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Strategies for Regeneration of Pt-alloy Catalysts Supported on Silica for Propane Dehydrogenation
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2023-03-22 , DOI: 10.1016/j.apcata.2023.119157
Ryan Alcala , David P. Dean , Isha Chavan , Che-Wei Chang , Brandon Burnside , Hien N. Pham , Eric Peterson , Jeffrey T. Miller , Abhaya K. Datye

Catalyst stability, resistance to deactivation, and regeneration remain a challenge for high temperature reaction processes. For Pt alloys used in propane dehydrogenation (PDH), the primary pathways of catalyst deactivation include coke formation and metal nanoparticle sintering over time. Recent work shows that silica-supported catalysts provide excellent selectivity for this reaction, but the regenerability of silica-supported catalysts has not been established. In this work, we study a series of Pt alloys, including PtMn, PtZn, and PtSn, for the PDH reaction at 550 °C and 600 °C, and we subject the catalyst materials to regeneration over multiple cycles. While oxidation in air restores the reactivity completely with minimal catalyst sintering, it is surprising to find that these catalysts can also be regenerated in pure hydrogen. Here we explore the types of coke formed on these catalysts using in situ temperature programmed oxidation (TPO). Two types of coke are found: one on the metallic NP surface, and a second on the silica support. Our work shows that treatment in hydrogen causes redistribution of the coke between the metal and support, which can restore most catalytic activity lost during a reaction run. Periodic introduction of H2 during a reaction cycle may constitute an unexplored strategy for extending the lifetime of PDH catalysts.



中文翻译:

丙烷脱氢二氧化硅负载铂合金催化剂的再生策略

催化剂稳定性、抗失活性和再生性仍然是高温反应过程面临的挑战。对于丙烷脱氢 (PDH) 中使用的 Pt 合金,催化剂失活的主要途径包括焦炭形成和金属纳米颗粒随时间烧结。最近的研究表明,二氧化硅负载的催化剂为该反应提供了出色的选择性,但二氧化硅负载的催化剂的可再生性尚未确定。在这项工作中,我们研究了一系列 Pt 合金,包括 PtMn、PtZn 和 PtSn,用于 550 °C 和 600 °C 下的 PDH 反应,并且我们对催化剂材料进行多次循环再生。虽然空气中的氧化完全恢复了反应活性,催化剂烧结最少,但令人惊讶的是,这些催化剂也可以在纯氢气中再生。原位程序升温氧化(TPO)。发现了两种类型的焦炭:一种在金属 NP 表面,另一种在二氧化硅载体上。我们的工作表明,在氢气中处理会导致金属和载体之间的焦炭重新分布,这可以恢复反应运行期间损失的大部分催化活性。在反应循环期间定期引入 H 2可能构成一种未开发的延长 PDH 催化剂寿命的策略。

更新日期:2023-03-22
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