INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Qian Zhang,Wenjun Liu,Shan Jiang,Minjun Kuang,Jiajin Li,Songbai Qiu,Xiaoping Wu
Motivated by the carbon neutrality policy and the demand for value-added bio-based chemicals, it is of great significance and interest to directly upgrade aqueous ethanol to produce long-chain alcohol chemicals and transportation biofuel. In this study, a bimetallic catalyst composed of Re doped Ni@C was prepared by a facile sol–gel method. The bimetal 70-NiRe@C demonstrated higher selectivity toward target long-chain alcohols product and lower selectivity of C1 byproducts than the monomeric metal Ni@C. The addition of Re promotes the dispersion of active Ni on the graphite carrier, contributing to the superior 59.9% ethanol conversion and 45.0% long-chain alcohol yield. This work guides future research into the direct upgrading of water-based bioethanol to the value-added long-chain fine chemicals and biofuels required.
研究领域:
化学工程
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催化科学
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可再生资源转化
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yang Peng,Zhanwei Xu,Le Yu,Xucheng Li,Weiran Yang
The direct conversion of furfural (FUR) to 2-methyltetrahydrofuran (2-MTHF) was investigated over a trimetallic CuNiRe/Hβ catalyst. Under optimal reaction conditions at 240 °C under 3 MPa H 2 for 1 h, almost complete conversion of FUR and high-yield of 2-MTHF (81 %) was achieved. This is the highest yield reported for the direct conversion of FUR to 2-MTHF. HR-TEM demonstrated that the growth of Cu nanoparticles (NPs) on the surface of Hβ was inhibited after loading Ni or Re resulted in the smaller Cu particle size and better hydrogenation and hydrodeoxygenation activity. H 2 -TPR characterization exhibited that the reducibility of bimetallic and trimetallic catalysts was higher than that of monometallic catalysts·NH 3 -TPD explained that Hβ acid sites mainly contributed to FUR deoxygenation. The adsorption configurations of FUR, furfuryl alcohol (FOL) and 2-methylfuran (2-MF) on the catalyst were revealed by ATR-IR. Catalyst evaluation and control experiments proved that FUR was first hydrogenated to FOL, followed by hydrodeoxygenation to 2-MF, and finally hydrogenated to 2-MTHF catalyzed by the combination of three metals.
研究领域:
催化化学
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可再生化学
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能源化学
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DOI
高影响因子
CATALYSIS TODAY
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2014
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IF 3.309
Junjie Zhang,Fang Lu,Weiqiang Yu,Jiazhi Chen,Shuai Chen,Jin Gao,Jie Xu
The use of high pressure fossil derived hydrogen limits the commercial prospects of transforming sorbitol to glycols. Ni–Re/C catalyst which was developed in this study demonstrated high selectivity toward hydrogenative cleavage of C2–C3 and C3–C4 bonds of sorbitol to produce glycols under 1 MPa nitrogen. Acetol which is proposed as important intermediate to explain the reaction mechanism was first detected in the sorbitol conversion reactions. Detailed investigations showed that the presence of Re could prevent the sintering of Ni particles during the reduction process and make the catalyst efficiently generate hydrogen on the active sites to selectively cleave C–C bonds in sorbitol under nitrogen atmosphere.
研究领域:
催化化学
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绿色化学
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DOI
高影响因子
ACS Catalysis
·
2026
·Vol. 16
·期 17
·16793-16808
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IF 13.6
Wang Nan,Fan Guorui,Guo Junhao,Chen Yuqiu,Liu Sibao,Liu Guozhu
To address the challenge of mixed plastic waste management, we present a one-pot hydrodeoxygenation (HDO) process that selectively converts mixed oxygenated aromatic plastics including polyethylene terephthalate (PET), polycarbonate (PC), polyphenyl ether (PPO), and bisphenol-A-based epoxy resin (E20) into high-value cycloalkanes suitable as blendstocks for aviation fuel. Employing a cost-effective Ni−Re/SiO 2 bimetallic catalyst with metal loadings of 15.0 wt % Ni and 11.9 wt % Re, we achieve near-quantitative conversion (up to ca. 94% carbon yield) under mild reaction conditions (240 ° C, 4 MPa H 2 ) and at a high substrate loading of 11.4 wt %. The HDO reaction proceeds through the initial depolymerization of the polymers via acyl and alkyl C−O hydrogenolysis, followed by hydrogenation and deoxygenation. Mechanistic studies including systematic characterizations, control experiments with model compounds, in situ spectroscopy, and DFT calculations indicate that Ni−Re alloy serves as the active site for HDO, with electron-deficient metallic Ni facilitating hydrogen activation and aromatic ring hydrogenation, while oxophilic Re species promote the adsorption and cleavage of diverse C−O bonds. Furthermore, the upscaling potential of this catalytic process was evaluated by integrating laboratory-scale batch experiments with steady-state process simulation (Aspen Plus). Techno-economic analysis (TEA) and life cycle assessment (LCA) reveal that increasing the plastic feedstock concentrations from 4.5 wt % to 11.4 wt % significantly optimizes both economic and environmental performance: the minimum selling price (MSP) is reduced by 6.89% (from 1349 $/t to 1256 $/t), and the global warming potential (GWP) is lowered by 20.7% (from 3.05 to 2.42 kg CO 2 eq). This work provides a practical and non-noble-metal approach for chemically upcycling high concentrated mixed plastic waste, effectively bridging plastic waste valorization with aviation fuel production.
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DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2023
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IF 5.7
Lin Ai,Haonan Shi,Jixiang Chen
Herein, TiO 2 supported Ni–Re alloy catalysts (i.e., NiRe(x:y)/TiO 2 , x:y denotes the Ni/Re atomic ratio) were prepared and tested for in situ deoxygenation of methyl palmitate to hydrocarbons in aqueous phase using methanol as hydrogen donor. Raman spectra indicates that there is interaction between NiO and ReO 4 − species via forming Ni–O-Re(=O) 3 species in the calcined catalysts, which contributes to the formation of Ni–Re alloy and promotes the Ni dispersion during the reduction with H 2 . Particularly, the Ni–Re alloy particles with average size of ∼1.4 nm highly disperse on spherical TiO 2 particles (∼14 nm in diameter) in NiRe(3:4)/TiO 2 (the nominal Ni content of 3 wt %). XPS reveals a charge transfer from metallic Ni to Re in the Ni–Re alloy. In in situ deoxygenation of methyl palmitate, compared with Ni/TiO 2 , NiRe(x:y)/TiO 2 give remarkably higher deoxygenation activity and lower activity for the C–C bond hydrogenolysis , ascribed to the synergistic effect between Ni and Re species and the geometrical effect of Re, respectively, which are further verified by propanoic acid-TPD and TPSR. The yield of C 6 ∼C 16 liquid hydrocarbons can achieve as high as 98.0% on NiRe(3:4)/TiO 2 at 330 °C. There is no obvious sintering of Ni–Re alloy and support TiO 2 particles during the recycling of NiRe(3:4)/TiO 2 , while the carbon deposition and the leaching of Re species slightly reduce the catalyst activity.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子