Theoretical calculation study on effects of OV and H2O on CO2 hydrogenation over Pd2/CeO2

ZHANG Dongjian; ZHA Yajun; LIU Bing; LIU Xiaohao

doi:10.12434/j.issn.2097-2547.20250044

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Theoretical calculation study on effects of O_V and H₂O on CO₂ hydrogenation over Pd₂/CeO₂

更新时间：2025-05-29

- Theoretical calculation study on effects of O_V and H₂O on CO₂ hydrogenation over Pd₂/CeO₂
- Vol. 50, Issue 5, Pages: 11-17(2025)
- 作者机构：
  
  江南大学化学与材料工程学院，江苏无锡 214122
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20250044
  CLC： TQ426.8
- Received：27 January 2025，
  
  Revised：12 March 2025，
  
  Published：25 May 2025
- 稿件说明：
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张东健,查雅君,刘冰等.Pd₂/CeO₂上O_V和H₂O对催化CO₂加氢反应影响的理论计算研究[J].低碳化学与化工,2025,50(5):11-17.

ZHANG Dongjian,ZHA Yajun,LIU Bing,et al.Theoretical calculation study on effects of O_V and H₂O on CO₂ hydrogenation over Pd₂/CeO₂[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(5):11-17.
张东健,查雅君,刘冰等.Pd₂/CeO₂上O_V和H₂O对催化CO₂加氢反应影响的理论计算研究[J].低碳化学与化工,2025,50(5):11-17. DOI： 10.12434/j.issn.2097-2547.20250044.

ZHANG Dongjian,ZHA Yajun,LIU Bing,et al.Theoretical calculation study on effects of O_V and H₂O on CO₂ hydrogenation over Pd₂/CeO₂[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(5):11-17. DOI： 10.12434/j.issn.2097-2547.20250044.

摘要

加氢生成乙醇及其他高级产物是实现CO

资源化利用的重要途径之一。Pd

/CeO

催化剂是CO

加氢制乙醇的理想催化剂之一。利用模拟方法可以更直观的表征其反应过程。采用密度泛函理论（DFT）计算方法，研究分析了氧空位（O

）和H

O对Pd

/CeO

催化剂上CO

加氢反应过程的影响。结果表明，相较于洁净催化剂表面，O

促进了CO

吸附和活化。此外，O

还改变了载体与负载Pd之间的电子状态，使得Pd能够向C物种提供更多电子，有利于后续C—O键断裂及C—C键偶联反应进行。然而，当催化剂表面存在H

O时，由于O物种的电负性较高，会与CO

及其衍生物种产生电子竞争，导致C物种电子密度降低，不利于C—O键解离及C—C键偶联，从而提高了生成乙醇的反应能垒。

Abstract

hydrogenation to produce ethanol and other advanced products is one of the important ways to realize the resource utilization of CO

. Pd

/CeO

catalyst is one of the ideal catalysts for CO

hydrogenation to ethanol. The simulation methods can provide a more intuitive representation of the reaction process. The influence o

f oxygen vacancy (O

) and H

O on the CO

hydrogenation process on Pd

/CeO

catalyst was studied and analyzed by density functional theory (DFT). The results show that compared to clean catalyst surfaces

promotes CO

adsorption and activation. In addition

also changes the electronic state between the support and the supported Pd

allowing Pd to provide more electrons to the C species

which is beneficial for subsequent C—O bond cleavage and C—C bond coupling reactions. However

when H

O is present on the surface of the catalyst

due to the high electronegativity of O species and H

O competes with CO

and its derivatives for electrons

resulting in a decrease in the electron density of C species

which is not conducive to the cleavage of C—O bonds and the coupling of C—C bonds

thereby increasing the reaction energy barriers for ethanol generation.

关键词

Keywords

references

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Related Institution

School of Chemistry and Chemical Engineering, Shihezi University

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