Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 4
·1156-1163
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IF 6.813
Guangzhi Ren,Guangyi Li,Ying Zhang,Aiqin Wang,Xiaodong Wang,Yu Cong,Tao Zhang,Ning Li
Jet fuel and diesel range C12 and C17 cycloalkanes were synthesized for the first time by a two-step process with 2-methylfuran and benzaldehyde, two platform compounds which can be derived from lignocellulose. In the first step, 5,5′-(phenylmethylene)bis(2-methylfuran) was obtained by the acid-catalyzed hydroxylalkylation/alkylation (HAA) of 2-methylfuran and benzaldehyde. Among the investigated commercial acidic resins, Nafion resin demonstrated the highest activity for the HAA of 2-methylfuran and benzaldehyde, which can be rationalized by the highest acid strength of Nafion resin. In the second step, the 5,5′-(phenylmethylene)bis(2-methylfuran) from the HAA reaction was further hydrodeoxygenated to jet fuel and diesel range C12 and C17 cycloalkanes. Among the investigated catalyst systems, the combination of H-ZSM-5 and Ru/hydroxyapatite (denoted as H-ZSM-5 + Ru/HAP) exhibited the best hydrodeoxygenation (HDO) performance. Over it, a high total carbon yield (87.3%) of jet fuel and diesel range C12 and C17 cycloalkanes was obtained under mild conditions (453 K and 4 MPa H2). According to our measurements, the mixture of C12 and C17 cycloalkanes obtained from the HDO process has high density (0.816 g mL−1) and low freezing point (240 K). Therefore, it can be blended into current bio-diesel and bio-jet fuel to increase their volumetric heat values. As another option, the C12 and C17 cycloalkanes can also be dehydrogenated to produce alkylbenzenes that can be used as feedstock in the production of surfactants.
研究领域:
生物化学工程
·
可再生能源化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Qiuxiang Yao,Lei He,Duo Ma,Yong Zhang,Dan Zhang,Ming Sun
The naphthalene derivatives in coal tar naphthalene and anthracene oil fractions mostly contain short-chain alkyl groups. The enrichment of PAHs (polycyclic aromatic hydrocarbons, mainly including naphthalene, anthracene, and pyrene) by the dealkylation of PAHs-rich fraction in coal tar was assumed to obtain high-purity PAHs by distillation. Based on this strategy, using 2-methylnaphthalene as the model compound, and the influences of catalysts with different supports (SiO 2 , Al 2 O 3 , ZSM-5, Beta, and HY) and different active metal components (Ni, Co, Mo, and W) prepared by the equivalent-volume impregnation method on the hydro-dealkylation performance of 2-methylnaphthalene under different technological conditions (temperature, H 2 initial pressure and reaction time) were systematically investigated in a pressurized batch reactor. The experimental results show that the conversion rate of 2-methylnaphthalene is 81.23 % and the selectivity of naphthalene is 64.22 % under conditions of 480 °C, 2 MPa, 4 h, and 6 W-HY. Loading 0.8 wt% La on the 6 W-HY catalyst can improve the dispersion of active metal component W on the support, but it does not change the skeleton structure of the support. In addition, one-dimensional diffusion is the most probable reaction mechanism for 2-methylnaphthalene, and the evolution profiles of naphthalene can be reflected by the reaction mechanism with a reaction order of n = 4 using the model fitting method.
研究领域:
化学工程
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催化
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石油化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Puxiang Yan,Haiyong Wang,Yuhe Liao,Chenguang Wang
Upgrading biomass to renewable diesel and jet fuels is essential to achieve carbon neutrality. Herein, diesel and jet fuels range alkanes were produced by HAA of 2-methylfuran and furfural over solid acid SO 4 2- /TiO 2 and subsequent HDO over Pd/NbOPO 4 . A series of SO 4 2- /TiO 2 catalysts were synthesized by wetness impregnation to produce C15 fuel precursors. S/Ti-450 with a calcination temperature of 450 °C exhibited the highest activity, affording 97.9 % yield of C15 fuel precursor. Sufficient Brønsted acid sites and moderate Brønsted acid strength are responsible for the super catalytic performance of S/Ti-450. Stability studies demonstrated that S/Ti-450 could be regenerated. Furthermore, the application of S/Ti-450 in the HAA reaction was extended to other carbonyl compounds (e.g., butanal, cyclohexanone and acetone) and high yields of desired fuel precursors were obtained. Finally, C15 fuel precursor was further converted to long-chain alkanes via HDO over Pd/NbOPO 4 , yielding 85.0 % diesel and jet fuels range alkanes.
研究领域:
化学工程
·
可再生能源
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Wei Wang,Shaoying Sun,Xing Zhang,Guangyi Li,Ling An,Chi Qian,Quan Liu,Xianzhao Shao,Xiaohui Ji,Ning Li
Carbon-based solid acid catalysts were prepared from polycarbonate waste by methanolysis, polymerization with polyformaldehyde, calcination, and sulfonation. These catalysts were very active in the hydroxyalkylation/alkylation (HAA) reactions between 2-methylfuran (2-MF) and furfural. Under mild reaction conditions, the PC-180 catalyst produced a good yield (79.1%) of the HAA product from furfural and 2-MF, equivalent to that of Nafion resin (81.1%). The remarkable efficiency of PC-180 can be comprehended by its high acid content and enhanced hydrophilicity, as determined through scanning electron microscopy, contact angle measurement, and infrared spectroscopy. Furthermore, this catalyst proved to be universal in the HAA reactions of 2-MF with different carbonyl compounds. After hydrodeoxygenation over the Ni/AlPO4-800 catalyst, these HAA products can be selectively transformed into jet fuel and diesel range branched alkanes.
研究领域:
化学工程
·
催化材料
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-15
·
IF 14.7
Liu Xixi,Huang Liang,Ma Yuandie,She Guoqiang,Zhou Peng,Zhu Liangfang,Zhang Zehui
A single-atom catalyst with generally regarded inert Zn–N 4 motifs derived from ZIF-8 is unexpectedly efficient for the activation of alcohols, enabling alcohol-mediated alkylation and transfer hydrogenation. C-alkylation of nitriles, ketones, alcohols, N -heterocycles, amides, keto acids, and esters, and N -alkylation of amines and amides all go smoothly with the developed method. Taking the α-alkylation of nitriles with alcohols as an example, the α-alkylation starts from the (1) nitrogen-doped carbon support catalyzed dehydrogenation of alcohols into aldehydes, which further condensed with nitriles to give vinyl nitriles, followed by (2) transfer hydrogenation of C=C bonds in vinyl nitriles on Zn–N 4 sites. The experimental results and DFT calculations reveal that the Lewis acidic Zn-N 4 sites promote step (2) by activating the alcohols. This is the first example of highly efficient single-atom catalysts for various organic transformations with biomass-derived alcohols as the alkylating reagents and hydrogen donors.
研究领域:
催化
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有机化学
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材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 20
·12932-12937
·
IF 4.036
Shaoying Sun,Xing Zhang,Yanqing Li,Xianzhao Shao,Jianwei Ji,Junhai Liu,Wei Wang,Zhizhou Li,Xiaohui Ji
New solid acid catalysts were prepared by bisphenol A, paraformaldehyde and chlorosulfonic acid, and applied to hydroxylalkylation/alkylation (HAA) of 2-methylfuran (2-MF) and cyclohexanone. After optimizing the reaction conditions, the conversion of 2-MF reached 99% and the yield of 5,5′-(cyclohexane-1,1-diyl)bis(2-methylfuran) acquired 98%. The activity and catalytic efficiency were higher than those of Amberlyst 15 and Amberlyst 36 resins, which could be rationalized by high acid strength. At the same time, the catalysts were characterized by acid–base titration and FTIR. Hydrodeoxygenation (HDO) of HAA products of 2-methylfuran and cyclopentanone were processed on the Ni/SiO2 catalyst prepared by wet impregnation method to further convert into aviation kerosene, and the yield reached 93%.
研究领域:
化学工程
·
催化
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Yangyang Xin,Yufeng Hu,Mengchen Li,Kebin Chi,Shang Zhang,Fei Gao,Siqi Jiang,Yichuan Wang,Chunxiao Ren,Guohua Li
Alkylation catalyzed by concentrated sulfuric acid (H2SO4) is an important process for industrial production of excellent high octane gasoline blending components. This process has some vital drawbacks such as extensive side reactions and high consumption of H2SO4 due to the presence of the most notorious impurities including H2O, acid soluble oil (ASO), and esters. In this study, isobutane alkylation was studied with H2SO4 (275 mL) in a batch reactor at −10 to 0 °C and 0.45 MPa, with the corresponding stirrer speed, feed rate, acid/hydrocarbon volume ratio, and isobutane/isobutylene volume ratio being 3000 rpm, 5.0 mL/min, 1.2, and 14.3, respectively. The effects of the acid strength and composition of acid on the alkylate quality were investigated. The composition of used acid was analyzed. The results show that used acid is mainly composed of roughly 89% free H2SO4, 6% H2O, 2% esters, and 3% ASO. The compounds existing in the ASO extracted from used acid were identified, and their concentrations were quantitatively determined. The results show that the most abundant ASO molecules are five-membered or six-membered cyclic homoannular conjugated olefins such as cyclopentadiene (15.67%) and cyclohexadiene (14.12%). The effects of acid strength, H2O, ASO, and esters on alkylation depend strongly on the concentrations of H2SO4 and these impurities. Therefore, their optimal concentrations were determined to achieve advantageous effects on the alkylation. The results are about 93–95% for H2SO4, 2–4% for H2O, 1.5–2.5% for ASO, and 0.4–1% for esters, beyond which an adverse effect will appear. Under the optimal concentrations, the value of the research octane number, the trimethylpentane (TMP)/dimethylhexane ratio, and the contents of C8 and TMP remained steady at high levels of about 92–93, 5.8–6.3, 68–70, and 58–60%, respectively.
研究领域:
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2019
·
IF 4.745
Shaofeng Wu,Jianyu Dong,Dan Zhou,Wan Wang,Long Liu,Yongbo Zhou
A H3PO3-catalyzed alkylation of phenols with alkenes is achieved in a facile, efficient, and selective manner. The reaction shows a unique selectivity, i.e., excellent regioselectivity, thorough suppression of overalkylation, without alkylation of a simple phenyl ring, and can selectively provide ortho-, meta-, or para-alkylated phenol derivatives in good to excellent yields. This feature along with mild reaction conditions, sensitive functional group tolerance, and scale-up synthesis and late modification of phenolic bioactive compounds make it an ideal and practical alternative for the modification of phenols.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2016
·
IF 2.75
Genkuo Nie,Xiangwen Zhang,Peijuan Han,Junjian Xie,Lun Pan,Li Wang,Ji-Jun Zou
Biofuels are important alternative for fossil-based fuel but they have either relatively low density or high freezing point and viscosity. Here we reported a simple and efficient route to synthesis biofuel with density comparable to widely used JP-10 fuel as well as good low-temperature properties. Substituted diphenyl methane was synthesized by acid catalytic alkylation of lignin-derived phenols (phenol, anisole, guaiacol) with benzyl ether or benzyl alcohols, and MMT-K10 exhibits better activity than HPW, Amberlyst-15, and Al-MCM-41, due to the modest acid strength and open lamellar structure. High selectivity along with good-to-excellent conversion was obtained under optimized conditions regardless of different reactant used. Then the alkylated product was subjected to hydrogenation with the presence of Pd/C and HZSM-5, and interestingly, intramolecular cyclization reaction occurred to produce a large amount of perhydrofluorene as well as dicyclohexylmethane. Subsequently, biofuel with density as high as 0.93 g/mL and freezing point as low as −40.0 °C was obtained, which surpasses the state-of-art of biofuel reported.
研究领域:
化学工程
·
能源科学
·
生物化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 77
·63044-63049
·
IF 3.84
Hualei Hu,Jinghui Lyu,Jie Cen,Qunfeng Zhang,Qingtao Wang,Wenwen Han,Jiayao Rui,Xiaonian Li
The effect of MgO and Pd modification on the catalytic performance of hierarchical porous ZSM-5 for benzene alkylation with methanol was investigated. The results indicated that the introduction of MgO could reduce the Brönsted acid sites which suppressed the side reaction of methanol to olefins and in turn effectively promoted the alkylation of benzene. However, the single modification of MgO could not completely suppress the formation of ethylbenzene and coke. Doping a small amount of Pd had a positive effect on inhibiting the generation of ethylbenzene and coke, which could be attributed to the hydrogenation of ethylene into ethane on Pd. The dual modified catalyst (MgO and Pd) exhibited high benzene conversion (56%) and xylene selectivity (39.1%), and the lowest ethylbenzene selectivity (0.13%) and coke content (0.4 wt%).
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Yangyang Xin,Yufeng Hu,Yichuan Wang,Siqi Jiang,Mengchen Li,Kebin Chi,Shang Zhang,Fei Gao,Chunxiao Ren,Shuai Zhang,Chenglong Ma
For alkylation catalyzed by H 2 SO 4 , the promotion of solubility of isobutane in H 2 SO 4 is of major importance to the enhancement of quality of alkylates. ASO (acid-soluble oils or conjunct polymers or red oil) are the potential co-catalyst to improve the solubility of isobutane and to optimize the interfacial characteristics of acid/hydrocarbon dispersions. On the basis of the calculation results of COSMO-RS method, we found that the solubility of isobutane in H 2 SO 4 was obviously increased upon the addition of most ASO molecules. Moreover, a better dissolution of isobutane in H 2 SO 4 can be achieved by adding the hydrocarbons like paraffins and cycloparaffins into H 2 SO 4 . On the basis of these findings, two cycloparaffins were selected and used as the co-catalyst (the co-catalysts A and B) to improve the performance of the H 2 SO 4 catalyst. The alkylation results showed that these cycloparaffins enhanced the quality of alkylates. In particular, upon the addition of the co-catalyst B, the RON (research octane number) value, the TMP/DMH (trimethylpentane/dimethylhexane) ratio, and the contents of C8 and TMP (trimethylpentane) were increased significantly from 92.67 and 6.51, 68.25% and 59.10% to 94.38 and 6.97, 74.81% and 65.34%, and the consumption of the H 2 SO 4 catalyst was reduced by 38%.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
PROGRESS IN ORGANIC COATINGS
·
2022
·
IF 6.206
Haihua Wang,Guangyu Hu,Xuan Liu,Liyuan Guo,Xiaorui Li,Ruiyuan Guo,Yanyu Li
The uniform dispersion and long-term stability of hydrophobic polyaniline (PANI) in waterborne polymer matrix always remains a challenge. Here, PANI was chemically modified by 1,12-dibromododecane to prepare functionalized PANI (PANI-12Br(II)), and simultaneously achieve N-alkylation and chemical crosslinking of PANI chains. In addition, 1-bromododecane was utilized to modify PANI to prepare PANI-12Br(I) as a control. The degree of alkylation of PANI-12Br(II) was higher than that of PANI-12Br(I), as well as the content of N + species in PANI-12Br(II). Also, the interaction between the PANI-12Br(II) chains decreased. The colloidal particle size decreased from 703.9 nm to 297.3 nm, and the dispersibility and long-term colloidal stability of PANI-12Br(II) in aqueous system were significantly improved. The water adsorption of as-prepared PANI-12Br(II)/WAR nanocomposite decreased from 18.37% to 4.27%, and the contact angle increased from 63.4° to 112.5°. Compared with WAR and PANI/WAR-0.5%, the coating resistance of PANI-12Br(II)/WAR-0.5% increased by 5 and 4 orders of magnitude, and the corrosion current density decreased by 3 and 2 orders of magnitude. The PANI-12Br(II)/WAR-0.5% displayed better long-term anticorrosive performance than PANI-12Br(I)/WAR-0.5%. The anticorrosive mechanisms were also put forward. The PANI-12Br(II) can be applied as a promising class of corrosion inhibitors in waterborne polymer matrices.
研究领域:
材料科学
·
腐蚀与防护
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）