光催化甲烷直接转化制甲醇提高甲烷转化率和甲醇选择性  

Photocatalytic Methane Oxidation to Methanol in Promoting Methane Conversion Rate and Methanol Selectivity

作　　者：韩春秋 曹玥晗 黄川 吕伟峰 周莹[1,2] Chunqiu Han;Yuehan Cao;Chuan Huang;Weifeng Lv;Ying Zhou(National Key Laboratory of Oil and Gas Reservoir Geology and Exploitation,Southwest Petroleum University,Chengdu 610500,China;School of New Energy and Materials,Southwest Petroleum University,Chengdu 610500,China)

机构地区：[1]西南石油大学,油气藏地质及开发工程全国重点实验室,成都610500 [2]西南石油大学,新能源与材料学院,成都610500

出　　处：《化学进展》2024年第6期867-877,共11页Progress in Chemistry

基　　金：国家自然科学基金项目(No.22209135、52325401、22209136);中国博士后科学基金(No.2022M722635);四川省博士后创新人才支持项目(BX202220)资助。

摘　　要：光催化甲烷(CH_(4))直接转化制甲醇(CH_(3)OH)为化学储能和高值化学品的合成提供了一种有效途径。然而,由于CH_(4)分子活化困难,且CH_(3)OH较CH_(4)更活泼,更容易发生过氧化反应,导致CH_(4)的转化率较低,CH_(3)OH的选择性也较低。因此,选择性光催化CH_(4)直接转化制CH_(3)OH仍面临巨大挑战。本文综述了近年来在光催化CH_(4)直接转化制CH_(3)OH研究中提高CH_(4)转化率和CH_(3)OH选择性的研究思路,以及相应的催化剂设计策略。在提高CH_(4)转化率方面,主要是通过改善活性氧自由基活化或催化活化路径有效活化CH_(4)。在提高CH_(3)OH选择性方面,主要为抑制CH_(3)OH的过氧化或实现CH_(3)OH再生。为了提高CH_(4)的转化率和CH_(3)OH的选择性,催化设计策略主要为负载助催化剂、调控催化材料的尺寸和构造氧空位等。最后,本综述对光催化CH_(4)直接转化制CH_(3)OH的未来研究方向提出了展望。Photocatalytic direct conversion of methane(CH_(4))to methanol(CH_(3)OH)provides an effective way for efficient energy storage and the synthesis of high-value chemicals.However,due to the difficulty in activating CH_(4)molecules and the fact that CH_(3)OH is more reactive than CH_(4)and prone to peroxidation,the conversion rate of CH_(4)is low,and the selectivity of CH_(3)OH is low as well.Therefore,the selective photocatalytic direct conversion of CH_(4)to CH_(3)OH still faces significant challenges.This review focuses on the research ideas on promoting CH_(4)conversion rate and CH_(3)OH selectivity in recent years in the direct conversion of photocatalytic CH_(4)to CH_(3)OH,as well as the corresponding catalyst design strategies.In terms of promoting the CH_(4)conversion rate,the main research idea is to effectively activate CH_(4)by improving reactive oxygen radical activation or catalytic activation pathways.In terms of promoting CH_(3)OH selectivity,the main idea is to inhibit the peroxidation of CH_(3)OH or achieve CH_(3)OH regeneration.In order to improve the conversion rate of CH_(4)and the selectivity of CH_(3)OH,catalytic design strategies mainly include loading cocatalysts,controlling the size of catalytic materials and constructing oxygen vacancies.Finally,this review provides an outlook on the future research direction of photocatalytic direct conversion of CH_(4)to CH_(3)OH.

关 键 词：光催化 甲烷转化 甲醇 促进C—H键活化 抑制甲醇过氧化 

分 类 号：O643.3[理学—物理化学] O622.3[理学—化学]