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通过石墨烯模板向超薄金属有机层进行便捷的电子传递以促进CO光还原。

Facile electron delivery from graphene template to ultrathin metal-organic layers for boosting CO photoreduction.

作者信息

Wang Jia-Wei, Qiao Li-Zhen, Nie Hao-Dong, Huang Hai-Hua, Li Yi, Yao Shuang, Liu Meng, Zhang Zhi-Ming, Kang Zhen-Hui, Lu Tong-Bu

机构信息

Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering, Tianjin University of Technology, Tianjin, 300384, China.

School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin, 300384, China.

出版信息

Nat Commun. 2021 Feb 5;12(1):813. doi: 10.1038/s41467-021-21084-9.

Abstract

Metal-organic layers with ordered structure and molecular tunability are of great potential as heterogeneous catalysts due to their readily accessible active sites. Herein, we demonstrate a facile template strategy to prepare metal-organic layers with a uniform thickness of three metal coordination layers (ca. 1.5 nm) with graphene oxide as both template and electron mediator. The resulting hybrid catalyst exhibits an excellent performance for CO photoreduction with a total CO yield of 3133 mmol g (CO selectivity of 95%), ca. 34 times higher than that of bulky Co-based metal-organic framework. Systematic studies reveal that well-exposed active sites in metal-organic layers, and facile electron transfer between heterogeneous and homogeneous components mediated by graphene oxide, greatly contribute to its high activity. This work highlights a facile way for constructing ultrathin metal-organic layers and demonstrates charge transfer pathway between conductive template and catalyst for boosting photocatalysis.

摘要

具有有序结构和分子可调性的金属有机层由于其易于接近的活性位点而作为多相催化剂具有巨大潜力。在此,我们展示了一种简便的模板策略,以氧化石墨烯作为模板和电子介质,制备具有三个金属配位层均匀厚度(约1.5nm)的金属有机层。所得的杂化催化剂在CO光还原方面表现出优异的性能,总CO产率为3133 mmol g(CO选择性为95%),约为块状钴基金属有机框架的34倍。系统研究表明,金属有机层中充分暴露的活性位点,以及由氧化石墨烯介导的多相和均相组分之间的便捷电子转移,极大地促进了其高活性。这项工作突出了构建超薄金属有机层的简便方法,并展示了导电模板与催化剂之间的电荷转移途径以促进光催化。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aa42/7864970/17275f623983/41467_2021_21084_Fig1_HTML.jpg

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