利用 GaPt SCALMS 催化剂增强丙烷脱氢的超微粒载体中的可控纳米孔径。

IF 5.3 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Nano Materials Pub Date : 2024-10-29 eCollection Date: 2024-11-08 DOI:10.1021/acsanm.4c03577
Nnamdi Madubuko, Umair Sultan, Simon Carl, Daniel Lehmann, Xin Zhou, Alexander Soegaard, Nicola Taccardi, Benjamin Apeleo Zubiri, Susanne Wintzheimer, Erdmann Spiecker, Marco Haumann, Nicolas Vogel, Peter Wasserscheid
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引用次数: 0

摘要

将 GaPt 液体金属合金液滴有效固定在定制的支撑物上可防止凝聚和随后的活性表面积损失,从而提高催化性能。在此,我们使用具有可控纳米孔的定制超微粒(SP)支撑物,系统地研究了孔径大小对丙烷脱氢(PDH)中GaPt支撑的催化活性液态金属溶液(SCALMS)催化稳定性的影响。首先,通过原子高效、可扩展的超声波循环法制备了 GaPt 液滴,得到了基于液滴 2 的 SPs,其孔径范围在 45 到 320 nm 之间。在 PDH 中进行的催化评估显示,固定在较大孔隙 SPs 上的 GaPt 在 15 小时的流化时间内表现出卓越的稳定性,失活率从 0.046 h-1 降低到 0.026 h-1。纳米计算机断层扫描和相同位置的扫描电镜证实,GaPt 液滴成功地固定在由构成 SPs 的主颗粒形成的间隙中。这些液滴在催化反应前后保持不变,证明了有效的防凝聚作用。我们的研究结果强调了支撑孔径工程对于提高 GaPt SCALMS 催化剂稳定性的重要性,并特别强调了在这种情况下使用 SPs 的巨大潜力。
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Controlled Nanopore Sizes in Supraparticle Supports for Enhanced Propane Dehydrogenation with GaPt SCALMS Catalysts.

The efficient immobilization of GaPt liquid metal alloy droplets onto tailored supports improves catalytic performance by preventing coalescence and subsequent loss of active surface area. Herein, we use tailored supraparticle (SP) supports with controlled nanopores to systematically study the influence of pore sizes on the catalytic stability of GaPt supported catalytically active liquid metal solution (SCALMS) in propane dehydrogenation (PDH). Initially, GaPt droplets were prepared via an atom-efficient and scalable ultrasonication method with recycling loops to yield droplets <300 nm. Subsequently, these droplets were immobilized onto SiO2-based SPs with controlled pore sizes ranging from 45 to 320 nm. Catalytic evaluations in PDH revealed that GaPt immobilized on SPs with larger pores demonstrated superior stability over 15 h time-on-stream evidenced by reduced deactivation rates from 0.046 to 0.026 h-1. Nanocomputed tomography and identical location SEM confirmed the successful immobilization of GaPt droplets within the interstitial sites formed by the primary particles constituting the SPs. These remained unchanged before and after the catalytic reaction, demonstrating efficient coalescence prevention. Our findings underscore the importance of support pore size engineering for improving the stability of GaPt SCALMS catalysts and highlight, particularly, the high potential of using SPs in this context.

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来源期刊
CiteScore
8.30
自引率
3.40%
发文量
1601
期刊介绍: ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.
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