The role of pentacoordinate Al3+ sites of Pt/Al2O3 catalysts in propane dehydrogenation

IF 6.2 3区综合性期刊 Q1 Multidisciplinary Fundamental Research Pub Date : 2024-11-01 DOI:10.1016/j.fmre.2022.08.020

Yan Wang , Chunlei Pei , Xianhui Wang , Guodong Sun , Zhi-Jian Zhao , Jinlong Gong

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Abstract

Pentacoordinate Al³⁺ (Al³⁺_penta) sites on alumina (Al₂O₃) could anchor and stabilize the active site over the catalyst surface. The paper describes the specific effect of Al³⁺_penta sites on the structure and the catalytic performance of Al₂O₃ supported Pt catalysts by modulating the quantity of Al³⁺_penta sites. The Al³⁺_penta site content of Al₂O₃ exhibits a volcano-type profile as a function of calcination temperature due to the structural rearrangement. The loading of Pt and subsequent calcination can consume a significant portion of Al³⁺_penta sites over the Al₂O₃ support. We further find that, when the calcination temperature of the impregnated Al₂O₃ is higher than the calcination temperature of Al₂O₃ precursor, the structural rearrangement of Al³⁺_penta sites could make Pt partially buried in Al₂O₃. Consequently, this partially buried structure leads to relatively low conversion but high stability for propane dehydrogenation. This work further elucidates the stabilization mechanism of the Al³⁺_penta site over Al₂O₃ support.

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Pt/Al2O3催化剂五配位Al3+在丙烷脱氢中的作用

氧化铝（Al2O3）上的五配位Al3+ (Al3+penta)位点可以锚定和稳定催化剂表面的活性位点。通过调节Al3+五价位的数量，研究了Al3+五价位对Al2O3负载Pt催化剂结构和催化性能的具体影响。由于结构重排，Al2O3的Al3+五羧基含量随煅烧温度的变化呈火山型分布。Pt的加载和随后的煅烧可以在Al2O3载体上消耗相当一部分Al3+penta位点。进一步发现，当浸渍Al2O3的煅烧温度高于Al2O3前驱体的煅烧温度时，Al3+五价位的结构重排可以使Pt部分埋埋在Al2O3中。因此，这种部分埋藏的结构导致丙烷脱氢的转化率相对较低，但稳定性较高。这项工作进一步阐明了Al3+五羧基在Al2O3载体上的稳定机制。

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