Phase-Transition-Induced Surface Reconstruction of Rh1 Site in Intermetallic Alloy for Propane Dehydrogenation,The Journal of Physical Chemistry Letters

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Phase-Transition-Induced Surface Reconstruction of Rh1 Site in Intermetallic Alloy for Propane Dehydrogenation
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2024-04-18 , DOI: 10.1021/acs.jpclett.4c00719
Peng Yin _{1,

2} , Jialong Shi ₃ , Ming Zuo ₂ , Wanqun Zhang ₂ , Bo Peng ₄ , Bin Jiang ₃ , Xian-Zhu Fu ₁ , Hai-Wei Liang ₂

Affiliation

The fine-tuning of the geometric and electronic structures of active sites plays a crucial role in catalysis. However, the intricate entanglement between the two aspects results in a lack of interpretable design for active sites, posing a challenge in developing high-performance catalysts. Here, we find that surface reconstruction induced by phase transition in intermetallic alloys enables synergistic geometric and electronic structure modulation, creating a desired active site microenvironment for propane dehydrogenation. The resulting electron-rich four-coordinate Rh₁ site in the RhGe_0.5Ga_0.5 intermetallic alloy can accelerate the desorption of propylene and suppress the side reaction and thus exhibits a propylene selectivity of ∼98% with a low deactivation constant of 0.002 h^–1 under propane dehydrogenation at 550 °C. Furthermore, we design a computational workflow to validate the rationality of the microenvironment modulation induced by the phase transition in an intermetallic alloy.

中文翻译：

丙烷脱氢金属间合金中 Rh1 位点的相变诱导表面重构

活性位点的几何和电子结构的微调在催化中起着至关重要的作用。然而，这两方面之间错综复杂的纠缠导致活性位点缺乏可解释的设计，给开发高性能催化剂带来了挑战。在这里，我们发现金属间合金中相变引起的表面重构能够实现协同几何和电子结构调制，为丙烷脱氢创造所需的活性位点微环境。在RhGe _0.5 Ga _0.5金属间合金中产生的富电子四配位Rh ₁位点可以加速丙烯的解吸并抑制副反应，从而表现出~98%的丙烯选择性和0.002 h ^–1的低失活常数在550℃下丙烷脱氢。此外，我们设计了一个计算工作流程来验证金属间合金中相变引起的微环境调制的合理性。

更新日期：2024-04-18

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