基于金属氧化物的光催化甲烷转化：原理、进展与挑战

doi:10.3969/j.issn.0253-2778.2020.11.001

中国科学技术大学学报 ›› 2020, Vol. 50 ›› Issue (11): 1361-1382.DOI: 10.3969/j.issn.0253-2778.2020.11.001

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基于金属氧化物的光催化甲烷转化：原理、进展与挑战

江文斌，刘敬祥，邱畅，龙冉，熊宇杰

1.中国科学技术大学合肥微尺度物质科学国家研究中心，能源材料化学协同创新中心，化学与材料科学学院，国家同步辐射实验室，安徽合肥 230026；<br>2.合肥综合国家科学中心能源实验室，安徽合肥 230031

收稿日期:2020-10-23 修回日期:2020-11-11 出版日期:2020-11-30 发布日期:2021-01-07

Photocatalytic methane conversion over metal oxides: Fundamentals, achievements, and challenges

Jiang Wenbin, Low Jingxiang, Qiu Chang, Long Ran, Xiong Yujie

1. Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China;<br>2. Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China<br>*Corresponding author: longran@ustc.edu.cn; yjxiong@ustc.edu.cn

Received:2020-10-23 Revised:2020-11-11 Online:2020-11-30 Published:2021-01-07
About author:Jiang Wenbin is currently a graduate student under the tutelage of Prof. Xiong Yujie at University of Science and Technology of China. His research interests focus on controlled synthesis of metal-oxide hybrid nanostructures for catalytic applications and mechanistic investigations. E-mail: jiangwb@mail.ustc.edu.cn

Low Jingxiang obtained his Ph.D. degree from Wuhan University of Technology in 2018, and is currently a postdoctoral fellow at University of Science and Technology of China. His research interests focus on photocatalyst design for carbon dioxide reduction, nitrogen fixation and methane conversion.

Qiu Chang is currently a senior student majoring in materials chemistry at University of Science and Technology of China. Her current research interest is photocatalysis for methane conversion.

Long Ran (corresponding author) is an associate professor at University of Science and Technology of China (USTC). She received her B.S. degree in Chemistry in 2009 and Ph.D. degree in Inorganic Chemistry under the tutelage of Prof. Xiong Yujie in 2014, both from USTC. Her research interests focus on controlled synthesis and catalytic applications of metal nanocrystals. So far, she has published more than 70 SCI papers in international high-level academic journals including J. Am. Chem. Soc., Angew. Chem. Int. Ed., Adv. Mater., Chem. Soc. Rev., Nano Energy and Small.

Xiong Yujie (corresponding author) is the Cheung Kong Chair Professor of Chemistry at University of Science and Technology of China (USTC). He received his B.S. degree in Chemical Physics in 2000 and Ph.D. degree in Inorganic Chemistry in 2004, both from USTC. From 2004 to 2009, he worked as a Postdoctoral Fellow at University of Washington in Seattle and as a Research Associate at University of Illinois at Urbana-Champaign, respectively. He was the Principal Scientist of the National Nanotechnology Infrastructure Network (NSF-NNIN) site at Washington University in St. Louis in 2009～2011, and joined the USTC faculty as a Professor of Chemistry in 2011. His research centers on solar-driven artificial carbon cycle. He has published more than 200 scientific papers with over 25000 total citations (H-index 77), and is among the Highly Cited Researchers by Clarivate Analytics and the Most Cited Chinese Researchers by Elsevier.

摘要/Abstract

摘要： 随着可燃冰和页岩气开采技术的迅速发展，甲烷的储量逐年增加.因此，甲烷不仅被视为一种清洁能源，同时也被认为是一种可用于生产高附加值化工产品的碳原料.然而，由于甲烷分子具有十分稳定的成键结构，所以传统的甲烷转化技术（尤其是甲烷水汽重整反应）通常需要大量的能量输入.针对这一问题，光催化技术可以利用具有高能量的光生载流子来打破甲烷转化的热力学势垒，被认为是在温和条件下实现甲烷转化的一种非常具有前景的途径.在光催化甲烷转化领域，金属氧化物基光催化剂已经得到了广泛的研究，这主要归因于它们的强氧化能力.在本文中，我们首先基于光催化甲烷转化反应的基本原理对金属氧化物在该反应中所具备的优势进行了讨论.随后，我们回顾了近年来金属氧化物基光催化剂在目前各类甲烷转化反应中的研究进展，包括甲烷完全氧化（TOM）、甲烷部分氧化（POM）、甲烷干重整（DRM）、甲烷无氧偶联（NOCM）以及晶格氧辅助的甲烷偶联（LOCM）等几类反应.最后，我们对基于金属氧化物的光催化甲烷转化技术所面临的挑战与机遇进行了展望.

关键词: 光催化, 甲烷转化, 金属氧化物, 表面反应, 选择性

Abstract: With the rapid development of combustible ice and shale gas mining technology, the reserve of methane (CH4) has been growing abundant. Therefore, there is a paradigm shift, where CH4 is not seen only as a hydrocarbon fuel, but also as carbon feedstocks for synthesizing various value-added chemicals. However, the conventional CH4 conversion technology, especially steam reforming of methane, normally requires extensive energy input due to the extremely stable bonding of CH4. To this end, photocatalysis, which can break the thermodynamic barrier of CH4 conversion, has been known as a promising candidate for reaching large-scale CH4 conversion under ambient condition. In the photocatalytic CH4 conversion researches, metal oxides have been extensively investigated mainly due to their high oxidation capability. In this review, a discussion is first given on the fundamentals of CH4 conversion and the advantages of metal oxides in such a reaction. Then the development of metal oxides-based photocatalysts in various CH4 conversion reactions is reviewed, including total oxidation of methane (TOM), partial oxidation of methane (POM), dry-reforming of methane (DRM), non-oxidative coupling of methane (NOCM), lattice oxygen mediated oxidative coupling of methane (LOCM) and so on. Finally, the opportunities of metal oxides-based photocatalytic CH4 conversion along with the challenges are summarized.

Key words: photocatalysis, methane conversion, metal oxides, surface reaction, selectivity

中图分类号:

O643.36

江文斌, 刘敬祥, 邱畅, 龙冉, 熊宇杰. 基于金属氧化物的光催化甲烷转化：原理、进展与挑战[J]. 中国科学技术大学学报, 2020, 50(11): 1361-1382.

JIANG Wenbin, LOW Jingxiang, QIU Chang, LONG Ran, XIONG Yujie. Photocatalytic methane conversion over metal oxides: Fundamentals, achievements, and challenges[J]. Journal of University of Science and Technology of China, 2020, 50(11): 1361-1382.

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基于金属氧化物的光催化甲烷转化：原理、进展与挑战

Photocatalytic methane conversion over metal oxides: Fundamentals, achievements, and challenges

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