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期刊论文 2

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2023 1

2022 1

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Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated Ni–Sn intermetallic compounds with methanol as hydrogen donor

《化学科学与工程前沿(英文)》 2023年 第17卷 第2期   页码 139-155 doi: 10.1007/s11705-022-2217-4

摘要: Porous carbon-encapsulated Ni and Ni–Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen donor. During the catalyst preparation, Sn doping reduces the size of carbon spheres, and the formation of Ni–Sn intermetallic compounds restrain the graphitization, contributing to larger pore volume and pore diameter. Consequently, a more facile mass transfer occurs in carbon-encapsulated Ni–Sn intermetallic compound catalysts than in carbon-encapsulated Ni catalysts. During the in-situ hydrothermal deoxygenation, the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to hexadecanol. At high reaction temperature, hexadecanol undergoes dehydrogenation–decarbonylation, generating n-pentadecane. Also, the C–C bond hydrolysis and methanation are suppressed on Ni–Sn intermetallic compounds, favorable for increasing the carbon yield and reducing the H2 consumption. The n-pentadecane and n-hexadecane yields reached 88.1% and 92.8% on carbon-encapsulated Ni3Sn2 intermetallic compound at 330 °C. After washing and H2 reduction, the carbon-encapsulated Ni3Sn2 intermetallic compound remains stable during three recycling cycles. This is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词: extended Stöber method     carbon encapsulated Ni–Sn intermetallic compounds     confinement     in-situ hydrothermal deoxygenation     hydrogenation     decarbonylation    

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation of methyl palmitate to hydrocarbons using methanol as the hydrogen donor

《化学科学与工程前沿(英文)》 2022年 第16卷 第3期   页码 443-460 doi: 10.1007/s11705-021-2079-1

摘要: Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n-pentadecane and n-C6n-C16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO2 recovered the catalyst reactivity.

关键词: Stöber method     carbon-coated Ni-Co alloy     in-situ hydrodeoxygenation     methyl palmitate     decarbonylation/decarboxylation    

标题 作者 时间 类型 操作

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated Ni–Sn intermetallic compounds with methanol as hydrogen donor

期刊论文

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation of methyl palmitate to hydrocarbons using methanol as the hydrogen donor

期刊论文