催化学报 ›› 2019, Vol. 40 ›› Issue (s1): 129-142.

• 综述 • 上一篇    下一篇

催化选择氧化领域近年研究进展、挑战与展望

谢顺吉, 王野   

  1. 厦门大学, 化学化工学院, 固体表面物理化学国家重点实验室, 能源材料化学协同创新中心, 醇醚酯化工清洁生产国家工程实验室, 福建 厦门 361005
  • 出版日期:2019-12-17 发布日期:2019-10-10
  • 通讯作者: 王野
  • 基金资助:
    国家自然科学基金(21690082,21503176).

Recent Advances, Challenges and Perspectives in Selective Oxidation Catalysis

XIE Shunji, WANG Ye   

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China
  • Online:2019-12-17 Published:2019-10-10
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21690082, 21503176).

摘要: 选择氧化是一类重要化学反应,在当今化学工业过程中占据极其重要的地位.近年来随着资源供给形势变化、可持续发展和绿色化学等的要求,追求100%高选择性以减少CO2排放、以廉价丰富或可再生资源取代耗竭型资源、以空气/氧气/过氧化氢等取代有机过氧化物氧化剂、以水取代有机溶剂等方面的研究已发展成为选择氧化催化研究领域的主要趋势.甲烷等低碳烷烃选择氧化、丙烯环氧化和苯选择氧化制苯酚是该领域最具挑战性的难题.生物质基化合物分子中特定官能团选择氧化是该领域的新生长方向,引入光催化和电催化构建选择氧化新体系为该领域带来新机遇.本文针对低碳烷烃选择氧化、烯烃环氧化、苯制苯酚和生物质基分子制有机酸等几类重要选择氧化反应,挂一漏万梳理了国内外近年的重要研究进展,探究了影响反应活性/选择性的关键因素,以及与催化活性位和反应机理相关的一些关键催化基础科学问题,分析并展望了催化选择氧化领域涌现的新方法、新材料以及未来发展方向.

关键词: 多相催化, 选择氧化, 低碳烷烃氧化, 烯烃环氧化, 苯制苯酚, 生物质选择氧化

Abstract: Selective oxidation is an important type of chemical reactions and is playing vital roles in the chemical industry. Following the changing trend in resources and the requirements from sustainable and green chemistry, the pursuit of 100% selectivity to abate CO2 emission, the substitution of deplete resources with abundant or renewable ones, the use of air/O2/H2O2 as an oxidant instead of organic peroxides and the use of H2O to replace organic solvents have become major research directions in selective oxidation catalysis. The selective oxidation of methane and other alkanes, the epoxidation of propylene and the oxidation of benzene to phenol remain as the most challenging subjects in selective oxidation catalysis. The selective oxidation of specific functional groups in biomass-derived molecules has become a new growing research direction. The harnessing of photocatalysis and electrocatalysis has offered new opportunities for selective oxidation catalysis. This article highlights recent advances in selective oxidation of lower alkanes, in particular methane, epoxidation of propylene, benzene to phenol and selective oxidation of biomass-derived molecules. The key factors that control the catalytic activity and selectivity, and the fundamental issues related to active sites and reaction mechanisms for selective oxidation are discussed. This present article also touches new catalytic materials and methods for selective oxidation, and provides perspectives for future studies in the area.

Key words: heterogeneous catalysis, selective oxidation, lower alkane oxidation, epoxidation of olefin, benzene to phenol, selective oxidation of biomass