JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Peng Song,Congcong Li,Ningmiao Zhao,Zhenyuan Ji,Linzhi Zhai,Xiaoping Shen,Qi Liu
Carbon nanosheets with heteroatom doping and well-developed porosity exhibit broad application foreground for Zn-ion hybrid supercapacitors (ZHSCs), but the simple and controllable preparation is still of great challenge. In this study, by using LiCl-KCl as in-built templates, histidine as carbon and nitrogen sources, and KNO 3 , K 2 SO 4 , KOH or Na 2 S 2 O 3 as active agent, a series of N and N S doped porous carbon nanosheets are developed. Results indicate that, with the activator introduction, pore structures of the carbonized products are notably boosted, showing an astounding 30–244 % increase in BET specific surface area, and meanwhile, heteroatom with a content of ca. 12 % can be doped into the resultant carbon skeletons. Specifically, the NSPCN-800 (activated by Na 2 S 2 O 3 ) with a large specific surface area of 1297 m 2 /g, a hierarchically porous structure composed of abundant micropores and mesopores, and a suitable heteroatom content (N: 11.9 wt%; S: 0.6 wt%) presents an impressive energy storage behavior as cathode for ZHSCs, including a specific capacitance of 165.8F/g, a specific capacity of 95.2 mAh/g, an energy density of 59.0 Wh kg −1 and a cyclic stability with a 82.6 % capacity retention after 5000 cycles. These performance parameters surpass numerous reported ZHSCs, making NSPCN-800 a very promising cathode for practical use.
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
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IF 6
Yongdi He,Jinou Song,Jiuzhong Yang,Yuan Zhuang,Liang Qiu,Zhijun Li,Shubao Song,Jibiao Xie
An experimental study of 5% 1 -nitropropane (1-NP)-initiated cyclohexane pyrolysis was carried out in a flow reactor at 30 Torr (4.0 kPa) over a temperature range of 673–1273 K. The pyrolysis species were detected with synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) technique. Pyrolysis species from m/z 15–106, including C 1 -C 8 hydrocarbons, CO, NO, NO 2 , CH 2 O, CH 3 OH and C 3 H 5 NO, were identified with near-threshold photoionization efficiency (PIE) spectra and quantified at different temperatures. The experimental results indicated that the addition of 1-NP obviously reduced the initial pyrolysis temperature of cyclohexane from 1048 to 1098–723 K, and caused the decreases of the initial formation temperatures for the species from cyclohexane pyrolysis. Almost all the high-temperature pyrolysis species in the mechanisms proposed in the literature were identified in the experiments. Based on the experimental results in this work and rate coefficients proposed in the literature, the primary pyrolysis mechanisms of cyclohexane in the presence of 1-NP were discussed. The 1-NP pyrolysis occurs at a lower temperature than the cyclohexane does, and produces HONO, NO 2 , C 3 H 7 , etc. It was demonstrated that cyclohexane was mainly consumed via the H-atom abstractions by H and OH attacks in this work and the cyclohexyl radical formed via H-atom abstractions mainly isomerized into 1-C 6 H 11 -6 radical, which further combines with H to form 1-C 6 H 12 .
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
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IF 6
Hongyan Wang,Yurou Zhou,Jingpei Cao,Bofeng Zhang,Yajie Tian,Guozhu Liu
Adamantane derivatives, as promising high-density fuels, have been widely concerned in fields of volume-limited aerospace vehicles due to high density, heat of combustion and thermal oxidation stability. To reveal insights into their high-temperature decomposition behaviors, an experimental and theoretical investigation of adamantane (A) and 1-methyl adamantane (1-MA) pyrolysis was performed in a flow tube reactor at atmospheric to high pressure. Over twenty species were detected and identified, including C1-C5 light hydrocarbons, C5-C7 cyclic olefins as well as C6-C12 aromatics. The favorable decomposition channels of A and 1-MA are proposed and the effects of fuel structure characteristics and pressures on product formation behaviors are revealed. For the primary decomposition of A and 1-MA, the contributions of reaction types exhibit the obvious dependence on the pressures and temperatures, involving the unimolecular C-C dissociations by ring-opening, CH 3 -elimination as well as H-abstractions by H and CH 3 attacking. Considering methyl-substitution weakens dissociation energies of C-C and C-H bonds and leads more H-abstraction sites, 1-MA shows a higher pyrolysis reactivity than A. The effects of structure characteristics are also embodied in the formation of newly chain-branched unsaturated species and the concentrations of common small hydrocarbons and aromatics. Compared to A decomposition, the methyl substituent in 1-MA promotes the emergence of 1-butene, 2-methyl-1-butene, mesitylene, methylindane and methylnaphthalene, and increases the concentrations of methane, 2-methylpropene and xylene isomers, formed via β-scission, hydrogen transfer, isomerization and dehydrogenation routes of fuel radicals. Meanwhile, more methyl-substitutions accelerate the decomposition of alkyl-adamantanes and pyrolysis activity follows by a sequence of dimethyl-adamantane > methyl-adamantane > adamantane, boosting the production of methyl-specific species.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 39
·18272-18284
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IF 3.3
Kai Zhang,Xiangyi Liu,Jiajun Bi,Amal BaQais,Ben Bin Xu,Mohammed A. Amin,Ying Hou,Xianglong Liu,Handong Li,Hassan Algadi,Juan Xu,Zhanhu Guo
Bimetallic NiCe/Lay catalysts were prepared using an impregnation method with a Lay molecular sieve as a carrier, and oleic acid (OA) as a model compound of unsaturated fatty acid for catalytic pyrolysis to prepare bio-airline fuel. Based on the reaction products, the reaction pathways of the products under the bimetallic NiCe/Lay catalyst were deduced. The bimetals were dispersed uniformly on the support Lay, and the catalyst retained the structure of the molecular sieve after loading and had good physical properties such as specific surface area and pore space. Under optimal conditions (pyrolysis/catalytic temperature = 500/500 °C, catalyst loading = 1.0 g, feedstock injection volume =0.5 mL min−1, and OA to methanol ratio = 1 : 5), 100% conversion, 92.77% hydrocarbon yield, and 75.06% hydrocarbon yield in the range of 8–17 carbon atoms were obtained over the Ni–3Ce/Lay catalyst. This study provides highly efficient catalysts for upcycling oleic acid and methanol for producing fuel.
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FUEL
·
2022
·
IF 8.035
Wei Feng,Mo Zheng,Lijun Jin,Jin Bai,Lingxue Kong,Huaizhu Li,Zongqing Bai,Wen Li
Co-pyrolysis of waste plastics and low-rank coal is a promising approach to deal with the serious waste crisis and improve the clean utilization of low-rank coal. In this work, the comprehensive co-pyrolysis behaviors of low-rank coal and polyethylene plastics were explored systematically by combining TG experiment, in-situ Py-TOF-MS technique, and ReaxFF MD simulation. The consistent results were obtained among three approaches to demonstrate the positive interaction exists between coal and PE during the co-pyrolysis process, which leads to volatile yield increasing with PE addition. TG experimental results showed that the blending ratio of 7:3 for coal and PE has the strongest synergy during the co-pyrolysis process, while Py-TOF-MS experimental results unraveled that the synergistic effect of coal and PE was determined by changing the content of pyrolysis products rather than by producing cross-reaction products. The PE addition significantly reduced the yield of MAHs and normal alkyl-substituted monophenols and increased the yield of olefins, alkanes, and aromatic derivatives. ReaxFF MD simulation results complement the experimental observation to obtain similar weight loss profiles with TG experiments and consistent identification of major representative tar pyrolyzates with Py-TOF-MS experiments. Particularly, the detailed gas evolving trends and the underlying bond-breaking reactions of C C, C O, and C H bonds were revealed by ReaxFF MD, which indicates PE addition promotes bond breaking of C C and C H to enhance more tar generation. The combination of experiments and ReaxFF MD simulations can capture the comprehension of the co-pyrolysis process between low-rank coal and PE, which can be extended to other co-pyrolysis applications for related solid fuels.
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高影响因子
Journal of Cleaner Production
·
2022
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IF 11.072
Bin Zhang,Meng Mei,Kaiwei Li,Jingxin Liu,Teng Wang,Si Chen,Jinping Li
Magnetic biochar adsorbents often suffer from the uneven distribution and shedding problems of nanoparticles . In this study, a one-pot sol-gel pyrolysis method was proposed to synthesize a MnFe 2 O 4 functionalized magnetic sawdust-based biochar (MnFe 2 O 4 @SBC) for efficient removal of diclofenac sodium (DCF). The MnFe 2 O 4 @SBC was characterized by XRD , Raman, VSM, TG-DSC, SEM, TEM, BET, FTIR and XPS . The results demonstrated that the combination of sol-gel and sawdust effectively led to a homogeneous distribution of MnFe 2 O 4 on biochar and the MnFe 2 O 4 @SBC possessed a much richer pore structure and functional groups than the original biochar. A systematic comparison of MnFe 2 O 4 @SBC with commercial activated carbon (CAC) was conducted by analyzing the effects of initial pH, adsorbent dosage, coexisting ions, contact time and temperature on their adsorption performance. Based on the adsorption isotherm study, the maximum adsorption capacity of MnFe 2 O 4 @SBC was predicted to be 352.17 mg/g, which was almost 3.5 times that of CAC. Selectivity adsorption study and real water-based removal experiment further demonstrated the satisfactory adsorption selectivity and applicability of MnFe 2 O 4 @SBC for DCF. This study reveals that the one-pot sol-gel pyrolysis is a promising method for synthesizing excellent magnetic biochar adsorbents.
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高影响因子
Polymers
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2022
·Vol. 14
·期 18
·3888
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IF 4.967
Yingying Zhong,Qibei Bao,Lifeng Yuan,Jiawen Liu,Yan Cai,Xianfeng Chen
Microplastics are harmful to both marine life and humans. Herein, a pyrolysis–gas chromatography–mass spectrometry (Py-GC/MS) technique for the detection of microplastics in aquatic shellfish is demonstrated. The organic matter in aquatic shellfish was removed by alkali digestion. Subsequently, using hexafluoroisopropanol as the extraction solvent, the extraction method was optimized. The influence of the digestion process on the nature of microplastics was investigated by analyzing the samples before and after the alkali treatment via infrared spectrometry, laser particle sizing, and scanning electron microscopy. Spiked recovery experiments and an analysis of actual samples were performed using PA6 and PA66 as analytes. A quantitative analysis of the characteristic ion fragment produced by high-temperature cracking was performed after chromatographic separation and mass spectrometry identification. The linear range of this method for PA6 and PA66 was 2–64 μg. The limits of detection of PA6 and PA66 were 0.2 and 0.6 μg, while the limits of quantitation were 0.6 and 2.0 μg, respectively. Recovery ranged from 74.4 to 101.62%, with a precision of 4.53–7.56%. The results suggest that the Py-GC/MS technique is suitable for the analysis and detection of trace microplastics in aquatic shellfish.Keywords:microplastics;alkali digestion;pyrolysis–gas chromatography–mass spectrometry;aquatic shellfish;nylon
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ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Jinxin Li,Dan Zhong,Yiru Chen,Kefei Li,Wencheng Ma,Shaobo Zhang,Jingna Zhang,Aoshuang Sun,Haijiao Xie
Coal pyrolysis wastewater (CPW) contained all kinds of toxic and harmful components, which would seriously threaten the natural environment and human health. However, the traditional advanced oxidation processes frequently failed to remove phenolic substances. An A 2 BO 4 -type perovskite (La 2 CuO 4 ) was successfully synthesized through sol-gel process and first applied in the treatment of CPW. More than 90% of 3, 5-dimethylphenol (DMP) was removed within 200 min at neutral conditions. Moreover, La 2 CuO 4 also displayed excellent catalytic activity and stability in the actual CPW treatment process. Results demonstrated that DMP was removed through the attack of ∙OH, ∙O 2 − and 1 O 2 in La 2 CuO 4 /H 2 O 2 system. The La 2 CuO 4 were more favorable for H 2 O 2 activation and have a lower adsorption energy than LaFeO 3 . XPS of fresh and spent La 2 CuO 4 illustrated that the decomposition of hydrogen peroxide (H 2 O 2 ) was mainly due to the redox cycle between surface copper and oxygen species. Moreover, the possible degradation pathway of DMP was deduced by identifying degradation products and analyzing density functional theory (DFT) calculations. This research provided a novel strategy for the development of perovskite-based catalytic materials on the treatment of practical CPW.
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FUEL
·
2022
·
IF 8.035
Peng Liu,Yuanyuan Zhang,Tieying Pan,Dexiang Zhang,Lishi Chen,Changrong Sun
Coal conversion to material or chemical by pyrolysis is the main methods for achieving carbon neutrality. To predict correct pyrolysis behavior, accurately quantifying carbon structural types of complex coal discussed in this study is significative. Carbon structural types in coal based on 13 C NMR Cp/MAS TOSS spectra were accurately quantified by coupling standard curve and peak-fitting method to reduce nuclear overhauser effect (NOE). The H/C atomic ratio and aromaticity is used to verify the accuracy of this method. The pyrolysis behavior was predicted by pyrolysis Gas Chromatography-Mass Spectrometer (Py-GC-MS), thermogravimetric analysis (TG), and fix-bed slow pyrolysis according to correction carbon structure. The results show that the H/C atomic ratio calculated by correction carbon structure is agreed with that from ultimate analysis, as well as aromaticity. Their correction relative deviations are below 10%, farther lower than experimental value, increasing with the increment of C daf %. The correction carbon structure evolution during pyrolysis is coincided with general conclusion and Py-GC-MS analysis. The mono-aromatics and phenolics are evaluated by correction carbon structure. It is significantly fundamental study for carbon material to chemicals from micro-angle. These results are also a guide for accurate calculation and simulations of quantum chemistry.
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高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Liuqun Fan,Zhiyan Hou,Tianbao Liu,Xiangjing Liang,Andrei Ivanets,Kongjun Ma,Xintai Su
Heteroatom-doped carbon materials derived from oil-bearing sludge exhibit excellent supercapacitor performance due to their unique electronic and chemical properties. However, the complex composition of heteroatoms in oil-bearing sludge makes it difficult to achieve sufficient and directional doping by direct pyrolysis . In this paper, an oleic acid pretreatment-roasting-secondary activation strategy was developed to make full use of hydrocarbons, iron- and nitrogen-containing compounds in oil-bearing sludge to prepare Fe-N X -C materials with excellent electrochemical properties. Characterization results such as transmission electron microscopy (TEM) and N 2 adsorption analysis showed that the best sample had a hierarchical pore structure and uniform Fe and N element loading. X-ray photoelectron spectroscopy (XPS) analysis found that the addition of oleic acid can promote the formation of Fe-Nx, and the dosage of oleic acid will affect the content of Fe-Nx in the carbon materials. Electrochemical characterization of this supercapacitor material was conducted. The best sample's specific capacitance was as high as 293.6 F g −1 at the current density of 0.5 A g −1 , and the capacitance retention rate could still reach 71.5% at the current density of 10 A g −1 . The assembled button-type symmetrical supercapacitors had an energy density of 8.68 Wh kg −1 and a power density of 137.53 W kg −1 , which is much higher than those of most other waste-based carbon materials. This work presents a new idea for the preparation of heteroatom doped carbon materials with excellent capacitive properties from oily sludge, which provides a new reference for the treatment and resource utilization of oily sludge.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Dun Fu,Tonni Agustiono Kurniawan,Herong Gui,Heng Li,Songbao Feng,Qingbiao Li,Yuanpeng Wang
This study investigated the effects of pyrolysis temperature on the physicochemical properties of pyrolyzed hydrochars (PHCs) and H2O2-catalyzed tetracycline (TC) degradation in a combined treatment with PHC and CuxO@PHCs. The effects of pH on TC degradation by CuxO@PHCs were also evaluated in the presence of H2O2 and compared with that by CuxO@GAC. To analyze their physicochemical changes due to the oxidant, the carbocatalysts were characterized using scanning electron microscopy (SEM), X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) analysis, and Fourier transform infrared (FTIR) spectroscopy. To sustain its cost-effectiveness, spent CuxO@PHC700 was regenerated using NaOH. Based on the characterization results, increasing the pyrolysis temperature from 300 to 700 °C enlarged their specific surface area and pore volume. The X-ray diffraction (XRD) analysis revealed that the Cu anchored in the carbocatalyst existed as Cu2O/CuO. The H2O2-catalyzed degradation by CuxO@PHC700 (0.231 min–1) was faster than that by CuxO@PHC500 (0.107 min–1), CuxO@PHC300 (0.013 min–1), and CuxO@GAC (0.041 min–1) (p ≤ 0.05; analysis of variance (ANOVA)). The maximum TC removal was achieved by CuxO@PHC700 at pH 6 due to the H-bonding and Cu-bridging effects between the Cu-loaded carbocatalyst and TC molecules in solutions. Treated effluents could meet the maximum discharge limit standard of 1 mg/L set by the local legislation. After the first regeneration, the spent CuxO@PHC700 could attain about 96% of TC degradation. This implies that the saturated carbocatalyst still had promising catalytic activity for reuse. Overall, CuxO@PHC is a cost-effective option for TC removal from contaminated water.
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高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Fuping Li,Yue Wang,Wei Dang,Zhuoli Xu,Xinyuan Zhang,Bo Zhang,Kang Zhao,Yufei Tang
Polycarbosilane-derived (PCS-derived) coatings were fabricated on iron substrate by dip-coating method. The effects of curing process including air curing and divinylbenzene (DVB) curing and pyrolysis temperature on the coating microstructure, adhesion and corrosion resistance in 3.5 wt% NaCl solution were systematically studied. Both curing process and pyrolysis temperature have a significant influence on the micro-cracks, surface roughness and ceramicization of the coatings. PCS-derived coatings fabricated by air curing process has the lower micro-crack width due to the higher curing degree. No matter in which curing process, the average micro-crack width and surface roughness of the coatings pyrolyzed at 600 °C are higher than those of the coatings pyrolyzed at 400 °C or unpyrolyzed. Electrochemical test results indicate that all coatings can protect the iron substrate from corrosion. The corrosion resistance of the PCS-derived coating is dominated by the microstructure including micro-cracks, surface roughness and ceramicization. Coatings fabricated through air curing and pyrolyzed at 400 °C have better corrosion resistance due to less micro-cracks, lower roughness and higher ceramicization. Corrosion resistance mechanism of the PCS-derived coatings was also analyzed.
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危险品化学品经营许可证（带存储）