Novel strategy to regulate the geometric and electronic structure of Pt catalyst for efficient propane combustion

IF 4.7 2区 化学 Q2 CHEMISTRY, PHYSICAL Applied Catalysis A: General Pub Date : 2024-05-03 DOI:10.1016/j.apcata.2024.119778
Cai-Hao Wen , Lin-Ya Xu , Wen-Ru Zhao , Hua-Hui Xu , Xi Zhao , Qian Zhou , Cen Tang , Wen-Zhi Jia , Meng-Fei Luo , Jian Chen
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Abstract

The geometric and electronic structure of Pt active sites plays a crucial role in determining the catalysts performance, but precise regulation remains challenging. Herein, we propose a novel approach to modulate the nature of Pt active sites by combining photo-deposition of Pt nanoparticles with ultra-low Mo loading (0.1 wt%) modification on Pt/SiO2 catalysts. The addition of ultra-low loading Mo promoter not only effectively reduces the size of Pt particles but also donates electrons to the Pt particles. Furthermore, the photo-deposited Pt particles exhibit a higher proportion of metallic Pt species, which is more stable than that metallic Pt species obtained by H2 reduction, compared to those prepared using traditional wetness impregnation methods. Propane oxidation activity evaluations confirm that the photo-deposited and Mo-modified Pt/0.1Mo/SiO2-P catalyst exhibits the highest activity among all the prepared catalysts. Combined with experiments of C3H8-TPSR and in-situ DRIFT spectra of propane oxidation, it is found that the Pt/0.1Mo/SiO2-P catalyst remarkably promotes propane activation and C-H bond cleavage due to the nature change of Pt active sites, and the presence of gaseous oxygen benefits propane cleavage on active sites. Our primary results provide a promising strategy for designing superior platinum catalysts by regulating Pt active sites nature for efficient propane complete oxidation.

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调节铂催化剂几何和电子结构以高效燃烧丙烷的新策略
铂活性位点的几何和电子结构在决定催化剂性能方面起着至关重要的作用,但精确调节仍具有挑战性。在此,我们提出了一种新方法,通过在 Pt/SiO2 催化剂上光照沉积 Pt 纳米颗粒和改性超低摩负载(0.1 wt%)来调节 Pt 活性位点的性质。超低负载钼促进剂的加入不仅有效地减小了铂粒子的尺寸,而且还为铂粒子提供了电子。此外,与传统的湿法浸渍法相比,光沉积铂粒子中金属铂的比例更高,比通过 H2 还原法获得的金属铂更稳定。丙烷氧化活性评估证实,在所有制备的催化剂中,光沉积和 Mo 改性 Pt/0.1Mo/SiO2-P 催化剂的活性最高。结合丙烷氧化的 C3H8-TPSR 和原位 DRIFT 光谱实验发现,由于铂活性位点的性质变化,Pt/0.1Mo/SiO2-P 催化剂显著促进了丙烷的活化和 C-H 键的裂解,气态氧的存在有利于活性位点上丙烷的裂解。我们的主要研究结果为通过调节铂活性位点的性质来设计优质铂催化剂提供了一种可行的策略,从而实现高效的丙烷完全氧化。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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