ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Sijie Li,Yiting Wu,Ayyaz Mahmood,Jin Liu,Ziqi Xu,Kaiyang Lu,Moshe Sheintuch,Xi Gao
The coupling of fast pyrolysis with green catalysis offers a sustainable approach for transforming waste polypropylene (PP) plastic into valuable hydrogen and carbon materials. The intrinsic catalytic activities of biochar, Al2O3@biochar, Fe3O4@biochar, Fe2AlO4@biochar, and FeAl2O4@biochar are explored for upgrading the fast pyrolysis vapors of PP powder. The FeAl2O4@biochar catalyst with tetrahedral iron sites achieves an excellent hydrogen yield, equivalent to 86.25 H% in PP. The hydrogen yield from converting practical PP mask waste reaches 57.98 ± 1.96 mmol gplastic–1, more than 673.61 ± 7.00 mmol gFe–1. The density functional theory (DFT) calculation indicates that a closer d-band center of FeAl2O4 is more favorable for C–H bond activation and that dehydrogenation of propylene as a model compound is the primary source of hydrogen production, more readily than C–C bond cleavage, and efficiently generates H2.
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APPLIED THERMAL ENGINEERING
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2025
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IF 6.9
Tianbao Liu,Weiguang Shi,Wei Li,Benxian Li,Xiaofei Fu,Zhiyong Chang,Sunhua Deng
Low to medium maturity shale oil, an essential energy source, faces challenges due to traditional pyrolysis methods, which are characterized by high energy consumption, low yield, and poor selectivity. Moreover, the inefficiencies in in-situ heat injection underscore the necessity for effective catalysts and improved heat transfer mechanisms involving water vapor. This study aims to elucidate the heat transfer enhancement and catalytic synergy of NiFe-layered double hydroxides (NiFe-LDH) in improving the in-situ pyrolysis efficiency of medium–low maturity oil shale via steam pyrolysis. Analyses conducted using GC–MS, Raman spectroscopy, and 13 C NMR demonstrated that the incorporation of NiFe-LDH with water vapor significantly enhances kerogen pyrolysis. This process increases the yields of alcohols, alkanes, and olefins by 1.32, 1.21, and 1.81 times, respectively, and it reduces the temperature needed to produce oil from kerogen. The catalyst helps turn aromatics into alcohols, olefins, and alkanes while breaking down residues into short-chain alkanes. It does this by weakening C–H bonds and removing hydrogen from methyl groups, ultimately reducing the energy required for heat injection by 38.17 %. Thermal and kinetic studies reveal that NiFe-LDH increases kerogen thermal diffusivity by 75.5 % and decreases specific heat capacity by 28.1 %, while elucidating the kinetic mechanism for a 59 °C elevation in the initial temperature of the main pyrolysis stage (increasing 6.1 times prefactor). A nucleation-reaction-order-geometric contraction multi-mechanism coupling model is established. This work proposes a novel “catalyst-water vapor pyrolysis-kerogen oxidation” synergistic enhancement theory, refining the multi-scale coupling mechanisms of heat/mass/chemical reactions during in-situ oil shale pyrolysis.
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Waste and Biomass Valorization
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2024
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IF 2.6
Luo Bo,Liu Huiyu,Shan Rui,Zhang Jun,Yuan Haoran,Chen Yong
Purpose This work aims to investigate the thermal behavior and kinetic characteristics of polyethylene (PE) pyrolysis over Cu/Ce modified ZSM-5. The influences of metal types, particles size of active center and interaction of Cu–Ce species on products distribution are elucidated. Methods Metal-modified ZSM-5 catalysts were prepared by negative pressure impregnation method. Catalytic fast pyrolysis and thermogravimetric experiments were conducted using Py–GC/MS and TG/MS for the qualitative and quantitative analysis of pyrolysis products. Results Morphology characterization indicated the interaction of Cu–Ce species facilitated the regulation of active center size into a nanoparticle scale. The final products were restricted to a carbon number of less than 9 over CuCe/ZSM-5. Cu–Ce modification increased the aliphatic content from 58.5 to 76.1%. Kinetic analysis revealed a remarkable reduction in activation energies during both the intermediate and final stages, where an average decrease of 30% was achieved. Conclusion The synergistic effects of Cu 0 and CeO x facilitated the formation of more short chain olefins by enhancing C–C bonds cleavage activity. Undesired polycyclic aromatic hydrocarbons (PAHs) were avoided by the optimal steric hindrance of CuCe/ZSM-5. Graphical Abstract
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Small Methods
·
2024
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IF 10.7
Yifan Dai,Jie Ju,Liling Luo,Hao Jiang,Yanjie Hu,Chunzhong Li
The synthesis of high-entropy alloys (HEAs) with ultra-small particle sizes has long been a challenging task. The complex and time-consuming synthesis process hinders their practical application and widespread adoption. This study presents the novel synthesis of TiO 2 nanoparticles loaded with a quinary high-entropy alloy through flame spray pyrolysis (FSP) for the first time. The extremely fast heating rate of flame combustion makes the precursor fast pyrolysis gasification, high temperature in the flame field promotes the metal vapor mixing uniformly, and the fast quenching process can reduce the particle aggregation sintering, the ultra-small particle size of HEA firmly attached to the TiO 2 surface. The catalysts prepared via this gas-to-particle pathway exhibit excellent performance in CO 2 hydrogenation, achieving a conversion rate of 62% at 450 °C, and maintaining their activity for over 220 h without significant particle agglomeration. This finding provides valuable insights for the future design of catalytically active materials with enhanced activity and long-term stability.
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PubMed
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
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IF 5.8
Wei Yu,Xijie Ban,Chao Liu,Qibin Li,Liyong Xin,Zhengyong Huang,Shukun Wang
In actual organic Rankine cycle systems (ORCs), the inclusion of lubricating oil in the working fluid is nearly unavoidable. Under the condition of high-temperature operation, the presence of lubricating oil can potentially exacerbate the thermal stability of the working fluid. The impact of polyol ester (POE) and mineral lubricant on the thermal stability of octadethyltrisiloxane (MDM) is studied. Results indicate that both POE and mineral lubricant contribute to the decomposition of MDM to a certain extent. Specifically, at a 5.0% mass fraction of POE and mineral lubricant, MDM remains its stable at 230 °C and 210 ℃, respectively. However, as the mass fraction of lubricant increases, the decomposition of MDM intensifies, with mineral lubricant exhibiting a more pronounced effect compared to POE lubricant. Regarding pyrolysis products, the presence of lubricants leads to an increase in CH 4 , C 2 H 6 and C 2 H 4 gases. Furthermore, the addition of lubricant promotes the formation of siloxane oligomers , particularly MD 5 M to MD 9 M, and enhances the production of unidentified products. Compared to MDM, both POE and mineral lubricant molecules exhibit lower bond dissociation Gibbs free energies . The free radicals generated from lubricant decomposition are prone to hydrogen abstraction reactions with MDM to promote MDM decomposition. Moreover, ReaxFF simulation results demonstrate that lubricant molecules also enhanced the activation of MDM and increased its susceptibility to Si-C bond cleavage . Following the removal of the methyl group , the Si-O bonds in the radicals are more likely to break, leading to the formation of additional siloxane oligomers through Si-O bond recombination. Kinetic analysis reveals that the apparent activation energy of MDM decomposition drops from 134.4 kJ∙mol −1 to 110.8 kJ∙mol −1 as the mass fraction of n-hexadecane (model compounds for mineral lubricant) rises from 0% to 10.30%.
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NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Wenli Liu,Pei Chen,Yanzhi Sun,Chuanjin Huang,Yongmei Chen,Jun Guo,Junqing Pan,Pingyu Wan
Conversion of pyrolysis carbon black (CBp) derived from waste tires into activated carbon for industrial wastewater treatment could be a sustainable waste reuse opportunity. However, untreated CBp has low surface activity and contains large amounts of ash and carbonaceous deposits. In this study, a highly efficient multifunctional adsorbent was successfully synthesized by converting CBp into hierarchical porous carbon featuring micro-, meso-, and macropore structures via a facile and scalable one-step KOH high-temperature molten chemical activation approach. The acid pretreatment was not as effective as KOH activation in removing ash from the adsorbents produced. The adsorption capacities and mechanism of the direct activated carbon black (ACBp) for methyl orange (MO) and methylene blue (MB) adsorption were also examined. ACBp with a hierarchical porous structure showed a high SBET value of 789 m2 g−1, far higher than CBp (49 m2 g−1), which enables ACBp to exhibit rapid adsorption kinetics for MO and MB. Batch adsorption experiments demonstrated that ACBp achieves maximum adsorption capacities of 390.6 mg g−1 for MO and 444.4 mg g−1 for MB. In addition, the removal of MO and MB was 90% and 80% after 5 cycles, respectively, indicating the good regeneration performance of ACBp, which has great potential for industrial applications. This work offers a feasible pathway to realize high-value recycling of waste tires and reduce the contamination of dye wastewater.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Tiefeng Xu,Chenyu Li,Ke Xiang,Yingxin Lu,Wangyang Lu
The photocatalytic removal of organic pollutants from wastewater has gained significant attention in recent years due to its environmental benefits and cost-effectiveness. In this study, a pyrolytic iron phthalocyanine/graphitic carbon nitride (FePc/g-C 3 N 4 ) composite photocatalyst was synthesized using ball milling and thermal cracking, and its performance in photocatalytic degradation along with the underlying mechanisms was investigated. Under solar light irradiation, the pyrolytic FePc/g-C 3 N 4 photocatalyst achieved complete carbamazepine (CBZ) degradation within 12 min by activating peroxymonosulfate (PMS), demonstrating a 29 % enhancement in degradation efficiency compared to the unpyrolytic FePc/g-C 3 N 4 . Additionally, the stability of the catalyst improved significantly post-pyrolysis, maintaining over 98 % degradation efficiency across nine cycles. The thermal treatment disrupted the phthalocyanine structure, modifying the coordination environment of the central Fe atom and facilitating the transfer of photogenerated charge carriers. This research provides valuable insights for designing stable single-atom iron-based composite photocatalysts.
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BIOMASS & BIOENERGY
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2025
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IF 5.8
Shiting Chen,Sisi Jia,Nan Xi,Qinglian Wang,Yixiong Lin,Chen Yang,Wang Yin,Ting Qiu
Noble metal catalysts, particularly Ru-based, demonstrate exceptional activity during catalytic hydrotreatment of fast pyrolysis liquids (PLs) from lignocellulosic biomass. However, their high cost poses a major barrier to practical applications. Herein, a series of cost-effective bimetallic Ru-Ni catalysts with varying Ru/Ni ratios (5 wt% metal loading, Ru x Ni y /NC) supported on hierarchical nitrogen-doped carbon materials (NC) were facilely prepared by the wet impregnation method. The performance was evaluated for catalytic hydrotreatment of PLs. The results revealed that the introduction of Ni to Ru significantly enhances catalytic performance. Among the tested catalysts, Ru 4 Ni 1 /NC exhibited optimal activity, achieving the product oils with the highest H/C ratio and lowest thermogravimetric (TG) residue. Under mild condition (200 °C, 6 MPa H 2 , 4 h), the catalyst yielded the product oil with an H/C ratio of 1.49 and a TG residue of 10.7 wt%. When subjected to deep hydrotreatment condition (340 °C, 6 MPa H 2 , 4 h), the catalyst generated the product oil with an H/C ratio of 1.32 and a TG residue of 2.9 wt%. To gain insights into the catalytic mechanism, the adsorption behavior of model components in PLs onto the catalyst was investigated through FT-IR. The results revealed that the incorporation of low electronegativity Ni to Ru, induces the electron transfer from Ni to Ru, resulting in electron enrichment at Ru sites and electron deficient at Ni sites, which promotes the adsorption of substrates onto the catalyst, thereby boosting hydrogenation of PLs. These findings highlight the significant potential of bimetallic Ru-Ni/NC for catalytic hydrotreatment of PLs into intermediates that can be co-processed with vacuum gas oil in FCC refinery for biofuel production.
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FUEL
·
2022
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IF 8.035
Maolin Xu,Chengyang Cao,Hongyun Hu,Yang Ren,Guangzhao Guo,Lifang Gong,Junwei Zhang,Tong Zhang,Hong Yao
With the massive production and discard of PVC artificial leather, it is urgently needed to find an efficient and environment-friendly method to dispose of this material made from PVC and blended cloth (BC). As a widely accepted way to dispose of municipal solid waste, pyrolysis was chosen for this study. The pyrolysis experiments of PVC, BC, and their mixture were conducted to characterize PVC artificial leather’s pyrolysis behavior and product characteristics. TG-FTIR and kinetics analysis showed the strong synergistic effect between PVC and cellulose in BC occurred at 240 °C – 314 °C, resulting in cellulose dehydration and aromatization. An exceptionally high tar yield of 54.96 wt% was obtained by fast pyrolysis of the mixture at 500 °C. GC–MS analysis of tar proved BC consisted of cellulose, PET, and PA. The high tar yield of co-pyrolysis came from the synergistic effects of PVC on cellulose and PET, both of which formed terephthalic acid, di(2-chloroethyl) ester (TADE). At 500 °C, the tar of the mixture mainly contained TADE (18.72 wt%), terephthalic acid (18.56 wt%), and aromatics (19.04 wt%). The co-pyrolysis interaction mechanism at 500 °C was deduced. Our study could provide theoretical guidance for recycling PVC artificial leather waste.
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PROCEEDINGS OF THE COMBUSTION INSTITUTE
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2022
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IF 6.535
Xing Yuan,Chaohe Zheng,Zuwei Xu,Qinghua Yang,Tiantian Zhang,Xi Luo,Haibo Zhao
Photothermocatalytic oxidation is an environmentally-friendly, low-temperature, and high-efficient method to remove the air pollutant. Yet, the lack of active, inexpensive, and superior stability catalysts has greatly limited its extensive utilization. In this work, the effect of single-atom Pt loading on TiO 2 support has been theoretically and experimentally studied to improve photothermocatalytic performance for the toluene combustion through flame spray pyrolysis (FSP). Pt loading can play two crucial roles into TiO 2 optimization: (1) The low-valence Pt cation incorporated into TiO 2 lattice is dramatically responsible for the anatase-rutile transformation (ART) and formation of sufficient oxygen vacancies ; (2) Introducing the defect energy level and Pt-3d orbitals remarkably promote the charge separation efficiency of single-atom catalysts. Moreover, the existence of single-atom Pt nanoparticles can signally boost the activity of surface adsorbed and lattice oxygen, as well as substantially reduce the oxygen vacancy formation energy. Thus, the toluene removal under light irradiation reaches 90% conversion below 160 °C and is maximally 18 °C lower than that under only thermocatalytic oxidation. It is attributed to larger specific surface area (SSA), outstanding low-temperature reducibility, extremely dispersed hybrid PtO x , more surface active oxygen, and higher mobility of bulk oxygen. Interestingly, when the oxygen-fuel equivalent ratio φ distinctly increases by shifting precursor solvent from xylene to ethanol, the photothermocatalytic property of toluene can be remarkably enhanced on single-atom Pt catalysts. It is due to the higher Pt dispersion resulting from more intense burning and drastic turbulent mixing, as well as the superior ratio of the metallic Pt active sites originating from higher flame temperature. Eventually, the rate-determining step of C 7 H 8 combustion on Pt/TiO 2 and Cu/TiO 2 slab are all the C C bond fracture of maleic anhydride to form acetic anhydride species, with the energy barriers of 112.03 and 188.74 kJ/mol, respectively.
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POLYMER SCIENCE SERIES B
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2021
·Vol. 63
·期 4
·358-366
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IF 1.049
Danbo Mao,Yuechuan Wang
Abstract Four 2,5-dicholorobenzoate monomers were prepared by chlorination and esterification and then polymerized to ester substituted poly( p -phenylene)s through Ni/Zn catalyzed coupling reaction. The thermal stability and pyrolysis behavior of ester substituted poly( p -phenylene)s were investigated through TGA method. The possible mechanism of thermal modification of the polymers was proposed that included de-esterification, dehydration and decarboxylation, and finally de-anhydridization. Only pyrolysis of esters substituted poly( p -phenylene)s containing two neighboring carboxyl groups may result in the formation of the corresponding anhydride.
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ENERGY & FUELS
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2020
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IF 3.421
Tawanda Matamba,Arash Tahmasebi,Salman Khoshk Rish,Jianglong Yu
This study reports the role of pressure (0.1–4.0 MPa) and temperature (600–900 °C) in flash pyrolysis of palm kernel shell (PKS). The main objective was to study the extent to which pressure affects the mechanism of pyrolysis reactions to enhance the selective production of target products. Higher pressures and temperatures selectively promoted the generation of polycyclic aromatic hydrocarbons (PAHs) and H2 gas. Bio-oil samples generated at lower temperatures and pressures were mainly composed of phenolics. Increasing the pressure and temperature favored the selective formation of phenanthrene, fluoranthene, pyrene, fluoranthene, and fluorene, which reached 96.17 area %. Elevated temperatures and pressures enhanced hydrogen transfer into a light gaseous phase. The yield of H2 peaked at 40.82 g of H2/kg of PKS at 900 °C and 2.0 MPa. The results obtained in this study implied that the pyrolysis of biomass at elevated pressures can be an effective method for polygeneration of hydrogen gas and PAHs as chemical feedstocks.
研究领域:
能源科学
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环境科学
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