CARBON
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2022
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IF 11.307
Shuhan Chen,Wei Lu,Ru Xu,Ji Tan,Xuanyong Liu
Metal-nitrogen-doped carbon single-atom nanozymes (M − NC SAzymes) have tremendous prospects to replace natural enzymes for the treatment of reactive oxygen species (ROS)-related diseases. However, developing a pyrolysis-free and universal synthesis of M − NC SAzymes with robust enzyme-mimicking activity still remains a challenge. Herein, a promising cytoprotective agent (Fe-NC SAzymes) with multiple enzyme-mimicking activities was fabricated based on the reaction of Schiff bases with Fe ions via one-pot solvothermal method. In Fe-NC SAzymes, Fe-N x moieties served as the main catalytic sites to mimick oxidase, peroxidase, and catalase; meanwhile, the co-catalytic sites of the π-conjugated nitrogen-doped carbon structure mimicked superoxide dismutase to achieve the multiple enzyme-mimicking catalysis. Owing to the dual catalytic sites and pyrolysis-free synthesis strategy, Fe-NC SAzymes showed enhanced catalytic performance and excellent biocompatibility, which could scavenge excessive intracellular ROS to alleviate oxidative stress. The viability of cells subjected to oxidative stress recovered from 1.4% to 80.3% after Fe-NC SAzymes treatment, demonstrating an outstanding cytoprotective performance. Remarkably, this synthetic strategy can be expanded to other metal-NC SAzymes (Cu, Mn, Co, Zn, and Ni), which provides a feasible route to design specific functional SAzymes for ROS-related diseases therapy.
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Chuan Peng,Jin Song,Surong Bai,Jinjin Wan,Jin Huang,Junfeng Zhang
ZT@HZ-X core-shell catalysts were synthesized from lithium mine tailings. • Tuning the Si/Al ratio optimizes hierarchical pores and strong acid sites. • ZT@HZ-30 yielded 43.0% monocyclic aromatics with full furan conversion. • Dense acid sites drive cascade furan cycloaddition and lignin demethoxylation. • Synergistic cascade catalysis for efficient biomass pyrolysis vapor upgrading. Catalytic fast pyrolysis (CFP) is a promising route for converting biomass into chemical products, but its industrial application is limited by the high oxygen content of primary pyrolysis vapors and rapid catalyst deactivation. Here, we report a hierarchical core-shell catalyst, ZT@HZ-X, comprising a lithium mine tailings-zirconia composite core uniformly encapsulated by an HZSM-5 zeolite shell with tuneable Si/Al ratios. The catalytic performance was evaluated by pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) during rapeseed straw pyrolysis. The high density of strong acid sites within the microporous shell, combined with a hierarchical mesoporous network, promotes a cascade catalytic mechanism: for holocellulose-derived intermediates, the acidic microenvironment destabilises primary furanic compounds, facilitating possible Diels-Alder-type cycloaddition pathways that contribute to increase the relative peak area of monocyclic aromatic hydrocarbons. Concurrently, in the lignin depolymerisation pathway, the acidic sites selectively cleave ether bonds, driving demethoxylation and demethylation that convert complex syringyl and guaiacyl phenols into simpler p -hydroxyphenyl species. This core-shell catalytic system enables deep deoxygenation and aromatic enrichment of the bio-oil whilst providing a sustainable strategy for valorising lithium mine tailings. Download: Download high-res image (424KB) Download: Download full-size image
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2023
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IF 6
Ke Wang,Junyu Pan,Yi Gao,Gang Wu,Guiying Lin,Kuan Ding,Xun Hu,Shu Zhang,Yong Huang
Levoglucosan (LG), a valuable chemical derived from carbohydrates, is challenging to obtain with high yield directly from raw biomass. In this study, pyrolysis of a lignocellulosic biomass to LG was studied with various pretreatment methods, including acid, alkali, and torrefaction pretreatments. The results indicated that the hydrochloric acid washing effectively promoted the production of LG when the concentration of HCl was lower than 0.5 mol/L, mainly caused by the improved crystallinity of the cellulose fraction and the removal of alkali and alkaline earth metals (AAEMs). When 4% of NaOH solution was employed for the alkali pretreatment, the relative content of LG significantly increased from 3.07 to 73.59 with the temperature ranging from 130 to 170 ℃, owing to the effective removal of lignin and hemicellulose fractions. Biomass torrefaction at temperature lower than 250 ℃ slightly promoted LG production, but it inhibited the formation of LG when the temperature reached 300 ℃.
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JOURNAL OF SEPARATION SCIENCE
·
2023
·
IF 3.1
Huijun Liu,Baoquan Pan,Jingkun Zhang,Zhongping Huang,Pingping Li,Jian Shen
A method for the determination of five microplastics in agricultural soil was established by double-shot pyrolysis-gas chromatography combined with two-step extraction. First, polycarbonate (PC), polystyrene (PS), polypropylene (PP), and polyethylene (PE) were extracted from soil samples using a mixed solvent of cyclohexanone and p -xylene, and then PE terephthalate was extracted with m -methylphenol. Subsequently, PC and PE terephthalate were analyzed by thermochemolysis, and PE, PP, and PS were investigated by direct pyrolysis at 600°C. The linearity of the method was satisfactory for five microplastics and the correlation coefficients were higher than 0.97 in the respective concentration range. The limits of detection and the limits of quantification were 0.2–10.0 and 0.5–20.0 μg/g, respectively. The method provided recoveries of 75.1%–141.5%, with acceptable repeatability within 20.0%. It was a supplementary method for the existing characterization of microplastics in agricultural soil.
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PubMed
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
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IF 6
Yuxin Yan,Chen Wang,Qingya Liu,Zhenyu Liu
Polyethylene mulch films (PEMFs) are widely used in agriculture to boost crop yields but pose significant environmental challenges due to their non-degradable nature. This study investigated the pyrolysis of PEMFs in nitric acid (HNO 3 ) using micro-glass reactors under mild conditions for the production of thermochemical degradation products (TDP) as potential organic fertilizer precursors. The effects of HNO 3 concentration (10–60 %), HNO 3 :PEMF ratio (0.5–2), pyrolysis temperature (150–250 °C), and reaction time (1 – 45 min) on the yield of TDP, tetrahydrofuran-soluble fraction (THF-S), tetrahydrofuran-insoluble fraction (THF-IS), and HNO 3 consumption were studied. SEM, elemental analysis , GPC, and FTIR were employed to assess product characteristics and degradability potential. Optimal conditions were HNO 3 concentration of 36 %, HNO 3 :PEMF ratio of 0.5, pyrolysis temperature of 200 °C, and reaction time of 10 min. Higher temperatures or longer time would lead to TDP condensation to carbonaceous residues. The introduction of N and O-containing functional groups in TDP suggested its potential as an organic soil fertilizer. This study presents a novel, eco-friendly, and cost-effective solution to address the waste PEMF disposal problem.
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International Journal of Coal Preparation and Utilization
·
2023
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IF 2.1
Xuexia Wang,Wencheng Xia,Yaoli Peng,Guangyuan Xie
Iron-assisted pyrolysis (Fe-assisted pyrolysis) is a high-efficiency technique to remove sulfur from low-rank coal. However, the sulfur removal mechanism of Fe-assisted pyrolysis did not compressively address. For filling this gap, this study explored the sulfur removal mechanism of diphenyl sulfone during Fe-assisted pyrolysis based on the factor optimization of desulfurization performance. The iron powder under the optimal conditions of Fe-assisted pyrolysis was characterized with X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS), showing that FeS and some FeS2 were formed on the surface of post-pyrolysis iron powder. Gas chromatography (GC) analysis manifested that the addition of iron powder in the pyrolysis process could considerably reduce the SO2 emission. GC and Fourier transform infrared spectrometer (FTIR) analyses demonstrated that there was C–S bond broken in the diphenyl sulfone structure during Fe-assisted pyrolysis. From the results of thermogravimetry-mass spectrometry (TG-MS), the addition of iron powder in the pyrolysis process could enhance the reaction rate and reduce the temperature required for the reaction. We believe that the results of the present study provided a theoretical basis for a profound understanding of the desulfurization mechanism of Fe-assisted pyrolysis.
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POLYMER DEGRADATION AND STABILITY
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2023
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IF 5.9
Yukun Zeng,Erwei Leng,Yuan Xue,Xun Gong,Jingchun Huang,Jiaqiang E
With the rapid growth of wind power, batteries, and aerospace industries, sustainable disposal of thermoset plastics has become a long-term concern. However, pyrolysis, a highly promising solution for this issue, has seen limited studied on thermoset plastics. Drawing inspiration from the synergistic interactions observed between thermoplastics and biomass, this study explored the co-pyrolysis of a thermoset epoxy resin, diglycidyl ether of bisphenol A, cured with 4,4′-Diaminodiphenylmethane, with ash-free biomass pseudo-components (cellulose, lignin, and xylan) using thermogravimetry and Py-GC/MS. The results revealed distinctive synergistic effects in Epoxy-Cellulose and Epoxy-Lignin mixtures, delaying the onset and hastening the conclusion of weight loss. This was accompanied by increased activation energies, assessed through the Friedman and Kissinger-Akahira-Sunose methods, as well as higher char yields. Conversely, in Epoxy-Xylan, synergistic effects led to reduced activation energy across most α values, resulting in a lower onset temperature and a heightened maximum rate of mixture degradation. Regarding product distribution, all three pseudo-components, particularly lignin, enhanced the selectivity of bisphenol A. Additionally, cellulose and xylan altered the kinetics of N–C and C(N)–C(OH) bond cleavage, reducing the amount and altering the distribution of 2-B-N compounds (compounds featuring two benzene rings and nitrogen). Conversely, the presence of resin reduced the volatiles from cellulose and xylan, promoting phenol-type products and –H and alkylene side chains while diminishing guaiacol-type products and alkyl side chains. Three mechanisms were proposed to elucidate these observed synergistic effects: catalytic effects of –OH groups from biomass pseudo-components, hydrogen exchange or hydrogen bonding between resin-derived nitrogen and biomass-derived oxygen-containing functional groups, and radical reactions. These insights into the co-pyrolysis of biomass and cured epoxy resin can inform the selection of suitable feedstocks for various applications.
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Aerospace
·
2023
·Vol. 10
·期 9
·800
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IF 2.6
Hongsheng Yu,Xiaodong Yu,Hongwei Gao,Luigi T. DeLuca,Wei Zhang,Ruiqi Shen
The slow regression rate induced by the high pyrolysis difficulty has limited the application and development of hydroxyl-terminated polybutadiene (HTPB)-based fuels in hybrid rocket propulsion. Nickel oxide (NiO) shows the possibility of increasing the regression rate of HTPB-based fuels by catalyzing the pyrolysis process of the polymer matrix in our previous investigation; hence, this paper studies the NiO particles in the thermal decomposition and combustion of HTPB fuel grains. The DSC/TG test shows that NiO can intensely decrease the thermal stability of HTPB, and the catalytic effect of NiO is mainly reflected in the final decomposition stages of polybutadiene components. 5 wt% NiO enhances the regression rate by 19.4% and 13.7% under an oxygen mass flux of 50 kg/m2s and 150 kg/m2s, respectively. Further investigation shows that NiO particles will also cause the reduction of combustion heat and the agglomeration at the regressing surface while catalyzing the pyrolysis process, improving the thermal conductivity, and promoting the radiative heat transfer of the HTPB-based fuels; thus, more NiO additive (5 wt% < [NiO] ≤ 10 wt%) does not lead to a faster regression rate in HTPB-based fuels. This study demonstrates the catalytic effect of NiO on the polymer matrix for HTPB-based fuels, showing the attractive application prospects of this additive in HTPB-containing fuel grains.Keywords:hybrid rocket propulsion;HTPB;combustion characteristics;regression rate;catalytic pyrolysis;nickel oxide
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CERAMICS INTERNATIONAL
·
2023
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IF 5.2
Xiao Lin,Zhongyu Long,Long Jiang,Zhiyuan Liu,Changyong Liu,Zhangwei Chen
High-performance SiOC(Fe) wave-absorbing ceramics, containing a large number of carbon nanowires, were successfully prepared using a combination of photopolymerization 3D printing technology and the polymer-derived ceramic pyrolysis method. By employing an optimized segmented slow heating scheme with extended holding time, the pyrolysis of SiOC(Fe) ceramics at 1000 °C facilitated the growth of carbon nanowires, Fe 3 C and SiO 2 grains. These carbon nanowires were interlaced and interconnected within the samples, forming abundant conductive networks. This highly conducive network efficiently converted electromagnetic energy into thermal energy, effectively dissipating electromagnetic waves, and consequently enhancing the microwave absorption performance of ceramics. Moreover, this approach not only reduced ceramic cracks but also improved the dielectric loss performance of the materials, achieving a minimum reflectivity value of −35.72 dB. The SiOC(Fe) ceramics added with 5 wt% VcFe effectively enhanced the magnetic loss of the material, reduced the difference between the relative complex permeability (μ r ) and the relative complex dielectric constant (ε r ), and improved the impedance matching between the material surface and air, thereby further improving its microwave absorption performance. This resulted in an increase in the maximum effective absorption bandwidth of the material to 12.7 GHz at 5 mm. This study offers a promising solution for the preparation of ceramic matrix composite materials incorporating carbon nanowires, magnetic particles and ceramic precursors, which would be potentially valuable for radar detection and sensor applications .
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ACS Catalysis
·
2023
·
IF 12.9
Peiqi Liu,Wanyun Shao,Zhen Yang,Jiuzhong Yang,Liangyuan Jia,Yang Pan,Zhongyue Zhou,Yingquan Chen,Fei Qi
Reactive intermediates are essential for determining the reaction mechanism of biomass pyrolysis. However, these short-life compounds are rarely reported because they are difficult to probe and identify. Here, the catalytic pyrolysis of furanic compounds over HZSM-5 was investigated by combining a low-pressure reactor and an in situ synchrotron vacuum ultraviolet photoionization molecular beam mass spectrometer (SVUV-PI-MBMS). Important reactive intermediates (m/z < 200) can be detected and characterized by this in situ analysis method, which also allows studying the dynamics of volatile formation as a function of catalyst deactivation. Strikingly, formaldehyde and acetaldehyde as reactive intermediates in the upgrading of 5-methylfurfural (5-MFF) are mainly produced from its side-chain cracking on the external surface of the zeolite, while their conversion is highly related to the contribution of the Brønsted acid site inside the zeolite. It is also evidenced that reactive methylcyclopenadienes (MCPDs) are formed from various compounds (alkynes, furans and olefins) and can be further converted to methylbenzenes (MBs) via ring-expansion. Finally, more complete conversion pathways that contain reactive intermediates for zeolite-catalyzed pyrolysis of furanic compounds are proposed. The key roles of some reactive intermediates in promoting the deoxidation and aromatization of furans are also illustrated.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hao Zhou,Yongheng Shi,Lingmei Dai,Dehua Liu,Wei Du
Pyrolyzing ZIF-8 into N-doped carbon is now inspiring new potential of ZIF-8 for extensive applications. However, the exploration of such ZIF-8-derived carbon for biotechnological applications has been rarely investigated, especially in this context that imidazole derivatives are of rich functionality in life science. Herein, we reported a facile temperature-dependent pyrolysis method to achieve the effective N-doping in ZIF-8-derived macroporous carbon, which was systematically investigated for the immobilization of lipase from Thermomyces lanuginosus (TLL) in biodiesel production. MNC-600 (macroporous N-doped carbon derived at 600 °C) exhibited the best immobilization performance, with the highest specific activity of 190.6 U mg −1 , a 36.9% increase than free TLL. Moreover, MNC-600@TLL showed superior effectiveness and robustness in biodiesel production. A much faster rate of conversion and the highest biodiesel yield of 87.4% were observed. After eight successive batches of recycling, MNC-600@TLL retained 93.4% of its initial activity. XPS analysis revealed the evolution of N species during the pyrolysis of ZIF-8. It was proposed that the abundant doping of pyrrolic N species played a major role in the surprising performance of MNC-600, mainly through hydrogen bonding interactions, which simultaneously realized the activation of reactants as well as the in-situ hydrophobization of biocatalyst. This report is anticipated to pave a way for the exploration of ZIF-8-derived N-doped carbon for extensive biotechnological applications.
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BIORESOURCE TECHNOLOGY
·
2023
·
IF 11.4
Zijing Guo,Xin Chen,Jiacheng Hang,Zhengzhang Li,Caihua Zhong,Ahui Sun,Jihui Li,Shuying Xu
A novel oxidative magnetization, involving phosphomolybdic acid and Fe(NO 3 ) 3 co-promoted pyrolysis, was established to manufacture highly adsorptive magnetic biochars for adsorbing aqueous tetracycline, methylene blue, and Cr 6+ . The modification of phosphomolybdic acid greatly boosted the formation of γ-Fe 2 O 3 and oxygen containing groups with enhancement of specific surface area and pore volume at 400 °C. Importantly, γ-Fe 2 O 3 was stably fixed on surface in quasi-nanoscale. The oxidized magnetic biochar displayed 631.53, 158.45, 155.13 mg/g adsorption capabilities for tetracycline, methylene blue, and Cr 6+ with 22.79 emu/g saturation magnetization, respectively. Oxygen containing groups and quasi-nanoscale γ-Fe 2 O 3 served as key adsorption sites for these pollutants. A general oxidative magnetization was established for manufacturing high-performance magnetic biochar through phosphomolybdic acid/Fe(NO 3 ) 3 co-promoted pyrolysis at relatively low temperature.
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