crystalline phase evolution of silicon boron carbonitride (SiBCN) ceramics through the polymer-to-ceramic process, still needs further clarification for the design of advanced ceramics. Therefore, PBSN precursors constructed with B–C bonds were systematically investigated in the polymer-to-ceramic conversion process. B–C bonds were transformed into B-N bonds between 300°C and 600°C, ultimately resulting in the formation of h-BN at high temperatures. Meanwhile, higher levels (8.11–14.12%) of B facilitated the formation of SiC at equivalent temperatures but hindered the formation of Si 3 N 4 crystal nuclei. That is due to the formation of B–N and NB 3 units, which inhibited the formation of Si–N bonds and SiN 4 units, thereby interfering with the nucleation process of Si 3 N 4 and facilitating the crystallization of SiC. This study offers valuable insights for regulating the microphase evolution and properties of PDC nanocomposites.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Zhaoying Li,Feixing Li,Yaohui Fan,Zijun Zhang,Mengyu Wan,Songsong Zhang,Lianghuan Wei,Weizun Li,Xianghao Zha
Co-pyrolysis of polypropylene (PP) waste and cotton stalks (CS) addresses the dual environmental challenges of plastic pollution and agricultural residue disposal while leveraging their complementary properties (PP: H-rich; CS: C, O-rich) for enhanced H 2 production. This study investigated the hydrogen production mechanism of lignocellulose via microwave-assisted catalytic fast co-pyrolysis (co-MACFP) experiments and density functional theory (DFT) theoretical calculations for the conversion of CS and PP. Co-MACFP (550 °C) with a SiC absorber was applied to PP-CS blends (1:1 ratio), mesoporous HZSM-5 (tetrapropylammonium hydroxide (TPAOH)-modified, HT-1.0), and Ni-loaded HT-1.0 catalysts. The reaction mechanisms were determined via DFT simulations using β- d -glucopyranose and propylene as molecular models. The concentration of H 2 obtained from the co-pyrolysis of CS and PP (the ratio is 1:1) was 32.7 vol% without catalysts, which exceeds the average concentration of 28.4 vol% ((27.1 + 29.7)/2) at 550 °C, indicating a synergistic effect between CS and PP. In addition, synergistic effects boost the H 2 yield to 38.0 vol% with Ni-HT1.0 (vs. 32.7 vol% without catalysts), exceeding the theoretical averages from the individual feedstocks. PP-derived H· radicals (energy barrier: 454.8 kJ/mol) attack CS intermediates as the dominant low-energy pathway (204.4 kJ/mol), suppressing CO/CO 2 formation via DFT. This integrated strategy enables efficient waste valorization and generation of green hydrogen. Future work should scale up catalyst synthesis and explore hybrid processes to improve economic viability.
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JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Ge Zhu,Mengran Gao,Kejun Bi,Shanshan Zhao
The magnetic biochar is prepared for ciprofloxacin removal by adsorption, photocatalytic degradation and activation peroxodisulfate degradation. The magnetic biochar contains the ZnO, Fe 3 O 4 and FeNi with abundant pore structure, based on characterization analysis. According to Langmuir model analysis, the adsorption amount of ciprofloxacin is 505.16 mg/g. The adsorption mechanism analysis indicates that the surface functional group of magnetic biochar contributes to ciprofloxacin removal from wastewater. The magnetic biochar can be used as the photocatalyst for photocatalytic degradation of ciprofloxacin with removal of the 99.43 %. The ciprofloxacin can be also removed in the activation peroxodisulfate degradation system by reactive oxygen species. The magnetic biochar has excellent reusability in ciprofloxacin removal process. Bio-oil and bio-gas are produced by recycling of pyrolysis gas in the magnetic biochar preparation process. The bio-oil and bio-gas are rich in furfural and H 2 , respectively. Besides, the heating value of bio-gas is 12.35 MJ/Nm³.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2025
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IF 6.2
Wenjun Wu,Jiuhong Wei,Shihua Zheng,Jun Liu,Guojie Zhang,Ying Wang,Huihui Wang,Guoqiang Li,Yuqiong Zhao
The combustion of fossil fuels has led to excessive CO 2 emissions and severe climate impacts, making efficient CO 2 capture an urgent priority. Although chemical activation can enhance the CO 2 adsorption performance of biochar, its extensive use often entails environmental, equipment, and cost challenges. In this study, we present an innovative bio-templating strategy to synthesize hierarchically porous, heteroatom-enriched biochars derived from waste bamboo shoot shells and starch, using K 2 CO 3 as an activator and yeast as the bio-template. This method significantly reduces activator consumption compared with conventional activation processes. The optimized biochar, BAS 0.5 KC-800, exhibited exceptional CO 2 adsorption capacities of 5.15 mmol/g at 0 ℃ and 3.38 mmol/g at 25 ℃. Structural analysis revealed that its high specific surface area (1186 m 2 /g) and micropore volume (0.55 cm 3 /g) provide abundant CO 2 adsorption sites. Furthermore, the bio-templating process successfully introduced N and O heteroatoms into the carbon framework. These functional groups enhance the affinity between biochar and CO 2 through electronic interactions, ensuring excellent adsorption stability over multiple adsorption–desorption cycles. Isotherm and kinetic analyses indicate that CO 2 adsorption proceeds via a multilayer diffusion-controlled mechanism. Moreover, density functional theory (DFT) calculations reveal that N dopants facilitate CO 2 capture through hydrogen bonding, whereas O atoms strengthen dipole–quadrupole interactions. Overall, this study presents a sustainable and cost-effective approach to produce high-performance CO 2 adsorbents from waste biomass and provides comprehensive mechanistic insights into how heteroatom doping promotes CO 2 capture efficiency.
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高影响因子
FUEL
·
2024
·
IF 6.7
Yuxin Wen,Zhixian Bao,Zhengzheng Liu,Dekang Li,Haoquan Hu,Lijun Jin
Pyrolysis of waste tire (WT) is an efficient method to convert it into fuels and high-value chemicals. However, the main organic components of tire including natural rubber (NR), styrene butadiene rubber (SBR) and butadiene rubber (BR) usually exert interaction during pyrolysis . To investigate the interactions between different rubbers, individual pyrolysis and co-pyrolysis of three pure rubbers were conducted using an infrared-heating fixed-bed reactor, and the synergy during co-pyrolysis was revealed based on products distribution, tar quality and compositions from pyrolysis of pure rubber and waste tire. The results show that tar yields from rubber pyrolysis exceed 90 wt% and tar compositions are related to the molecular structures of rubbers. Co-pyrolysis between different rubbers promotes gases formation and inhibits char formation. The interaction between NR and SBR facilitates the formation of cycloolefin and chain olefin , but co-pyrolysis of SBR and BR contributes to the aromatic hydrocarbons formation. Similar tar components from pyrolysis of demineralized waste tire as those from pyrolysis of NR/SBR/BR sample indicate that waste tire pyrolysis contains individual pyrolysis and co-pyrolysis of different rubbers. The potential reaction process of WT was also proposed. The insight on interaction between different rubbers will provide a good guide for efficient pyrolysis of waste tire.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
·
IF 5.8
Liqiang Zhang,Ningmin Zhu,Chaochao Wang,Rongzheng Cui,Riyi Lin
Two-step catalytic pyrolysis of Nannochloropsis sp (NS) was conducted with SBA-15 and ZSM-5. Thermogravimetric analyzer (TG) and pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) were used to investigate the effects of SBA-15 and ZSM-5 on the two-step pyrolysis of NS. The comparative study showed that ZSM-5 and SBA-15 had different effects on the pyrolysis characteristic of NS because of their different property. ZSM-5 had no effects on the kinetic mechanism, but SBA-15 obviously changed DTG curves and the reaction order of the low temperature pyrolysis stage. SBA-15 increased the contents of amines and alkanes to 19.40% and 5.62% in the first step compared with those of the one-step pyrolysis (1.95% and 1.83%). Due to the stronger acid sites, ZSM-5 improved the content of olefins (33.79%) and esters (10.79%) in the first step and the contents of nitriles (11.75%) and aromatic hydrocarbons (31.01%) in the second step compared with those of one-step pyrolysis (10.61%, 5.41%, 0.00%, 8.42%). Acid catalyst had no positive effects on the generation of N-heterocyclic compounds. This study is expected to provide a reference for the efficient pyrolysis utilization of microalgae.
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
·
2024
·
IF 5.3
Wen-luan Xie,Bin Hu,Xiao Yang,Ji Liu,Zhi-mo Fang,Kai Li,Yang-wen Wu,Bing Zhang,Qiang Lu
Phosphoric acid is an effective and widely used catalyst for biomass pyrolysis, with significant catalytic impact on the pyrolytic reactions and product distribution. However, its fundamental catalytic mechanism in lignin pyrolysis remains unclear. In this work, we proposed and investigated three possible H 3 PO 4 -assisted pyrolysis mechanisms, i.e., hydrogen-bond-induced decomposition, phosphoric-acid-assisted hydrogen transfer (H 3 PO 4 -AHT), and phosphorolysis, and carefully discussed them through theoretical calculations, electronic structure analyses, catalytic pyrolysis experiments using the β -O-4 linked lignin model. The results indicated that the H 3 PO 4 -AHT mechanism played a dominant role in lignin catalytic pyrolysis, superior to the other two mechanisms. The phosphoric acid molecule could take advantage of its unsaturated P = O and saturated P −OH groups for hydrogen donation and acceptance in concerted H 3 PO 4 -AHT reactions. Alternatively, it could also participate in concerted intermolecular hydrogen transfer with the active hydroxyl group as a mediator. The C β −O bond cleavage could be significantly enhanced by effectively reducing the tension of the transition state ring, leading to the generation of more phenol and styrene in pyrolysis experiments. Due to the inhibition of hydrogen abstraction, C α −C β breakage of β -O-4 linkage, side chain removal of primary products, etc., the formation of other products in phosphoric acid catalytic pyrolysis of β -O-4 linked lignin was restrained. This H 3 PO 4 -AHT catalytic mechanism was also confirmed to be conductive to tautomerism, elimination, dehydration, α -O-4 linkage fracture, β -1 linkage fracture, and other important decomposition reactions in lignin pyrolysis. The understanding of these mechanisms provides valuable insights into the role of phosphoric acid in lignin pyrolysis and may guide the development of effective biomass catalytic conversion methods.
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