O-(La)促进氢转移使低负荷Pd催化剂选择性乙炔加氢

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Guandong Wu, Mengchen Yang, Yejiao Han, Yufei He, Dianqing Li
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引用次数: 0

摘要

钯基催化剂对乙炔的选择性加氢往往受到贵金属用量高和氢与乙炔在活性位点上竞争性吸附的限制,从而降低了催化效率。为了解决这个问题,我们开发了一种由La掺杂的Al2O3支撑的PdAg催化剂,引入了O-(La)位点,增强了氢的储存和转移。原位傅里叶变换红外光谱(FTIR)、程序升温解吸(TPD)和质谱分析表明,O-(La)位点能够有效储存解离氢,从而选择性地与乙炔反应,减少对Pd位点的竞争。密度泛函理论(DFT)计算证实,O-(La)位降低了氢迁移的能垒,增强了乙炔的加氢作用。这种创新的方法将Pd含量降低了30%,同时实现了卓越的催化性能,为工业加氢过程提供了一种经济高效且可扩展的解决方案。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

O-(La)-promoted hydrogen transfer enables low-loading Pd catalysts for selective acetylene hydrogenation

O-(La)-promoted hydrogen transfer enables low-loading Pd catalysts for selective acetylene hydrogenation
The selective hydrogenation of acetylene using Pd-based catalysts is often limited by high precious metal usage and competitive adsorption between hydrogen and acetylene on active sites, which reduces catalytic efficiency. To address this, we developed a PdAg catalyst supported on La-doped Al2O3, introducing O-(La) sites that enhance hydrogen storage and transfer. In-situ Fourier Transform Infrared Spectroscopy (FTIR), temperature-programmed desorption (TPD), and mass spectrometry analyses revealed that the O-(La) sites enable efficient storage of dissociated hydrogen, which selectively reacts with acetylene, reducing competition on Pd sites. Density Functional Theory (DFT) calculations confirmed that the O-(La) sites reduce the energy barrier for hydrogen migration and enhance acetylene hydrogenation. This innovative approach reduces the Pd content by up to 30% while achieving superior catalytic performance, offering a cost-effective and scalable solution for industrial hydrogenation processes.
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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