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
{"title":"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。","authors":"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","doi":"10.1021/acsanm.4c03577","DOIUrl":null,"url":null,"abstract":"<p><p>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 SiO<sub>2</sub>-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<sup>-1</sup>. 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.</p>","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":"7 21","pages":"24356-24367"},"PeriodicalIF":5.3000,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11555637/pdf/","citationCount":"0","resultStr":"{\"title\":\"Controlled Nanopore Sizes in Supraparticle Supports for Enhanced Propane Dehydrogenation with GaPt SCALMS Catalysts.\",\"authors\":\"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\",\"doi\":\"10.1021/acsanm.4c03577\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>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 SiO<sub>2</sub>-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<sup>-1</sup>. 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.</p>\",\"PeriodicalId\":6,\"journal\":{\"name\":\"ACS Applied Nano Materials\",\"volume\":\"7 21\",\"pages\":\"24356-24367\"},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2024-10-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11555637/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Nano Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsanm.4c03577\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/11/8 0:00:00\",\"PubModel\":\"eCollection\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Nano Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsanm.4c03577","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/11/8 0:00:00","PubModel":"eCollection","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
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.
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.