Lei Qian, Jun Cheng, Kai Xin, Hao Guo, Yuxiang Mao, Jiacan Tu, Weijuan Yang
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引用次数: 0
摘要
考虑到微藻的快速生长和高含油量,利用微藻油生产生物柴油是解决原油资源减少和环境污染问题的关键技术。为了提高锆基金属有机框架(Zr-MOFs)的低温活性,我们采用了一种简单、多用途的一锅合成方法,制备了掺杂混合价铈的 MOF-808,并增强了桥接羟基,用于在显著降低的温度下转化微藻脂质。密度泛函理论计算表明,成功掺入 Ce(III) 离子可促进 Zr/Ce-MOF-808 中邻近原子的电子脱ocal,降低甲醇的活化温度,形成独特的富电子桥接羟基结构,从而大大提高低温活性。与原始 MOF-808 相比,Zr/Ce(1:1)-MOF-808 在 100 °C 时的催化转化效率从 8.34% 提高到 89.51%,反应器压力从 200 °C 时的 4036 kPa 显著降低到 100 °C 时的 352 kPa。由于催化剂的金属中心与反应物之间建立了间接接触,催化剂在使用五个周期后,转化效率仅降低了 3%。
Enhanced hydroxyl bridge-mediated microalgal lipid conversion via mixed-valence Zr/Ce-MOF-808 catalysts at reduced temperatures
Considering the rapid growth and high oil content of microalgae, biodiesel production from microalgal oil is a key technology to address declining crude oil resources and environmental pollution. To enhance the low-temperature activity of Zr based metal–organic framework (Zr-MOFs), we employed a simple and versatile one-pot synthesis approach to fabricate mixed-valence Ce-doped MOF-808 with enhanced bridging hydroxyl groups, for the conversion of microalgal lipids at significantly reduced temperatures. Density functional theory calculations revealed that successful doping of Ce(III) ions facilitated electronic delocalization of neighboring atoms in Zr/Ce-MOF-808, lowering the activation temperature of methanol and forming a unique electron-rich bridging hydroxyl structure, thereby greatly enhancing low-temperature activity. Compared to pristine MOF-808, Zr/Ce (1 : 1)-MOF-808 exhibited a catalytic conversion efficiency increase from 8.34% to 89.51% at 100 °C, significantly reducing reactor pressure from 4036 kPa at 200 °C to 352 kPa at 100 °C. With indirect contact established between the catalyst's metal centers and reactants, the catalyst demonstrated only a 3% decrease in conversion efficiency after five cycles of use.
期刊介绍:
Sustainable Energy & Fuels will publish research that contributes to the development of sustainable energy technologies with a particular emphasis on new and next-generation technologies.