UiO-66-X催化剂负载Ni-Fe纳米颗粒催化脂肪酸酯加氢制醇

Chem & Bio Engineering Pub Date : 2024-09-16 eCollection Date: 2025-01-23 DOI:10.1021/cbe.4c00108
Pengcheng Li, Tianyu Ma, Youyang Wu, Jianping Wu, Haoran Yu, Lirong Yang, Gang Xu
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引用次数: 0

摘要

提高非贵金属催化剂的性能有助于提高化学转化过程的经济可行性。通过金属纳米颗粒(MNPs)尺寸控制和载体功能化修饰等策略,制备了Ni2Fe6/ uui -66-X-y催化剂(X代表H、OH、CH3和NH2, y代表NaBH4溶液浓度),用于月桂酸甲酯(ML)高效选择性加氢制备1-十二醇。高浓度NaBH4溶液有利于制备较小尺寸的MNPs,而载体功能化可以改变载体的化学微环境,从而促进适当尺寸的MNPs与载体之间的电子转移。其中,Ni2Fe6/ uyo -66- nh2 -0.4 M催化剂在220℃、3 MPa H2条件下反应8 h时,ML转化率达到99.9%,1-十二醇选择性达到98.6%。讨论了基于η2(C, O)醛构象的催化机理,并计算了反应动力学。此外,该催化剂实现了五次稳定的循环运行,并证明了对其他脂肪酸甲酯的催化通用性,包括硬脂酸甲酯、棕榈酸甲酯和戊酸甲酯。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Ni-Fe Nanoparticles Supported on UiO-66-X Catalyst for Hydrogenation of Fatty Acid Esters to Alcohols.

Enhancing the performance of non-noble-metal catalysts would facilitate the economic feasibility of the chemical conversion process. Through strategies involving metal nanoparticles (MNPs) size control and support functionalization modification, Ni2Fe6/UiO-66-X-y catalysts (X stands for H, OH, CH3, and NH2, and y stands for the concentration of NaBH4 solution) were prepared for the efficiently selective hydrogenation of methyl laurate (ML) to 1-dodecanol. High-concentration NaBH4 solution facilitated the preparation of smaller-sized MNPs, while support functionalization could alter the chemical microenvironment of the support, thereby promoting electron transfer between appropriately sized MNPs and the support. In particular, the Ni2Fe6/UiO-66-NH2-0.4 M catalyst could achieve 99.9% conversion of ML and 98.6% selectivity for 1-dodecanol when it was reacted at 220 °C and 3 MPa H2 for 8 h. The probable catalytic mechanism based on the η2(C, O)-aldehyde conformation was discussed, and reaction kinetics were calculated. Furthermore, the catalyst achieved five stable recycling runs and demonstrated catalytic versatility for other fatty acid methyl esters, including methyl stearate, methyl palmitate, and methyl valerate.

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