高硅faujasite沸石定制的金属封装,用于低温生产戊烷生物燃料

IF 14 1区 化学 Q1 CHEMISTRY, APPLIED 能源化学 Pub Date : 2023-10-17 DOI:10.1016/j.jechem.2023.10.009
Wenhao Cui , Yuanshuai Liu , Pengfei Guo , Zhijie Wu , Liqun Kang , Huawei Geng , Shengqi Chu , Linying Wang , Dong Fan , Zhenghao Jia , Haifeng Qi , Wenhao Luo , Peng Tian , Zhongmin Liu
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引用次数: 0

摘要

沸石包裹的金属纳米团簇是双功能催化剂的核心,在石化转化和新兴的可持续生物炼制中具有巨大的潜力。然而,将金属纳米团簇有效地封装到高硅分子筛Y中,特别是具有良好的结构完整性,仍然是一个重大挑战。在此,我们通过直接合成沸石和连续浸染金属封装的合作策略,构建了Ru纳米团簇(~ 1 nm)封装在SiO2/Al2O3比(SAR)为10的高硅沸石Y (SY)中。与基准的Ru/H-USY和其他类似物相比,制备的Ru/H-SY在180°C的温和温度下显著提高了戊烷生物燃料的产率和生物质衍生的乙酰丙酸酯的直接加氢脱氧稳定性,这是由于良好的结构完整性增强了酸的可及性和适当的沸石腔尺寸限制,从而显著稳定了过渡态。
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High-silica faujasite zeolite-tailored metal encapsulation for the low-temperature production of pentanoic biofuels

Zeolite-encapsulated metal nanoclusters are at the heart of bifunctional catalysts, which hold great potential for petrochemical conversion and the emerging sustainable biorefineries. Nevertheless, efficient encapsulation of metal nanoclusters into a high-silica zeolite Y in particular with good structural integrity still remains a significant challenge. Herein, we have constructed Ru nanoclusters (∼1 nm) encapsulated inside a high-silica zeolite Y (SY) with a SiO2/Al2O3 ratio (SAR) of 10 via a cooperative strategy for direct zeolite synthesis and a consecutive impregnation for metal encapsulation. Compared with the benchmark Ru/H-USY and other analogues, the as-prepared Ru/H-SY markedly boosts the yields of pentanoic biofuels and stability in the direct hydrodeoxygenation of biomass-derived levulinate even at a mild temperature of 180 °C, which are attributed to the notable stabilization of transition states by the enhanced acid accessibility and properly sized constraints of zeolite cavities owing to the good structural integrity.

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23.60
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2875
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