Comparative study on transition metal promoted Pt/SiO2 for oxidative dehydrogenation of propane with carbon dioxide

IF 7.2 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of CO2 Utilization Pub Date : 2025-05-17 DOI:10.1016/j.jcou.2025.103116

Heng-Bo Zhang, Guo-Qing Yang, Jiageng Li, Zhong-Wen Liu

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引用次数: 0

Abstract

Transition metal is quantitatively investigated as a promoter of Pt-supported catalysts for the oxidative dehydrogenation of propane with CO₂ (CO₂-ODP). However, the criteria for selecting the transition metal are largely from trial and error. In this work, Pt/SiO₂ catalysts promoted with 3d transition metals (TMs) of Mn, Fe, Co or Ni (PtTM/SiO₂) are comparatively studied for CO₂-ODP. We found that the C₃H₆ selectivity and conversions of propane and CO₂ are clearly improved when TMs are introduced into Pt/SiO₂. Moreover, the apparent activation energy for the C₃H₆ formation during CO₂-ODP is decreased in the order of PtNi/SiO₂ > PtCo/SiO₂ > PtFe/SiO₂ > PtMn/SiO₂. Among the investigated catalysts, PtMn/SiO₂ is the most active and selective catalyst for the activation of C-H bonds in propane to produce C₃H₆ while PtNi/SiO₂ is the most favorable catalyst for the formation of by-products via the dry reforming of propane with CO₂ and propane cracking. Essentially, the catalytic results are well explained as the increased electron density of Pt over the PtTM/SiO₂ catalysts via the enhanced electron transfer from TM having a smaller electronegativity. This understanding is important for the rational design of a high-performance Pt-based bimetallic catalyst for CO₂-ODP.

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过渡金属促进Pt/SiO2丙烷与二氧化碳氧化脱氢的比较研究

本文定量研究了过渡金属作为铂负载型丙烷氧化脱氢催化剂（CO2- odp）的促进剂。然而，选择过渡金属的标准主要来自试验和错误。本文比较研究了Mn、Fe、Co或Ni三维过渡金属（PtTM/SiO2）对Pt/SiO2催化剂CO2-ODP的促进作用。我们发现，在Pt/SiO2中引入TMs后，C3H6的选择性和丙烷和CO2的转化率明显提高。CO2-ODP过程中C3H6生成的表观活化能依次为PtNi/SiO2 >； PtCo/SiO2 >； PtFe/SiO2 >； PtMn/SiO2。在所研究的催化剂中，PtMn/SiO2是丙烷中C-H键活化生成C3H6的活性和选择性最强的催化剂，而PtNi/SiO2是丙烷与CO2干重整和丙烷裂解生成副产物的最有利催化剂。从本质上讲，催化结果可以很好地解释为Pt在PtTM/SiO2催化剂上的电子密度增加，这是通过电负性较小的TM增强的电子转移来实现的。这一认识对于合理设计高性能pt基CO2-ODP双金属催化剂具有重要意义。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of CO2 Utilization CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL

CiteScore

13.90

自引率

10.40%

发文量

406

审稿时长

2.8 months

期刊介绍： The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials. The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications. The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.