Characterization and catalytic performance of Cu<sup>Ⅰ</sup>/solid acids catalysts in oxidative carbonylation of methanol

LI Zhong; LIU Yuanyuan; ZHENG Huayan; HUANG Haibin; YIN Lihua

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Characterization and catalytic performance of Cu^Ⅰ/solid acids catalysts in oxidative carbonylation of methanol

更新时间：2025-12-10

- Characterization and catalytic performance of Cu^Ⅰ/solid acids catalysts in oxidative carbonylation of methanol
- CIESC Journal Issue 6, Pages: 1443-1449(2010)
- 作者机构：
  
  太原理工大学煤科学与技术教育部和山西省重点实验室
- 作者简介：
- 基金信息：
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- Online First：05 June 2010，
  
  Published：05 June 2010
- 稿件说明：
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LI Zhong, LIU Yuanyuan, ZHENG Huayan, et al. Characterization and catalytic performance of Cu^Ⅰ/solid acids catalysts in oxidative carbonylation of methanol[J]. CIESC Journal, 2010, (6): 1443-1449.
DOI：

LI Zhong, LIU Yuanyuan, ZHENG Huayan, et al. Characterization and catalytic performance of Cu^Ⅰ/solid acids catalysts in oxidative carbonylation of methanol[J]. CIESC Journal, 2010, (6): 1443-1449. DOI：

摘要

采用稀H2SO4和(NH4)2S2O8溶液浸渍Fe(OH)3，高温焙烧制得SO2-4/Fe2O3和S2O 2-8/Fe2O3固体酸，然后与CuCl 混合高温处理制备CuⅠ/SO 2-4/Fe2O3和CuI/S2O2-8/Fe2O3催化剂。该催化剂在CH3OH液相氧化羰基化合成碳酸二甲酯(DMC)反应中表现出良好的催化活性，明显高于传统CuCl催化剂。载体和催化剂的XRD、NH3-TPD和XPS等表征结果表明，制备的SO2-4/Fe2O3和S2O 2-8/Fe2O3固体酸为超强酸，与CuCl混合高温处理中发生了固体离子交换，形成了负载CuⅠ的低氯催化剂。固体酸载体酸量越多，离子交换负载的CuⅠ离子的含量越高，催化活性越好。550℃焙烧制备S2O2-8/Fe2O3固体酸有较多的酸量，与CuCl热处理获得的CuⅠ/S2O2-8/Fe2O3催化剂具有较好的催化活性，CH3OH转化率达到16.58%，DMC选择性和时空收率分别为97.00%和2.83 g·g-1·h-1，且Cu/Cl原子比达到1.69。

Abstract

Two solid acids SO 2-4/ Fe2O3 and S2O2-8/Fe2O3 were prepared by impregnation of Fe(OH)3 in the solution of H2SO4 and (NH4)2S2O8， and calcination

then mixed with CuCl to obtain CuⅠ/SO 2-4/Fe2O3 and CuⅠ/S2O2-8/Fe2O3 catalysts by heat treatment at high temperature under N2 flow.They were of more active than the commercial catalysts CuCl for oxidative carbonylation of methanol to dimethyl carbonate (DMC).One of the main factors affecting activity of CuI/SO 2-4/Fe2O3 and CuⅠ/S2O2-8/Fe2O3 catalysts was calcined temperature of SO 2-4/ Fe2O3 and S2O2-8/Fe2O3 solid acid.The results indicated that the catalyst prepared with SO2-4/Fe2O3 and S2O2-8/Fe2O3 solid acid calcined at 550℃ showed the excellent catalytic activity.By the characterization with XRD

NH3-TPD and XPS techniques

it was found that SO2-4/Fe2O3 and S2O2-8/Fe2O3 were solid superacids

and ion-exchange was carried out between Brnsted acid site H+ on SO2-4/Fe2O3 and S2O2-8/Fe2O3 with Cu+ on CuCl during heat treatment which led to the formation of low chlorine CuⅠ catalyst.It was also found that structure of these solid acids had no obvious change if the loading of CuⅠ was at mass ratio of WCuCl/Wcarrier≤1∶2.The more acidity of solid acid carrier

the more CuⅠ loaded

and the higher activity of catalyst.The acid sites was much more for S2O2-8/Fe2O3 calcined at 550℃

and there was of high Cu/Cl of 1.69 and excellent catalytic activity for CuⅠ/S2O2-8/Fe2O3 catalyst.Its conversion of methanol

DMC selectivity and space-time yields were 16.58%

97.00% and 2.83 g·g-1·h-1 respectively.

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Characterization and catalytic performance of CuⅠ/solid acids catalysts in oxidative carbonylation of methanol

DOI：

摘要

Abstract

关键词

Keywords

references

Characterization and catalytic performance of Cu^Ⅰ/solid acids catalysts in oxidative carbonylation of methanol