Ni/Al2O3-CeO2催化剂上乙烷干重整反应本征动力学研究

郭冰洋; 杜春丽; 范志辉; 杨旭港; 张艺; 闫龙飞; 张振洲; 涂维峰

doi:10.12434/j.issn.2097-2547.20240298

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Ni/Al₂O₃-CeO₂催化剂上乙烷干重整反应本征动力学研究

低碳分子转化合成 | 更新时间：2025-03-27

- Ni/Al₂O₃-CeO₂催化剂上乙烷干重整反应本征动力学研究
- Study on intrinsic kinetics of ethane dry reforming reaction on Ni/Al₂O₃-CeO₂ catalysts
- 低碳化学与化工 2025, 50(3): 39-46.
- 作者机构：
  
  郑州大学化工学院，河南郑州 450001
- 作者简介：
  
  郭冰洋（1998—），硕士研究生，研究方向为催化反应动力学，E-mail：2356679381@qq.com。
  张振洲（1987—），博士，副教授，研究方向为CO2资源化利用，E-mail：zhangzhenzhou@zzu.edu.cn；
  涂维峰（1986—），博士，教授，研究方向为CO2资源化利用，E-mail：weifengtu@zzu.edu.cn。
- 基金信息：
  
  国家自然科学基金面上项目(22278379);河南省科技研发计划联合基金(222301420010)
- DOI：10.12434/j.issn.2097-2547.20240298
  中图分类号： TQ032
- 收稿日期：2024-07-15，
  
  修回日期：2024-09-11，
  
  纸质出版日期：2025-03-25
- 稿件说明：
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郭冰洋,杜春丽,范志辉等.Ni/Al₂O₃-CeO₂催化剂上乙烷干重整反应本征动力学研究[J].低碳化学与化工,2025,50(03):39-46.

GUO Bingyang,DU Chunli,FAN Zhihui,et al.Study on intrinsic kinetics of ethane dry reforming reaction on Ni/Al₂O₃-CeO₂ catalysts[J].Low-carbon Chemistry and Chemical Engineering,2025,50(03):39-46.
郭冰洋,杜春丽,范志辉等.Ni/Al₂O₃-CeO₂催化剂上乙烷干重整反应本征动力学研究[J].低碳化学与化工,2025,50(03):39-46. DOI： 10.12434/j.issn.2097-2547.20240298.

GUO Bingyang,DU Chunli,FAN Zhihui,et al.Study on intrinsic kinetics of ethane dry reforming reaction on Ni/Al₂O₃-CeO₂ catalysts[J].Low-carbon Chemistry and Chemical Engineering,2025,50(03):39-46. DOI： 10.12434/j.issn.2097-2547.20240298.

摘要

乙烷干重整反应是实现CO

利用的重要途径之一。Ni基催化剂因具有低成本和高催化活性等特点被广泛用于乙烷干重整反应。然而，乙烷干重整反应机理仍不明晰，这制约了高效Ni基催化剂的开发。采用溶胶凝胶法制备了Ni质量分数分别为5%和10%的Ni基催化剂（5%Ni/Al

-CeO

和10%Ni/Al

-CeO

），通过本征动力学方法分析了反应物分压（

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366010&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76365986&type=

5.92666674

和

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76365972&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366013&type=

5.16466665

）和产物分压（

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366019&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366015&type=

3.97933316

和

）对相关反应的影响，研究了反应温度、Ni团簇平均粒径对乙烷干重整反应过程中乙烷活化的影响。结果表明，在温度为823 K、常压、

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366001&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366002&type=

5.92666674

为0.1~7.0 kPa、

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366023&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366049&type=

5.16466665

为2.0~20.0 kPa和空速为6.9 × 10

mL/(g·h)下，催化剂上乙烷正向转化速率与

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366065&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366066&type=

5.92666674

线性相关，且不受

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366023&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366049&type=

5.16466665

、

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366019&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366015&type=

3.97933316

和

的影响；在本征动力学区间内，乙烷重整反应速率的速率控制步骤为乙烷活化，活化能为(108 ± 10) kJ/mol。在温度为823 K、常压和空速为6.9 × 10

mL/(g·h)下，Ni团簇平均粒径为6.5 nm的5%Ni/Al

-CeO

具有较高的乙烷活化速率（(7.26 ± 0.80) mol/(mol·min·kPa)）。

Abstract

Ethane dry reforming is one of the important ways to realize CO

utilization. Ni-based catalysts are widely used in ethane dry reforming reactions due to their characteristics of low costs and high catalytic activities. However

the mechanism of ethane dry reforming is still unclear

which restricts the development of high-efficienct Ni-based catalysts. Using the sol-gel method

Ni-based catalysts with nickel mass fractions of 5% and 10% (5%Ni/Al

-CeO

and 10%Ni/Al

-CeO

)

respectively

were prepared. The effects of the reactants partial pressures (

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366052&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366043&type=

6.01133299

and

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366044&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366054&type=

5.24933338

) and the products partial pressures (

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366070&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366056&type=

3.97933316

and

) on the related reactions were analyzed by intrinsic kinetic method. The influences of reaction

temperatures and Ni clusters average particle sizes on the activation of ethane during ethane dry reforming were studied. The results show that at temperature of 823 K

atmospheric pressure

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366057&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366078&type=

6.01133299

of 0.1 kPa to 0.7 kPa

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366058&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366079&type=

5.24933338

of 2.0 kPa to 20.0 kPa and space velocity of 6.9 × 10

mL/(g·h)

the forward rate of ethane conversion increases linearly with

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366059&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366080&type=

6.01133299

while independent with

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366058&type=

3.30200005

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=76366079&type=

5.24933338

and

over the catalysts. In the intrinsic kinetic interval

the rate-controlled step of the ethane dry reforming reaction rate is ethane activation

and the activation energy is (108 ± 10) kJ/mol. At temperature of 823 K

atmospheric pressure and space velocity of 6.9 × 10

mL/(g·h)

5%Ni/Al

-CeO

with Ni clusters average particle sizes of 6.5 nm exhibits relative high ethane activation rate

which is (7.26 ± 0.

80) mol/(mol·min·kPa).

关键词

Keywords

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