Journal of Materials Chemistry A
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2024
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IF 10.7
Hairui Jiao,Yushuai Sang,Hong Chen,Yongdan Li
Herein, an Ni9Fe1/NiAlOz catalyst is reported to be an efficient catalyst for conversion of enzymatic hydrolysis lignin (EHL) and 2-phenethyl phenyl ether (PPE), a lignin dimer model compound. Interspecies electron transfer within the alloy phase enhances the intrinsic hydrogenation activity of Ni, while Fe doping generates abundant interfacial oxygen vacancies (OVs). The combination of H* from high-intensity hydrogen spillover and abundant OVs promotes the depolymerization of EHL into cycloalkanes. Because of this combination, Ni9Fe1/NiAlOz achieves 99.4% of PPE conversion under mild reaction conditions (100 °C, 0.8 MPa H2, and 3 h) and achieves the yield of cycloalkanes (169.5 mg per g EHL at 300 °C) from EHL that exceeds the theoretical yield. The catalyst is also stable for 6 runs without much deactivation. This strategy provides new insights into the rational design of an efficient and stable transition metal catalyst using a simple preparation method for the valorization of EHL.
研究领域:
催化化学
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可再生资源转化
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DOI
高影响因子
FUEL
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2022
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IF 8.035
Mingxing Zhao,Jun Hu,Ping Lu,Shiliang Wu,Chao Liu,Yahui Sun
Efficient hydrodeoxygenation of lignin-derived bio-oils to cycloalkanes was achieved over bifunctional RuCoW x /NC catalyst prepared by in situ pyrolysis method. The performance of RuCoW x /NC was investigated in HDO of 4-propylguaiacol, considering the influences of catalysts, initial H 2 pressure, and reaction temperature. Catalyst screening reveals that RuCoW 0.03 /NC afforded the highest propylcyclohexane yield of 71.3% from 4-propylguaiacol at 220 ℃. At 240 ℃, the yield of propylcyclohexane increased to 95.2 %. The heavy fraction of rice husk bio-oil, primarily composed of lignin-derived phenolic compounds, could be upgraded to 98.3% hydrocarbons at 280 ℃ over RuCoW 0.03 /NC. The synergistic interaction between highly dispersed Co and Ru metal sites and WO x acidic sites is responsible for the excellent HDO activity of RuCoW 0.03 /NC. Besides, RuCoW 0.03 /NC exhibited high stability after four cycles.
研究领域:
化学工程
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能源科学
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高影响因子
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
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2010
·Vol. 24
·期 9
·1335-1342
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IF 2.695
Zhongyue Zhou,Lidong Zhang,Mingfeng Xie,Zhandong Wang,Dongna Chen,Fei Qi
Absolute photoionization and dissociative photoionization cross-sections of eleven n- alkanes ( n- pentane, n -hexane, n- heptane, n- nonane, n- decane, n -undecane, n- dodecane, n- tridecane, n- tetradecane, n- pentadecane and n- hexadecane), three cyclo -alkanes (cyclopentane, methylcyclohexane and trans -decahydronaphthalene) and iso -octane were measured for photon energies from the ionization thresholds to 11.5 eV. The measurements were performed with the binary-liquid-mixture method utilizing the photoionization cross-sections of benzene as a calibration standard. The ionization energies of n -alkanes and cyclo -alkanes were also calculated at the B3P86/6-31 + +G(d,p) level and by the G3B3 method. Copyright © 2010 John Wiley & Sons, Ltd.
研究领域:
化学
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物理化学
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Yiting Lei,Yulong Ma,Yonggang Sun,Liqiong Wang,Yingbo Zhu,Jinpeng Wei,Bolong Zhao,Li Zhu
Lignin, as a kind of biomacromolecule, plays a crucial role in the development of renewable energy sources. However, achieving excellent catalytic efficiency and selectivity towards expected products over a single catalytic system remains a significant challenge. The adjustment of acidic sites is an effective strategy to enhance hydrodeoxygenation (HDO) activity and product selectivity. This strategy facilitates charge transfer and activates substrate migration with the catalyst. Therefore, it is necessary to understand the relationship between the structure and activity of acid sites in catalysts, and construct synergistic Brønsted-Lewis sites. In this study, the incorporation of Ni@NC active phase derived from metal-organic frameworks (MOFs) significantly enhanced both the strength and quantity of Lewis acid sites (LASs) in the Ni@NC-HZSM-5 composite catalyst. This enhancement facilitated the cleavage of C Ar –OCH 3 bonds in lignin oil. Furthermore, the abundant Brønsted acid sites (BASs) present in HZSM-5 markedly promoted the cleavage of C Ar –OH bonds. Efficient conversion of real lignin oil was achieved through the synergistic action of the dual-acid sites, resulting in the conversion of 98.50 % and the C 6+ cycloalkane selectivity of 95.05 %. This study proposed a novel approach to the efficient upgrading of lignin-based bio-oil into alternative fuels using heterogeneous catalysts.
研究领域:
生物化学
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催化化学
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DOI
PubMed
高影响因子
Sustainable Energy & Fuels
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2022
·Vol. 6
·期 6
·1616-1624
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IF 6.813
Haofei Gao,Fengan Han,Guangyi Li,Aiqin Wang,Yu Cong,Zhizhou Li,Wei Wang,Ning Li
In this work, jet fuel range high-density polycycloalkanes, dicyclohexylmethane and dodecahydrofluorene, were first synthesized by a two-step method with vanillin and cyclohexanone, two platform compounds that can be derived from lignin. In the first step, 2-(4-hydroxy-3-methoxybenzylidene)cyclohexan-1-one, a jet fuel range C13 polycycloalkane precursor, was obtained through an acid-catalyzed aldol condensation reaction between vanillin and cyclohexanone over a series of titanium dioxide based nanometer material catalysts. Among them, sulfated titania nanofibers (STNFs) exhibited the highest activity. Over them, a high yield (81%) of 2-(4-hydroxy-3-methoxybenzylidene)cyclohexan-1-one was obtained after the reaction was carried out at 423 K for 10 h. On the basis of the characterization results, the good performance of the STNF catalyst can be attributed to its higher acid strength and higher Brønsted to Lewis acid site ratio. Subsequently, the aldol condensation product was further converted to a mixture of dicyclohexylmethane and dodecahydrofluorene by hydrodeoxygenation (HDO) under the co-catalysis of Pd/C and H-Y zeolite. According to our measurement, the cycloalkane mixture as obtained from the HDO process has a higher density (0.95 g mL−1) and lower freezing point (256 K). As a potential application, it can be blended into low freezing point jet fuels to improve their volumetric heat values.
研究领域:
化学工程
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能源科学
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高影响因子
RENEWABLE ENERGY
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2024
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IF 9
Cuicui Wu,Meng Wang,Yunming Fang
The productive motivation of high-energy-density fuels from sustainable feedstocks has been prompted by environmental concerns and resource scarcities. To address this demand, here, the energy-rich C10 cycloalkanes were first afforded with biomass-derived 2-cyclopentenone (2CPE). Initially, bio-based 2CPE can be converted to tricyclo-diketones by (2 + 2) cycloaddition under UV irradiation or zeolite catalysis. The UV-light photocatalysis for dimerization of 2CPE to diketol-cycloadducts disclosed outstanding advantages of cost-effectiveness and feasibility than traditional zeolite-catalyzed manner, with a yield of 53.61 % at ambient temperature for 2 h. Despite the potential for high dimer yield (77.28 %) under thermo-catalysis of H-ZSM-5 zeolite, the reaction conditions (120 °C, 18 h) were found to be suboptimal. Subsequently, diketol-cycloadducts were selectively and efficiently hydrodeoxygenated to provide cyclopentane-based hydrocarbons using a Huang-Minlon methodology with a yield of 97.04 %, where the target components were directly distilled during the reaction. Specifically, the as-synthesized C10 cycloalkane mixture originated from 2CPE possess high density of 0.96 g mL −1 , large volumetric heat net of combustion (NHOC) of 40.02 MJ L −1 , along with low freezing point of −49 °C. These properties suggest that the bio-liquid cycloalkanes can be used as a standalone high-energy fuel or as a blending agent to enhance the performance of conventional jet fuels.
研究领域:
生物化学
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能源科学
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产品关联
DOI
高影响因子
FUEL
·
2023
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IF 7.4
Zehao Han,Lun Pan,Kang Xue,Jisheng Xu,Qing Liu,Ying Xu,Zhouyang Shen,Xiangwen Zhang,Ji-Jun Zou
Polycyclic alkanes are not only the important components of high-density fuels, but also can be used to cool the overheating parts of hypersonic vehicle through catalytic endothermic dehydrogenation reaction. However, the dehydrogenation performances of cycloalkanes with different molecule structures vary widely. Herein, we investigated the effects of cycloalkane structures, including the length of branched chains, the number of branched chains, the number of rings, and the shape of rings, on the dehydrogenation performance. The results show that cyclohexane (CH) exhibits the best dehydrogenation performance (600 °C, 3 MPa) with >99% conversion, >99% benzene selectivity, and highest total heat sink of 4.47 MJ/kg. The branched chains, ring number and five-membered rings all have negative effects on dehydrogenation. Among them, the number of rings has the minimum negative impact. Moreover, we correlated the density, volumetric net heat of combustion (NHOC) and heat sink with the molecular structure of the cyclic alkanes and found that the polycyclic alkanes with low H/C ratio and high M have both high density, high volumetric NHOC and high heat sink. This work can provide guidance for development and design of advanced fuels for endothermic dehydrogenation.
研究领域:
化学工程
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燃料科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Taimei Cai,Qiang Deng,Hailong Peng,Jin Zhong,Jun Wang,Guiping Dai,Zheling Zeng,Ji-Jun Zou,Shuguang Deng
The synthesis of dibenzofurans and bicycloalkanes from biomass is important for sustainable high-value chemicals and high-density fuels. Currently, their biomass-based precursor is mainly derived from lignin with limited yields. Herein, we propose a cellulose-based synthesis route for dibenzofurans with a yield of 72.3% via the integration of oxidative coupling of 1,2,4-benzenetriol to diphenol combined with subsequent dehydration under environmentally friendly reaction conditions. After hydrodeoxygenation, bicycloalkanes are obtained with a yield of 70.5% by catalysis performed over Pd/C and various zeolites. This work provides a powerful cellulose-based strategy for the synthesis of dibenzofurans and bicycloalkanes, which was previously unattainable in the conventional lignin-based route.
研究领域:
化学工程
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可再生资源利用
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催化科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xing Zhang,Jingfeng Wu,Tian Li,Chengzhi Zhang,Lingjun Zhu,Shurong Wang
Hydrodeoxygenation (HDO) of lignin-derived bio-oil offers a promising route for the production of advanced biofuels. However, the conventional HDO of lignin-derived bio-oil faces serious problems, such as low hydrocarbon yield and easy deactivation of catalysts. Herein, a novel reaction system consisting of a highly stable bifunctional catalyst (i.e., Ni−WO x /NiAl 2 O 4 ) and a dodecane solvent was developed for the HDO of lignin-derived phenolics. The Ni 0 species, derived from NiWO 4 precursors on the NiAl 2 O 4 , were of small crystallite size and high dispersion, together with the strong oxophilicity of W, thereby exhibiting high activity. The use of a highly stable NiAl 2 O 4 spinel support and the replacement of common solid acid with more stable WO x for the cleavage of C O bond accounted for excellent stability. The optimized 10Ni−15WO x /NiAl 2 O 4 exhibited a high guaiacol conversion of 97.8% with a high cycloalkane yield of 83.8% under the optimum conditions (250 °C, 5 MPa H 2 , and 4 h). Cycloalkanes with a high yield over 90% were also obtained by the HDO of other complex lignin-derived compounds. More importantly, the catalyst always retained its initial activity for the HDO of guaiacol in five runs, with negligible coke formation. Subsequently, the HDO behavior of the bio-oil obtained from walnut shell pyrolysis was also studied. The relative content of cycloalkanes in the products reached 44.3% after the reaction. This study highlights the prospect of a highly stable catalyst consisting of hydrogenation metal and oxophilic promoter, and dodecane solvent to enable efficient production of cycloalkanes from the HDO of lignin-derived phenolics.
研究领域:
能源化学
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催化化学
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DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2018
·Vol. 92
·期 11
·2118-2123
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IF 0.549
Xu Zhigang,Junqiang Wang,Wei Zhao,Xiaoliang Li
Abstract New isobaric vapor-liquid equilibrium data for the binary mixtures of methylcyclopentane + 2‑methylthiophene, cyclohexane + 2-methylthiophene, methylcyclohexane + 2-methylthiophene and ethylcyclohexane + 2-methylthiophene systems were determined by a modified Rose-Williams equilibrium still under the pressure of 90.00 kPa. All the vapor-liquid equilibrium data measurements passed the thermodynamic consistent test by using the Herington method and the Van Ness test, respectively. No azeotropic behavior was observed in the tested four binary systems. Meanwhile, the experimental data were correlated by the Wilson activity coefficient model and also compared with the original UNIFAC and UNIFAC Dortmund predictive models. All results demonstrated that the original UNIFAC model gave better predictions than the UNIFAC Dortmund model.
研究领域:
化学工程
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热力学
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DOI
高影响因子
Advanced Sustainable Systems
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2020
·Vol. 4
·期 10
·1900136
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IF 4.869
Xing Zhang,Hui Yan,Lingjun Zhu,Tian Li,Shurong Wang
The monomers and dimers produced via lignin depolymerization are a promising alternative to transportation fuels after hydrodeoxygenation (HDO). However, these compounds contain numerous oxygen-containing functional groups that are strongly bonded to aromatic rings. Therefore, the conventional HDO of lignin-derived compounds faces serious problems of catalyst deactivation due to coke deposition and low hydrocarbon yields. A metal–solid super acid catalyst, i.e., Ru(SO 4 2− )/ZrO 2 –CeO 2 , is synthesized, characterized, and evaluated for the HDO of various lignin-derived monomers and dimers in a biphasic n -dodecane/H 2 O system. A high cyclohexane yield of 98.5% is obtained by the HDO of phenol performed at 200 °C and 5 MPa. The “hydrated” configuration can be formed between the hydrogenation intermediates and H 2 O on the Ru sites. In addition, the anionic vacancies of ZrO 2 –CeO 2 can be occupied by H − derived from the heterolytic cleavage of H 2 , leading to the formation of metal hydrides. The strong acidity of SO 4 2− /ZrO 2 –CeO 2 is beneficial for the subsequent deoxygenation of the hydrotreated products. In addition, the biphasic system can minimize the side reactions induced by the strong acidity of the catalyst. The catalytic system also exhibits a good catalytic performance for the HDO of other lignin-derived monomers and dimers to produce cycloalkanes.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Zhisong Cui,Yingchao Li,Xiaoyan Jing,Xiao Luan,Na Liu,Jinyan Liu,Yu Meng,Jian Xu,David L. Valentine
The consumption of cycloalkanes is prevalent in low-temperature marine environments, likely influenced by psychrophilic microorganisms. Despite their significance, the primary active species responsible for marine cycloalkane degradation remain largely unidentified due to cultivation challenges. In this study, we provide compelling evidence indicating that the uncultured genus C1-B045 of Gammaproteobacteria is a pivotal participant in cycloalkane decomposition within China’s marginal seas. Notably, the relative abundance of C1-B045 surged from 15.9% in the methylcyclohexane (MCH)-consuming starter culture to as high as 97.5% in MCH-utilizing extinction cultures following successive dilution-to-extinction and incubation cycles. We used stable isotope probing, Raman-activated gravity-driven encapsulation, and 16 S rRNA gene sequencing to link cycloalkane-metabolizing phenotype to genotype at the single-cell level. By annotating key enzymes (e.g., alkane monooxygenase, cyclohexanone monooxygenase, and 6-hexanolactone hydrolase) involved in MCH metabolism within C1-B045 's representative metagenome-assembled genome, we developed a putative MCH degradation pathway.
研究领域:
微生物学
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环境科学
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DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）