摘要
甲烷是天然气、煤层气、页岩气和生物气的主要成分,高热值使其成为化学工业广泛使用的燃料。将甲烷选择性转化为增值化学品是一种更环保的替代途径。对于探究在温和条件下的反应环境中进行活化和催化过程,仍然面临重大难题。本文综述了分子氧作为氧化剂低温催化甲烷转化为增值化学品的研究进展。从沸石催化剂、金属有机骨架催化剂、氧化物催化剂、单原子催化剂和钯基催化剂等方面介绍了甲烷直接氧化转化为增值含氧化合物的催化剂基本原理和设计策略;并对活性中心和催化剂类别进行了详细的阐述和讨论;最后,对甲烷在温和条件下生产化学品的潜力提出了建议,强调了实现理想产品高产率所面临的挑战,并简要提出了可能的解决方案。
Methane,the primary component of natural gas,coalbed methane,shale gas,and biogas,is highly valued in the chemical industry due to its high calorific value.The selective conversion of methane into value-added chemicals presents a more environmentally friendly alternative.However,significant challenges remain in exploring activation and catalysis processes under mild reaction environments.This paper provides a comprehensive review of the research progress in the low-temperature catalytic conversion of methane into value-added chemicals,using molecular oxygen as an oxidant.It delves into the fundamental principles and design strategies of catalysts for the direct oxidation of methane into value-added oxygenates,from various aspects.These include zeolite catalysts,metal-organic frameworks catalysts,oxide catalysts,single-atom catalysts,and palladium-based catalysts.The paper also offers detailed explanations and discussions from the perspectives of active centers and types of catalysts.Finally,it suggests the potential of methane in producing chemicals under mild conditions,emphasizing the challenges of achieving high yields of desired products and proposing possible solutions briefly.
作者
王书航
周志航
张航
陈雪
赵思思
田天一
赵震
Wang Shuhang;Zhou Zhihang;Zhang Hang;Chen Xue;Zhao Sisi;Tian Tianyi;Zhao Zhen(Institute of Catalysis for Energy and Environment,College of Chemistry and Chemical Engineering,Shenyang Normal University,Shenyang,110034)
基金
国家自然科学基金项目(22102106和22109105)
辽宁省“兴辽英才计划”项目(XLYC2203120)
辽宁省高校基本科研业务费专项资金平台建设项目(LJ232410166021,LJ232410166030)
沈阳师范大学大学生创新创业项目(X202410166210)资助。
关键词
甲烷转化
低温
分子氧
C-H
键的活化
Methane conversion
Low temperature
Molecular oxygen
C-H bond activation
作者简介
联系人:张航,E-mail:zhangh@synu.edu.cn;联系人:赵思思,E-mail:zhaoss@synu.edu.cn;联系人:赵震,E-mail:zhenzhao@cup.edu.cn。
