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通过超声处理制备的镓-铂负载催化活性液态金属溶液(SCALMS)——合成条件对庚烷脱氢性能的影响

Ga-Pt supported catalytically active liquid metal solutions (SCALMS) prepared by ultrasonication - influence of synthesis conditions on -heptane dehydrogenation performance.

作者信息

Sebastian Oshin, Al-Shaibani Asem, Taccardi Nicola, Sultan Umair, Inayat Alexandra, Vogel Nicolas, Haumann Marco, Wasserscheid Peter

机构信息

Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU), Lehrstuhl für Chemische Reaktionstechnik (CRT) Egerlandstraße 3 91058 Erlangen Germany

Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU), Lehrstuhl für Feststoff- und Grenzflächenverfahrenstechnik (LFG) Cauerstraße 4 91058 Erlangen Germany.

出版信息

Catal Sci Technol. 2023 Jul 10;13(15):4435-4450. doi: 10.1039/d3cy00356f. eCollection 2023 Jul 31.

DOI:10.1039/d3cy00356f
PMID:38014413
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10388703/
Abstract

Supported catalytically active liquid metal solution (SCALMS) materials represent a recently developed class of heterogeneous catalysts, where the catalytic reaction takes place at the highly dynamic interface of supported liquid alloys. Ga nuggets were dispersed into nano-droplets in propan-2-ol using ultrasonication followed by the addition of Pt in a galvanic displacement reaction - either directly into the Ga/propan-2-ol dispersion () or consecutively onto the supported Ga droplets (). The galvanic displacement reaction between Ga and Pt was studied in three different reaction media, namely propan-2-ol, water, and 20 vol% water containing propan-2-ol. TEM investigations reveal that the Ga-Pt reaction in propan-2-ol resulted in the formation of Pt aggregates on top of Ga nano-droplets. In the water/propan-2-ol mixture, the desired incorporation of Pt into the Ga matrix was achieved. The prepared Ga-Pt SCALMS were tested in -heptane dehydrogenation. Ga-Pt SCALMS synthesized in pure alcoholic solution showed equal dehydrogenation and cracking activity. Ga-Pt SCALMS prepared in pure water, in contrast, showed mainly cracking activity due to oxidation of Ga droplets. The Ga-Pt SCALMS material prepared in water/propan-2-ol resulted in high activity, -heptene selectivity of 63%, and only low cracking tendency. This can be attributed to the supported liquid Ga-Pt alloy where Pt atoms are present in the liquid Ga matrix at the highly dynamic catalytic interface.

摘要

负载型催化活性液态金属溶液(SCALMS)材料是一类最近开发的多相催化剂,催化反应发生在负载型液态合金的高度动态界面处。使用超声处理将镓块分散在异丙醇中的纳米液滴中,然后在电置换反应中加入铂——要么直接加入到镓/异丙醇分散液中(),要么依次加入到负载的镓液滴上()。在三种不同的反应介质中研究了镓和铂之间的电置换反应,即异丙醇、水和含20体积%水的异丙醇。透射电子显微镜研究表明,在异丙醇中镓与铂的反应导致在镓纳米液滴顶部形成铂聚集体。在水/异丙醇混合物中,实现了将铂所需地掺入镓基体中。所制备的镓-铂SCALMS在庚烷脱氢反应中进行了测试。在纯醇溶液中合成的镓-铂SCALMS表现出同等的脱氢和裂解活性。相比之下,在纯水中制备的镓-铂SCALMS主要表现出裂解活性,这是由于镓液滴的氧化。在水/异丙醇中制备的镓-铂SCALMS材料具有高活性、63%的庚烯选择性且只有低裂解倾向。这可归因于负载型液态镓-铂合金,其中铂原子存在于高度动态催化界面处的液态镓基体中。

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