化工进展 ›› 2021, Vol. 40 ›› Issue (12): 6714-6720.DOI: 10.16085/j.issn.1000-6613.2021-0083

• 工业催化 • 上一篇    下一篇

非平衡负离子与ZnO-ZrO2固溶体协同催化CO2与H2O反应制甲醇

徐瑞(), 杨凡, 贾显枝, 刘璐, 赵彬然, 马晓迅()   

  1. 西北大学化工学院,陕西 西安 710069
  • 收稿日期:2021-01-13 修回日期:2021-03-20 出版日期:2021-12-05 发布日期:2021-12-21
  • 通讯作者: 马晓迅
  • 作者简介:徐瑞(1994—),男,硕士研究生,研究方向为非平衡负离子方法转化CO2。E-mail:1033407675@qq.com
  • 基金资助:
    国家自然科学基金(21536009);陕西省重点研发计划(2020ZDLGY11-06);陕西省科技计划(2017ZDCXL-GY-10-03)

Preparation of methanol from CO2 and H2O catalyzed by non-equilibrium anion and ZnO-ZrO2 solid solution

XU Rui(), YANG Fan, JIA Xianzhi, LIU Lu, ZHAO Binran, MA Xiaoxun()   

  1. School of Chemical Engineering, Northwest University, Xi’an 710069, Shaanxi, China
  • Received:2021-01-13 Revised:2021-03-20 Online:2021-12-05 Published:2021-12-21
  • Contact: MA Xiaoxun

摘要:

近年,CO2加氢制甲醇技术初步克服了催化剂选择性低和稳定性差的难题,实现了工业化生产。然而作为氢源,氢气的廉价替代品却极少被报道。本文利用二元金属氧化物ZnO-ZrO2固溶体作为催化剂,在负电晕等离子体的辅助下将CO2和水蒸气转化为甲醇。结果表明,甲醇产量达到33.56μmol/h,是单独等离子体和单独催化剂条件下甲醇产量之和的1.4倍,催化剂与等离子体联用产生协同性。甲醇产量随反应电流和水蒸气流量的增大而增大,随CO2流量的增加而降低。X射线衍射(XRD)、X射线光电子能谱分析(XPS)和CO2-程序升温脱附(CO2-TPD)表征发现,催化剂在负电晕等离子体反应条件下晶面间距增大,氧空位增多,这增强了催化剂的CO2吸附性能。CO2-漫反射傅里叶红外光谱(CO2-DRIFTs)分析结果表明,负电晕等离子体处理后的催化剂反应过程中会产生羧酸盐(COO-),是形成甲醇的主要中间物种。

关键词: 二氧化碳, 等离子体, 催化剂, 甲醇, 协同作用,

Abstract:

CO2 and water vapor was converted into methanol with the catalyst of ZnO-ZrO2 solid solution and the aid of negative corona plasma, which provided synergistic effect when employed together. The yield of methanol was 33.56μmol/h, which was 1.4 times of the sum of those under plasma alone and catalyst alone. The methanol yield increased with the increase of reaction current and steam flow rate, but decreased with the increase of CO2 flow rate. The results of XRD, XPS and CO2-TPD showed that the crystal plane spacing and oxygen vacancies of the catalyst increased under negative corona plasma condition, which enhanced the CO2 adsorption on the catalyst. The CO2-DRIFTs results showed that carboxylate (COO-) was the main intermediate species during the methanol formation.

Key words: carbon dioxide, plasma, catalyst, methanol, synergy, alcohol

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