IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2025-01-20 DOI:10.1039/d4cy01226g
Xiyue Lu , Hui Wang , Wei Liu , Mooeez ur Rehman , Lu Wang , Yan Xu , Shengnian Wang , Yujun Zhao
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摘要

有效的非贵金属催化剂对于通过加氢脱氧反应(HDO)将木质素衍生化合物升级为有价值的产品至关重要。本研究结合溶胶-凝胶法和浸渍法合成了新型 Ni0-NiNbOx/SiO2 催化剂。然后评估了这些催化剂在从木质素衍生的酚类化合物生产环烷烃过程中的 HDO 性能。与 Ni/SiO2 催化剂相比,这些 Ni0-NiNbOx/SiO2 催化剂的比表面积要大得多。它们在 HDO 过程中可作为双功能催化剂发挥作用,其中 Ni0 物种作为氢化的活性位点,而 NiNbOx 则提供脱氧所需的路易斯酸位点。这样,在这些 Ni0-NiNbOx/SiO2 催化剂上,愈创木酚 HDO 的环己烷产率从 18% 显著提高到 94.4%。最佳催化剂 10Ni/20Nb@SiO2 在 250 °C 下可实现愈创木酚的完全转化,环烷的选择性几乎达到 100%。10Ni/20Nb@SiO2 催化剂的表观活化能为 54.2 kJ mol-1,明显低于其他已报道的镍基催化剂。这些发现凸显了 Ni0-NiNbOx/SiO2 催化剂在木质素衍生酚类化合物 HDO 中的卓越性能,强调了其在利用可再生资源生产环烷烃方面的巨大潜力。我们的努力有助于为木质素催化转化为有价值的生物燃料铺平道路,从而推动全球实现燃料的可持续供应。
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The promoting effect of Nb on Ni/SiO2 in the hydrodeoxygenation of lignin derivatives to cycloalkanes†
Effective non-noble metal catalysts are critical for upgrading lignin-derived compounds into valuable products by hydrodeoxygenation (HDO). In this study, new Ni0–NiNbOx/SiO2 catalysts were synthesized by combining sol–gel and impregnation methods. The HDO performance of these catalysts was then evaluated in the production of cycloalkanes from lignin-derived phenolic compounds. These Ni0–NiNbOx/SiO2 catalysts present a considerably larger specific surface area than their Ni/SiO2 counterparts. They work as bifunctional catalysts in the HDO process, where Ni0 species act as active sites for hydrogenation while NiNbOx provides the Lewis acid sites necessary for deoxygenation. In this way, a significant improvement in the cyclohexane yield from 18% to 94.4% in guaiacol HDO was achieved on these Ni0–NiNbOx/SiO2 catalysts. The best catalyst 10Ni/20Nb@SiO2 exhibits complete conversion of guaiacol and almost 100% selectivity of cycloalkanes at 250 °C. The apparent activation energy for the 10Ni/20Nb@SiO2 catalyst was identified to be 54.2 kJ mol−1, notably lower than that for other reported Ni-based catalysts. These findings highlight the superior performance of Ni0–NiNbOx/SiO2 catalysts in the HDO of lignin-derived phenolic compounds, underscoring their great potential in producing cycloalkanes from renewable resources. Our efforts help pave the way for the catalytic transformation of lignin into valuable biofuels to advance the global mission toward a sustainable supply of fuels.
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
期刊最新文献
Back cover Polystyrene-bound AlCl3 - a catalyst for the solvent-free synthesis of aryl-substituted tetrazoles. Back cover Inside back cover Back cover
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