室温电子还原法制备的正十六烷加氢异构化高效 Pt-Pd/ZSM-22 催化剂

IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Fuel Processing Technology Pub Date : 2024-08-14 DOI:10.1016/j.fuproc.2024.108117
Huiyan Li , Kaihang Sun , Shuxiang Xiong , Wei Wang , Wei Wu
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引用次数: 0

摘要

开发高效的正十六烷加氢异构化双功能催化剂对于生产第二代生物柴油仍然至关重要。本文采用室温电子还原(RTER)法,以辉光放电为电子源,制备了一种 Pt-Pd/ZSM-22-G(简称 Pt-Pd/Z22-G)双金属催化剂。相比之下,传统的氢还原法制备了一系列 Pt/Z22-H、Pd/Z22-H 和 Pt-Pd/Z22-H 催化剂。与 Pt/Z22-H、Pd/Z22-H 和 Pt-Pd/Z22-H 催化剂相比,Pt-Pd/Z22-G 催化剂暴露的金属位点更多,CMe/CH+ 值更大,Pt-Pd(111) 面分布更广。这些变化源于高能还原电子作用下更强的电子相互作用和更小的金属纳米颗粒。正十六烷加氢异构化结果表明,Pt-Pd/Z22-G 催化剂的异构十六烷产率为 82.9%,是本次研究的四种催化剂中产率最高的。出现这种现象的原因是,根据密度泛函理论(DFT)计算,更多的 Pt-Pd(111)面暴露和更大的 CMe/CH+ 比有利于异构烯中间体在金属位点的吸附和氢化,从而提高异构烷烃的产率。此外,由于金属聚集和碳沉积有限,Pt-Pd/Z22-G 催化剂上的异构烷烃产率在经过 120 小时的长期测试后也保持稳定。
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Highly effective Pt-Pd/ZSM-22 catalysts prepared by the room temperature electron reduction method for the n-hexadecane hydroisomerization

The development of highly effective bifunctional catalysts for n-hexadecane hydroisomerization is still essential to produce second-generation biodiesel. Herein, a Pt-Pd/ZSM-22-G (abbreviated as Pt-Pd/Z22-G) bimetallic catalyst was prepared by employing a room temperature electron reduction (RTER) method with glow discharge as the electron source. As a contrast, a series of Pt/Z22-H, Pd/Z22-H and Pt-Pd/Z22-H catalysts were prepared by the conventional hydrogen reduction method. The Pt-Pd/Z22-G catalyst reveals more exposed metal sites, larger CMe/CH+ values and an enhanced distribution of Pt-Pd(111) facets compared with the Pt/Z22-H, Pd/Z22-H and Pt-Pd/Z22-H catalysts. These modifications are originated from the stronger electron interactions and the smaller metal nanoparticles because of the effects of highly energetic reducing electrons. The n-hexadecane hydroisomerization results show that the iso-hexadecane yield over the Pt-Pd/Z22-G catalyst is 82.9%, which is the highest among four investigated catalysts in this work. This phenomenon occurs because more exposed Pt-Pd(111) facets and larger CMe/CH+ ratios are beneficial for the adsorption and hydrogenation of iso-alkene intermediates at metal sites to increase the iso-alkanes yield based on density functional theory (DFT) calculations. Furthermore, the iso-alkanes yield over the Pt-Pd/Z22-G catalyst also keeps steady after long-term tests for 120 h because of the limited metal aggregation and carbon deposition.

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来源期刊
Fuel Processing Technology
Fuel Processing Technology 工程技术-工程:化工
CiteScore
13.20
自引率
9.30%
发文量
398
审稿时长
26 days
期刊介绍: Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.
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