连续性气相催化转化低浓度生物燃气制甲醇

陆志恒; 谢玄兰; 李文志

doi:doi:10.19912/j.0254-0096.tynxb.2025-0142

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连续性气相催化转化低浓度生物燃气制甲醇

更新时间：2026-07-22

- 连续性气相催化转化低浓度生物燃气制甲醇
- 连续性气相催化转化低浓度生物燃气制甲醇
- 太阳能学报 2026年47卷第4期页码：467-477
- 作者机构：
- 作者简介：
- 基金信息：
  
  安徽省自然科学基金（2408085ME143）;合肥综合性国家科学中心能源研究院重大培育项目（21KZS219）;安徽省重点研发项目（2022107020013）
- DOI：doi:10.19912/j.0254-0096.tynxb.2025-0142
  中图分类号： TQ223
- 网络首发：2026-05-08，
  
  纸质出版：2026
- 稿件说明：
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陆志恒, 谢玄兰, 李文志. 连续性气相催化转化低浓度生物燃气制甲醇[J]. 太阳能学报, 2026,47(4):467-477.

陆志恒, 谢玄兰, 李文志. 连续性气相催化转化低浓度生物燃气制甲醇[J]. 2026, 47(4): 467-477.
陆志恒, 谢玄兰, 李文志. 连续性气相催化转化低浓度生物燃气制甲醇[J]. 太阳能学报, 2026,47(4):467-477. DOI： doi:10.19912/j.0254-0096.tynxb.2025-0142.

陆志恒, 谢玄兰, 李文志. 连续性气相催化转化低浓度生物燃气制甲醇[J]. 2026, 47(4): 467-477. DOI： doi:10.19912/j.0254-0096.tynxb.2025-0142.

摘要

采用浸渍法制备一系列铜基沸石催化剂（xCu/MOR）

并在以水为氧化剂的连续性气相条件下开展催化生物燃气部分氧化制甲醇性能研究。结果表明

350 ℃条件下

甲醇产率随着铜负载量的增加呈火山型趋势

其中2Cu/MOR催化剂可实现67.3 μmol/（g·h）的高甲醇产率;进一步优化反应温度

2Cu/MOR催化剂在400 ℃反应条件下甲醇产率高达142.5 μmol/（g·h）。此外

使用X射线衍射、高分辨透射电子显微镜、X射线光电子能谱、紫外-漫反射可见光谱、甲烷程序升温脱附及傅里叶变换红外光谱技术进行催化剂表征分析

结果表明铜基沸石催化剂中铜元素分散均匀

表现出优异活性的2Cu/MOR催化剂有更多的孤立二价铜活性位点

反应过程中甲烷在孤立二价铜位点上吸附活化

形成的甲氧基中间体与水解离产生的羟基反应生成甲醇。

Abstract

A series of copper-based zeolite catalysts （Cu/MOR） were prepared by impregnation method

and the performance of catalytic partial oxidation of biogas to methanol was investigated under continuous gas-phase conditions with water as oxidant. The results show that the methanol yield at 350 ℃ shows a volcano trend with the increase of copper loading

in which the 2Cu/MOR catalyst can achieve a high methanol yield of 67.3 μmol/（g·h）; further optimization of the reaction temperature results in a high methanol yield of up to 142.5 μmol/（g·h） for the 2Cu/MOR catalyst at 400 ℃. In addition

catalyst characterization using X-ray diffraction

high-resolution transmission electron microscopy

X-ray photoelectron spectroscopy

UV-diffuse reflectance visible spectroscopy

methane programmed warming desorption

and Fourier transform infrared spectroscopy show that the copper element in the copper-based zeolite catalysts is uniformly dispersed

and the 2Cu/MOR catalysts that demonstrated excellent activity have more isolated divalent copper active species. During the reaction process

methane is adsorbed and activated on the isolated divalent copper sites

and the formed methoxy intermediate reactes with the hydroxyl group produced by hydrolysis to form methanol.

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