FUEL
·
2023
·
IF 7.4
Guang-Hui Liu,Yong-Chao Qi,Han Wang,Ai-Min Wang,Yu-Hong Kang,Yong Gao,Ni Bai,Zhan-Ku Li,Xian-Yong Wei
This paper focused on the complementary advantages of density functional theory (DFT) calculation and catalytic reaction regulation. Based on the effective identification of intermediates, the possible catalytic hydroconversion (CHC) pathways of lignite-derived aryl ethers over Ni/mordenite were discussed. Bond dissociation energy (BDE) calculations of >C–O– bonds in different substrates and intermediates show that BDEs of >C ar –O– bonds are generally higher than those of >C al –O– bonds, and there is obvious electron aggregation near O atoms. Mulliken charge distribution analyses of different atomic sites further revealed the possible adsorption sites of active hydrogen, especially H · and H + . Possible cleavage pathways were further speculated by evaluating the stability of different leaving groups. In the early stage of CHC, aromatic ring hydrogenation and >C al –O– bond cleavage dominate, rather than >C ar –O– bond cleavage. Enthalpy change analyses combined with the CHC of real substrates further indicate that lowering temperature is beneficial to the cleavage of >C ar –O– bonds under the premise of inhibiting H ··· H transfer and obtaining H · effectively. Appropriately increasing the support acidity to ensure sufficient H + release is conducive to >C al –O– bond cleavage, especially direct dehydroxylation/dehydration. The analysis of synergetic transfer pathways of active hydrogen during the CHC provides theoretical guidance for the pathway optimization of converting lignite into high-quality clean liquid fuels.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2018
·
IF 4.908
Qing-Qing Teng,Xian-Yong Wei,Yi-Bing Sun,Sheng-Kang Wang,Jing-Hui Lv,Zhan-Ku Li,Zhong-Qiu Liu,Zhi-Min Zong
Catalysts trifloromethanesulfonic acid (TFMSA)/treated attapulgite powder (TAP), Ni/TAP, and Ni-TFMSA/TAP with different Ni and TFMSA loadings were prepared. The typical catalysts were characterized with multiple instruments and used for catalyzing hydroconversion of di(1-naphthyl)methane (DNM), which was used as a coal-related model compound. The suitable loadings of Ni and TFMSA in Ni-TFMSA/TAP were determined to be 28.6% of Ni and 33% of TFMSA. Under optimal reaction conditions of 5 MPa of initial hydrogen pressure, 240 °C, and 4 h over Ni-TFMSA/TAP, DNM was completely converted, producing decalin and 1-methyldecalin as the main products. The result suggests that Ni-TFMSA/TAP is highly active for both cleaving the C ar -C alk bond in DNM and hydrogenating the resulting naphthalene and 1-methylnaphthalene under mild conditions. Based on the identification of reaction products, the catalytic mechanism for DNM hydroconversion was discussed.
研究领域:
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Guang-Hui Liu,Jin-Jun Bai,Kun-Lang Lu,Hui Kan,Xiao-Qi Zhang,Yu-Hong Kang,Cui-Ying Lu,Zhan-Ku Li,Hong-Cun Bai,Xian-Yong Wei
Two flexible regulation systems were designed and used for the integrated catalytic hydroconversion (CHC) of lignocellulose to valuable oxygenated organic chemicals. Under the dual constraints of initial H 2 pressure (IHP) and temperature, three crop stalks can be almost completely degraded over a hydrothermally stable Ru/La(OH) 3 in one-pot, while the synergetic transfer of active hydrogen effectively promotes the cleavage of >C-O- bridged bonds in organic matter with highly complex structures during this period. As a result, abundant >C al -O- (>32%) and >C=O (>24%) derived platform chemicals such as alkanols, cyclanols, carboxylic acids, and esters were obtained at high IHP and low temperature. Correspondingly, various >C ar -O- (>50%) and >C=O (>30%) derived platform chemicals such as phenols, alkoxy-substituted phenols, ketones, and carboxylic acids dominated the derived bio-oils at low IHP and high temperature. The designed selective CHC strategies have the characteristics of convergent conversion to the two major derivative chemical demand directions. Therefore, these two atom-economic and effective degradation approaches are conducive to obtaining abundant functional small molecules, which can be further converted to various downstream platform products.
研究领域:
化学工程
·
生物质能
·
催化科学
✓ 已验证
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Guang-Hui Liu,Wen-Ao Shi,Jun Li,Han Wang,Ai-Min Wang,Yu-Hong Kang,Yong Gao,Ni Bai,Jie Kang,Chen Shi,Xian-Yong Wei
To produce high-density liquid fuels from lignite, a novel Ni-based bifunctional MCM-41/ β composite zeolite (Ni@ M / β ) is reported for the catalytic hydroconversion (CHC) of lignite-derived aryl ethers to high-yield polycyclic alkanes (PCAs). Ni@ M / β has a three-dimensional channel-type hierarchical porous texture with β as the core and MCM-41 as the shell. Stable Brønsted/Lewis acid sites and abundant internal/inter-zeolite defects also effectively promote the CHC of aryl ethers to PCAs. Under optimal conditions (5 MPa initial H 2 pressure and 160 °C), selectivities of 2-(benzyloxy)naphthalene (BON) and benzyloxybenzene derived PCAs are as high as 76.0 and 90.5 %, respectively, with dimers and trimers dominating. DFT calculation based on electrostatic potential distribution on the van der Waals surface and Mulliken charge distribution of BON and derived oxygenated monomers shows that aromatic intermediates with >C aromatic OH have multiple accessible sites and are easy to bind with cation/radical fragments. Therefore, it is speculated that PCAs are mainly derived from C-C coupling induced by cation/radical fragments after the activation of aromatic α -carbon. In addition, the activation of H 2 to H + , H · , δ+ H ··· H δ- , and H ··· H is mainly attributed to the strong Ni- M / β interaction and abundant defects. The whole CHC process is triggered mainly by the adsorption of H + released by Ni@ M / β at O sites of aryl ethers, and >C aliphatic -O- bridged bond cleavage is dominant. During this period, benzyl cation/radical produced by >C-O- bond cleavage and aromatic α -carbon activation (mainly) is coupled/reformed with adjacent aromatic fragments into corresponding polymers with non-oxygen bridged bonds, which are more easily converted to PCAs. This polycrystalline composite strategy improves the accessibility of large-sized molecules to active centers, and then increases the yields of PCAs, which is attractive for the clean and efficient conversion of lignite-derived oils to high-density liquid fuels.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Fuxiang Feng,Xiaopo Niu,Li Wang,Xiangwen Zhang,Qingfa Wang
Ni/ZSM-5 nanosheet catalysts with different Si/Al ratios were modified by chemical liquid deposition (CLD) of tetraethoxysilane (TEOS) to tailor their acid spatial distribution. Their catalytic performance was evaluated with the hydroconversion of oleic acid to aviation-fuel-range-alkanes (AFRAs) at different reaction temperatures and H 2 pressures. The modified catalysts inherit the nanosheet structure with decreased external Brønsted acid concentration, especially the strong one. External Brønsted acid sites mainly favor the cracking of the deoxygenated products (C 17 /C 18 ). Internal Brønsted acid sites mainly enhance the isomerization of the linear AFRAs. And the catalytic activity of the external Brønsted acid sites was more sensitive to reaction temperature than that of the internal ones. The deoxygenation and cracking reactions were also more sensitive to H 2 pressure compared to the isomerization reaction. High AFRA selectivity of 51.4% as well as high iso/n -alkanes ratio of 1.7 were achieved at 250 °C and 10 bar over NS200(1).
研究领域:
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Zi-Fan Wu,Xian-Yong Wei,Wen-Long Mo,Yu-Hong Kang,Xiao-Qi Zhang,Xian-Kang Shan,Guang-Hui Liu,Xing Fan
TFMSA/ATA was prepared by impregnating trifluoromethanesulfonic acid (TFMSA) onto the acid-treated attapulgite (ATA). Yinggemajianfeng lignite was extracted ultrasonically with a mixed solvent obtain the extract and extraction residue (ER), and then ER was separated by density difference to obtain the light residue (LR). The non-catalytic hydroconversion (NCHC) and TFMSA/ATA-catalyzed hydroconversion of LR were investigated in cyclohexane at 160 °C under 4 MPa of initial hydrogen pressure for 12 h. The soluble portions from NCHC (SP NCHC ) and catalytic hydroconversion (SP CHC ) were analyzed with a Fourier transform infrared spectrometer and gas chromatograph/mass spectrometer. As a result, the yield of SP CHC (60.0%) is significantly higher than that of SP NCHC (1.8%), suggesting that the thermal dissolution of LR at 160 °C is negligible and TFMSA/ATA significantly catalyzed the hydrocracking of LR to release SP CHC . Oxygen-containing organic compounds, especially 4-methylpent-3-en-2-one and 4-hydroxy-4-methylpentan-2-one, are predominant produced from the CHC of LR, suggesting that the cleavage of > C α -O β - and > C β -O α - bonds in LR significantly proceeded during the CHC of LR over TFMSA/ATA. Such a mechanism was proved by the CHC of oxybis(methylene)dibenzene.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2025
·
IF 6.2
Wen-Ao Shi,Zhong-Hao Jiang,Ni Bai,Ai-Min Wang,Ai-Rong Mao,Zi-Long Zhao,Lin Lang,Jian Wei,Hai-Yan Liu,Qing-Qing Sun,Yong Gao,Yu-Hong Kang,Yan-Jun Li,Jin-Jun Bai
The separation of condensed aromatic compounds from coal tar residue (CTR), converted into cyclanes via catalytic hydroconversion (CHC) to produce essential blending components for coal-based jet fuel, represents a significant strategy for enhancing CTR's value. A highly efficient bifunctional catalyst was prepared by loading Ni nanoparticles (NNPs, ca . 10 %) on β /MCM-41 composite zeolite ( β / M) and denoted as Ni 10 % @ β / M . CTR was sequentially extracted with acetone/carbon disulfide, petroleum ether, and petroleum ether/methanol (5 vol% H 2 O) to obtain the soluble portion in methanol phase (PEEP M ). PEEP M mainly consists of phenols (64.8 %) and arenes (18.9 %). It was conducted to CHC over Ni 10 % @ β / M at 160 °C for 16 h under 5 MPa of an initial hydrogen pressure (IHP) to obtain CHPEEP M . The results indicate that the relative content of cyclanes in CHPEEP M reaches as high as 93.4 %. In Ni 10 % @ β / M , abundant defects, hierarchical porous composite zeolite with strong Lewis acid sites and uniformly dispersed NNPs play crucial roles in removing heteroatoms and hydrogenating aromatic rings (ARs), respectively. Benzyloxybenzene (BOB) is a model compound with a >C-O- bridge bond and ARs, used to study the catalytic activity of Ni 10 % @ β / M . BOB was completely converted into cyclanes at 160 °C for 2 h under 5 MPa IHP. The high yield of polycyclic alkanes is related to the coupling between the active fragments formed after >C-O- cleavage and the main structure. The synergistic transfer of H···H, δ+ H···H δ- , and H + generated by Ni 10 % @ β / M activation of H 2 is key to the hydrogenation of ARs via induced >C-O- bond cleavage, leading to the formation of saturated cyclanes.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2021
·
IF 6.186
Hao Xu,Xing Fan,Guo-Sheng Li,Yang-Yang Xu,Wen-Long Mo,Peter N. Kuznetsov,Feng-Yun Ma,Xian-Yong Wei
Co-Mo/γ-Al 2 O 3 bimetallic catalyst was prepared by incipient wetness impregnation and the physicochemical properties were obtained by a series of characterization methods. The active components are mainly MoS 2 and Co-Mo-S existing on γ-Al 2 O 3 , the support. Meanwhile, the activity of catalyst in hydroconversion of four coal-related model compounds (CRMCs), dibenzyl ether, furan, thiophene and quinoline, was investigated. Hydroconversion products were analyzed by gas chromatography/mass spectrometry (GC/MS) and the possible reaction pathways were proposed according to the GC/MS data. Oxygen was removed from dibenzyl ether via the direct cleavage of C alk -O bridge bond to produce benzylium cation followed by the combination with H − to generate toluene. The hydroconversion of furan can be realized by the direct cleavage of C ar -O bond and direct hydrogenation, respectively. For thiophene, H + directly transferred to sulfur atom, leading to the cleavage of C ar -S bond to produce H 2 S and 1,3-butadiene, which abstracted active hydrogen to yield butane. Another indirect desulfurization pathway for thiophene is hydrogenating to form tetrahydrothiophene and C–S bond cracking to produce butane. Hydroconversion of quinoline started with either N-ring or benzene ring , and the first one was the main pathway.
研究领域:
催化化学
·
煤炭化学
✓ 已验证
DOI
高影响因子
FUEL
·
2019
·
IF 5.128
Xue-Ke Li,Zhi-Min Zong,Yi-Feng Chen,Zheng Yang,Guang-Hui Liu,Fang-Jing Liu,Xian-Yong Wei,Bao-Jun Wang,Feng-Yun Ma,Jing-Mei Liu
A highly active difunctional Ni-Mg 2 Si/γ-Al 2 O 3 was prepared by thermally decomposing nickel tetracarbonyl onto γ-Al 2 O 3 impregnated with Mg 2 Si. The non-catalytic hydroconversion (NCHC) and catalytic hydroconversion (CHC) of the extract ( E ) and extraction residue (ER) from Yinggemajianfeng lignite were investigated over Ni-Mg 2 Si/γ-Al 2 O 3 at 240 °C in n -hexane. Benzyloxybenzene and oxybis(methylene)dibenzene were used as lignite-related model compounds to speculate the possible mechanisms for the catalytic hydrocracking and hydrogenation over Ni-Mg 2 Si/γ-Al 2 O 3 . As a result, more organic matter in ER was converted to soluble portion (SP) by the CHC than by the NCHC. The main SP from the CHC are chain alkanes and cyclanes, while that from the NCHC is rich in arenes and oxygen-containing organic compounds. The results indicate that Ni-Mg 2 Si/γ-Al 2 O 3 effectively catalyze the hydrocracking of >C alk –O– linkages and the hydrogenation of aromatic rings in E and ER.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2017
·
IF 4.601
Zhong-Qiu Liu,Xian-Yong Wei,Hai-Hong Wu,Wei-Tu Li,Yang-Yang Zhang,Zhi-Min Zong,Feng-Yun Ma,Jing-Mei Liu
Modified microfiber attapulgite (MFA)-supported nickel was prepared by thermally decomposing nickel tetracarbonyl on MFA modified with an acidic ionic liquid (AIL, 1-sulfobutyl-3-methylimidazolium trifluoromethanesulfonate). It was characterized with multiple instruments and used for catalyzing hydroconversion of lignite-related model compounds (LRMCs) oxydibenzene, benzyloxybenzene, and oxybis(methylene)dibenzene. The results indicate that Ni 15% /MFA@AIL effectively catalyzes hydroconversion of the LRMCs to afford cyclanes by inducing the formation of H + , H − , and biatomic active hydrogen.
研究领域:
催化化学
·
能源材料化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Ji Zhao,Xian-Yong Wei,Jing-Hui Lv,Qian-Qian Kong,Jia-Hao Li,Zhuang Li,Zi-Chun Fan,Li Li,Yang-Yang Zhang,Zhi-Min Zong
Ni/CeO 2 with medium-strong acidity was prepared by in - situ carbon templating (ISCT) and reduction with H 2 . Oxydibenzene (ODB) and benzyloxybenzene (BOB) were used as lignin-related model compounds (LRMCs). Over Ni/CeO 2 , ODB was completely converted into cyclohexane ( CH I ) under initial hydrogen pressure (IHP) of 2 MPa at 160 °C for 2 h and complete conversion of BOB to CH I and methylcyclohexane (MCH) was achieved under IHP of 2 MPa at 120 °C for 1.5 h. H … H transfer to the benzene rings (BRs) in the LRMCs and phenol from BOB hydrocracking results in the BR hydrogenation, while H + transfer to the oxygen atom in BOB, hydrogenated ODB, and BOB-derived cyclohexanol ( CH II ) leads to the >CH-O- bond cleavage and subsequent dehydration of the resulting protonated CH II (PCH II ) . In addition, Ni/CeO 2 exhibits an excellent reusability.
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
JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Ji Zhao,Xiang Bai,Xian-Yong Wei,Yierxiati Dilixiati,Jing-Hui Lv,Qian-Qian Kong,Zhuang Li,Zi-Chun Fan,Yong-Hui Feng,Zhi-Min Zong
The combination method of impregnation, desiccation, and subsequent reduction with H 2 was applied to prepare Ni x /CeO 2 . Each catalyst was characterized with multiple tools and its catalytic performance for the catalytic hydroconversion (CHC) of lignin-related model compounds (LRMCs) containing oxybis(methylene)dibenzene (OBMDB) and guaiacol was evaluated. Over Ni 14% /CeO 2 , OBMDB was completely converted into methylcyclohexane under initial hydrogen pressure (IHP) of 3 MPa at 200 °C for 2 h. The complete conversion of guaiacol to cyclohexanol ( CH II ) was realized under IHP of 4 MPa at 200 °C for 3 h. Additionally, H 2 can be activated to H⋯H, H + , and H − over Ni 14% /CeO 2 . H + is attracted by oxygen atom in OBMDB, leading to the cleavage of >CH 2 -O- bond to produce phenylmethanol (PM) and benzylium, which is subsequently comminated with H − to produce toluene. Next, H⋯H transfers to toluene and PM resulting in the hydrogenation of benzene rings (BRs) to produce methylcyclohexane and cyclohexylmethanol followed by the dehydration to form methylcyclohexane. BR in guaiacol was hydrogenated by H⋯H transfer to produce 2-methoxycyclohexan-1-one (MCH I ) and 2-methoxycyclohexan-1-ol (MCH II ) in sequence and subsequent demethoxylation of them to generate cyclohexanone ( CH I ) and CH II , respectively. Finally, H⋯H transfers to CH I to produce CH II .
研究领域:
化学工程
·
催化材料科学
✓ 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）