Ultrastable Pt/Zn-Doped-Al2O3 Catalyst for Propane Dehydrogenation

IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry C Pub Date : 2024-12-20 DOI:10.1021/acs.jpcc.4c05898
Yanan Xing, Bonan Li, Leilei Kang, Yang Su, Xiaoli Pan, Lin Li, Hua Liu, Xiao Yan Liu, Aiqin Wang, Tao Zhang
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Abstract

Propane dehydrogenation (PDH) is a crucial and effective technology to produce propylene industrially and is in great demand around the globe. Silica/zeolite-supported PtZn bimetallic catalysts have been reported to exhibit long-term operation and a consecutive regeneration process at high temperatures. However, over the industrially most commonly used support Al2O3, PtZn bimetallic nanoparticles suffer from low stability. Herein, we develop Zn-doped Al2O3 (ZnAlOx) to stabilize PtZn nanoparticles (<1 nm) for the PDH reaction, for which the structure and composition of the PtZn intermetallic nanoparticles could be controlled by tuning the ratio of Zn/Al. The optimized catalyst with Zn/Al = 1/5 (mole ratio) exhibited the most remarkable stability with an extremely low kd value of 0.0007 h–1 and survived 10 cycles of regeneration tests with negligible deactivation. Characterizations by HAADF-STEM, XAS, and XRD, together with in situ XPS and CO-DRIFTS, proved that the excellent performance originated from the Pt1Zn1 intermetallic compound formed during the reaction and the enhanced interaction between the Pt1Zn1 nanoparticles and the Zn-doped Al2O3 support.

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超稳定Pt/ zn掺杂al2o3丙烷脱氢催化剂
丙烷脱氢(PDH)是工业化生产丙烯的一项重要而有效的技术,在全球范围内需求量很大。据报道,二氧化硅/沸石支撑的 PtZn 双金属催化剂可在高温下长期运行并可连续再生。然而,在工业上最常用的载体 Al2O3 上,PtZn 双金属纳米颗粒的稳定性较低。在此,我们开发了掺杂锌的 Al2O3(ZnAlOx)来稳定用于 PDH 反应的 PtZn 纳米粒子(<1 nm),其 PtZn 金属间纳米粒子的结构和组成可通过调节 Zn/Al 的比例来控制。Zn/Al = 1/5(摩尔比)的优化催化剂表现出最显著的稳定性,其 kd 值极低,仅为 0.0007 h-1,并且在 10 次再生试验中几乎没有失活。利用 HAADF-STEM、XAS 和 XRD 以及原位 XPS 和 CO-DRIFTS 进行的表征证明,优异的性能源于反应过程中形成的 Pt1Zn1 金属间化合物,以及 Pt1Zn1 纳米粒子与掺杂 Zn 的 Al2O3 载体之间增强的相互作用。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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