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使用生物质衍生的氢源,在负载于HY沸石上的镍交换12-钨磷酸上生产生物基液体燃料添加剂γ-戊内酯。

Production of a bio-based liquid fuel additive, γ-valerolactone, over Ni-exchanged 12-tungstophosphoric acid anchored to zeolite HY using a biomass-derived H source.

作者信息

Patel Anjali, Chauhan Kavan

机构信息

Polyoxometalates and Catalysis Laboratory, Department of Chemistry, Faculty of Science, The Maharaja Sayajirao University of Baroda Vadodara- 390020 Gujarat India

出版信息

RSC Adv. 2025 Aug 21;15(36):29490-29499. doi: 10.1039/d5ra04872a. eCollection 2025 Aug 18.

Abstract

In present scenario the synthesis of sustainable biofuel additive using hydrogenation of biomass derived compound with green hydrogen source gained tremendous attention due to the fast-growing attention on the circular economy. So, in this work, we demonstrated the liquid phase hydrogenation of levulinic acid to γ-valerolactone using biomass derived green hydrogen source over a non-noble metal based heterogenous catalyst. Here, a non-noble metal-based catalyst, comprising nickel exchanged 12-tungstophosphoric acid anchored Zeolite HY, was synthesized and thoroughly characterized using various techniques, including EDS, NH-TPD, BET, FTIR, UV-vis-NIR, XPS, and HRTEM. In catalytic study it demonstrated outstanding performance, as obtained 72% yield of GVL, and 514 turnover number (TON). These confirmed the innovative strategy of eliminating the need for an external hydrogen source. These results emphasize the catalysts efficiency, superior activity, and stability under mild reaction conditions, make it as a more sustainable and effective alternative to existing non noble metal-based catalysts. Also, kinetic studies were conducted to determine the reaction order. Additionally, the in-situ reduction of Ni(II) to Ni(0), was studied and confirmed via XPS analysis. This work demonstrate the potential of catalyst in sustainable and renewable energy solutions, contributing significantly to the development of green and economically viable processes.

摘要

在当前形势下,由于对循环经济的关注度迅速上升,利用生物质衍生化合物与绿色氢源进行氢化反应合成可持续生物燃料添加剂受到了极大关注。因此,在本工作中,我们展示了在非贵金属基多相催化剂上,使用生物质衍生的绿色氢源将乙酰丙酸液相加氢生成γ-戊内酯。在此,合成了一种由镍交换的12-钨磷酸锚定在HY沸石上的非贵金属基催化剂,并使用多种技术进行了全面表征,包括能谱分析(EDS)、程序升温脱附(NH-TPD)、比表面积分析(BET)、傅里叶变换红外光谱(FTIR)、紫外-可见-近红外光谱(UV-vis-NIR)、X射线光电子能谱(XPS)和高分辨率透射电子显微镜(HRTEM)。在催化研究中,它表现出优异的性能,γ-戊内酯的产率达到72%,周转数(TON)为514。这些结果证实了无需外部氢源的创新策略。这些结果强调了该催化剂在温和反应条件下的效率、卓越活性和稳定性,使其成为现有非贵金属基催化剂更可持续、更有效的替代品。此外,还进行了动力学研究以确定反应级数。另外,通过XPS分析研究并证实了Ni(II)原位还原为Ni(0)的过程。这项工作展示了该催化剂在可持续和可再生能源解决方案中的潜力,对绿色且经济可行的工艺开发做出了重大贡献。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be40/12377281/6dfbfa963ce0/d5ra04872a-s1.jpg

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