Role of Ce in supported Pd catalyst for oxidative carbonylation of phenol to diphenyl carbonate

WANG Zhimiao; ZHANG Hongqi; ZHOU Lichao; LI Fang; XUE Wei; WANG Yanji

doi:10.11949/0438-1157.20190395

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Role of Ce in supported Pd catalyst for oxidative carbonylation of phenol to diphenyl carbonate

Catalysis\, kinetics and reactors | 更新时间：2026-07-24

- Role of Ce in supported Pd catalyst for oxidative carbonylation of phenol to diphenyl carbonate
- CIESC Journal Vol. 70, Issue 12, Pages: 4625-4634(2019)
- 作者机构：
  
  1. 河北工业大学化工学院，河北省绿色化工与高效节能重点实验室，天津 300130
  2. 天津市本质安全化工技术重点实验室，天津 300130
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20190395
  CLC： O 643;X 511
- Received：16 April 2019，
  
  Revised：2019-08-23，
  
  Online First：09 June 2020，
  
  Published：05 December 2019
- 稿件说明：
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王志苗, 张洪起, 周立超, 李芳, 薛伟, 王延吉. Ce在负载Pd催化苯酚氧化羰基化合成碳酸二苯酯反应中的作用[J]. 化工学报, 2019, 70(12): 4625-4634

WANG Zhimiao, ZHANG Hongqi, ZHOU Lichao, LI Fang, XUE Wei, WANG Yanji. Role of Ce in supported Pd catalyst for oxidative carbonylation of phenol to diphenyl carbonate[J]. CIESC Journal, 2019, 70(12): 4625-4634
王志苗, 张洪起, 周立超, 李芳, 薛伟, 王延吉. Ce在负载Pd催化苯酚氧化羰基化合成碳酸二苯酯反应中的作用[J]. 化工学报, 2019, 70(12): 4625-4634 DOI： 10.11949/0438-1157.20190395.

WANG Zhimiao, ZHANG Hongqi, ZHOU Lichao, LI Fang, XUE Wei, WANG Yanji. Role of Ce in supported Pd catalyst for oxidative carbonylation of phenol to diphenyl carbonate[J]. CIESC Journal, 2019, 70(12): 4625-4634 DOI： 10.11949/0438-1157.20190395.

摘要

采用微乳液法制备了Ce为助剂的Pd-Ce-O/SiO

催化剂，用于苯酚氧化羰基化合成碳酸二苯酯（DPC）反应。活性评价结果显示，催化剂性能随着Ce用量的增加而提高，当Ce/Pd摩尔比为10/1时，苯酚转化率为64.4%，碳酸二苯酯选择性为83.4%。利用XRD表征发现，部分Ce

进入到PdO晶格中，使得失活Pd原子中的电子更容易向Ce转移，从而易于再生，表现出更好的催化性能。根据上述结果，设计制备了Pd-O/CeO

催化剂用于本反应，苯酚转化率和碳酸二苯酯选择性分别仅为24.0%和23.3%。表征发现，在Pd-Ce-O/SiO

催化剂表面，Pd物种主要是PdO，而Pd-O/CeO

表面的Pd物种则以PdO

为主。由于苯酚氧化羰基化反应的活性中心为Pd(Ⅱ)，所以Pd-O/CeO

催化性能较差。并且，由于Pd与CeO

之间存在强相互作用，催化剂表面Pd含量较低，这也是Pd-O/CeO

催化活性较差的原因之一。

Abstract

A Pd-Ce-O/SiO

catalyst with Ce as auxiliary was prepared by microemulsion method for oxidative carbonylation of phenol to synthesize diphenyl carbonate (DPC). The activity evaluation results showed that the catalyst performance increased with the increase of the amount of Ce. When the Ce/Pd molar ratio was 10/1

the phenol conversion rate was 64.4%

and the diphenyl carbonate selectivity was 83.4%. The XRD results showed that part of Ce

entered into PdO crystal lattice

erefore the electrons of deactivated Pd could easily be transferred to Ce. So the Pd-Ce-O/SiO

catalyst could be easily regenerated and showed better performance. According to the above mentioned results

Pd-O/CeO

was designed and prepared for oxidative carbonylation of phenol. However

unlike Pd-Ce-O/SiO

Pd-O/CeO

showed poor catalytic performance. The phenol conversion and DPC selectivity was only 24.0% and 23.3% respectively. The characterization results showed that PdO was the main species of Pd on the surface of Pd-Ce-O/SiO

but there was more PdO

on Pd-O/CeO

. Because Pd(Ⅱ) is the active site for oxidative carbonyation

Pd-O/CeO

exhibited inferior activity to Pd-Ce-O/SiO

. In addition

in Pd-O/CeO

catalyst

the surface Pd content was lower than that of other catalyst because of the strong interaction between Pd species and CeO

. That s one of the reasons for the poor activity of Pd-O/CeO

关键词

Keywords

references

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