不同酸强度HY分子筛对正己烷裂解机理影响的理论研究

卫丽莎; 王慧; 董奇; 李永旺; 相宏伟

doi:10.12434/j.issn.2097-2547.20240391

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不同酸强度HY分子筛对正己烷裂解机理影响的理论研究

低碳分子转化合成 | 更新时间：2025-06-23

- 不同酸强度HY分子筛对正己烷裂解机理影响的理论研究
- Theoretical study on effects of HY zeolites with different acid strengths on cracking mechanism of n-hexane
- 低碳化学与化工 2025, 50(6): 52-62.
- 作者机构：
  
  1.中国科学院山西煤炭化学研究所煤炭高效低碳利用全国重点实验室，山西太原 030001
  2.中国科学院大学，北京 100049
  3.中科合成油技术股份有限公司，北京 101407
  4.太原理工大学化学工程与技术学院，山西太原 030024
- 作者简介：
  
  卫丽莎（1995—），博士研究生，研究方向为分子筛催化， E-mail：weilisha18@mails.ucas.ac.cn。
  相宏伟（1964—），博士，研究员，研究方向为多相催化，E-mail：hwxiang@sxicc.ac.cn。
- 基金信息：
  
  国家重点研发计划(2022YFB4101201);中国科学院先导专项(XDA29030700)
- DOI：10.12434/j.issn.2097-2547.20240391
  中图分类号： TQ426;O643.32+2;
- 收稿日期：2024-09-17，
  
  修回日期：2024-10-09，
  
  纸质出版日期：2025-06-25
- 稿件说明：
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卫丽莎,王慧,董奇等.不同酸强度HY分子筛对正己烷裂解机理影响的理论研究[J].低碳化学与化工,2025,50(06):52-62.

WEI Lisha,WHANG Hui,DONG Qi,et al.Theoretical study on effects of HY zeolites with different acid strengths on cracking mechanism of n-hexane[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(06):52-62.
卫丽莎,王慧,董奇等.不同酸强度HY分子筛对正己烷裂解机理影响的理论研究[J].低碳化学与化工,2025,50(06):52-62. DOI： 10.12434/j.issn.2097-2547.20240391.

WEI Lisha,WHANG Hui,DONG Qi,et al.Theoretical study on effects of HY zeolites with different acid strengths on cracking mechanism of n-hexane[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(06):52-62. DOI： 10.12434/j.issn.2097-2547.20240391.

摘要

能源需求增长与化石燃料枯竭促使重质原油的高效转化成为研究重点，烷烃裂解技术可将长链烷烃转化为短链烃产物，从而提升长链烷烃的经济价值。HY分子筛因具有比表面积较高和酸强度较适宜的优点，是目前常用的烷烃催化裂解催化剂之一，但HY分子筛酸强度对烷烃裂解机理影响的理论研究还比较少。采用周期密度泛函理论计算方法，以丙烷和正己烷为模型底物，研究了不同酸强度（Al取代结构分别为1Al取代、3Al取代和6Al取代，相应

(Si)/

(Al)分别为47、15和7）的HY分子筛对烷烃裂解机理的影响，并分析了正己烷中不同C—C键断裂的难易程度。结果表明，随着HY分子筛Brønsted酸强度增强，丙烷和正己烷质子化反应的表观吉布斯自由能垒降低，HY分子筛的烷烃裂解反应催化活性增强。正己烷中3种C—C键的断裂难度由易到难分别为C

—C

键、C

—C

键和C

—C

键。

Abstract

Growth of energy demand and depletion of fossil fuels have made efficient conversion of heavy crude oil a research focus. Alkane cracking technology can convert long-chain alkanes into short-chain hydrocarbon products

thereby increasing the economic value of long-chain alkanes. HY zeolites are one of the commonly used catalysts for alkane catalytic cracking due to their advantages of high specific surface area and suitable acid strength. However

there are relatively few theoretical studies on the effect of HY zeolites acid strengths on alkane cracking mechanism. Using periodic density functional theory calculation method

with propane and

-hexane as model substrates

the effects of HY zeolites with different acid strengths (Al substitution structures are 1Al substitution

3Al substitution and 6Al substitution

and the corresponding

(Si)/

(Al) are 47

15 and 7

respectively) on the alkane cracking mechanism were

systematically studied

and the difficulty of breaking different C—C bonds in

-hexane was analyzed. The results show that with the increase of the Brønsted acid strength of HY zeolites

the apparent Gibbs free energy barrier of the protonation reaction of propane and

-hexane decreases

and the catalytic activity of HY zeolites in alkane cracking reaction is enhanced. The difficulty of breaking the three C—C bonds in

-hexane from easy to difficult are C

—C

bond

—C

bond and C

—C

bond.

关键词

Keywords

references

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