一种用于合成单原子催化剂的通用石墨烯量子点 tethering 设计策略。

A Universal Graphene Quantum Dot Tethering Design Strategy to Synthesize Single-Atom Catalysts.

作者信息

Jin Song, Ni Youxuan, Hao Zhimeng, Zhang Kai, Lu Yong, Yan Zhenhua, Wei Yajuan, Lu Ying-Rui, Chan Ting-Shan, Chen Jun

机构信息

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Renewable Energy Conversion and Storage Center (RECAST), College of Chemistry, Nankai University, Tianjin, 300071, China.

National Synchrotron Radiation Research Center, Hsinchu, 300, Taiwan.

出版信息

Angew Chem Int Ed Engl. 2020 Dec 1;59(49):21885-21889. doi: 10.1002/anie.202008422. Epub 2020 Sep 29.

DOI:10.1002/anie.202008422

PMID:32822086

Abstract

A general graphene quantum dot-tethering design strategy to synthesize single-atom catalysts (SACs) is presented. The strategy is applicable to different metals (Cr, Mn, Fe, Co, Ni, Cu, and Zn) and supports (0D carbon nanosphere, 1D carbon nanotube, 2D graphene nanosheet, and 3D graphite foam) with the metal loading of 3.0-4.5 wt %. The direct transmission electron microscopy imaging and X-ray absorption spectra analyses confirm the atomic dispersed metal in carbon supports. Our study reveals that the abundant oxygenated groups for complexing metal ions and the rich defective sites for incorporating nitrogen are essential to realize the synthesis of SACs. Furthermore, the carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications.

摘要

提出了一种用于合成单原子催化剂（SACs）的通用石墨烯量子点束缚设计策略。该策略适用于不同的金属（Cr、Mn、Fe、Co、Ni、Cu和Zn）以及载体（0D碳纳米球、1D碳纳米管、2D石墨烯纳米片和3D石墨泡沫），金属负载量为3.0 - 4.5 wt%。直接透射电子显微镜成像和X射线吸收光谱分析证实了碳载体中原子分散的金属。我们的研究表明，用于络合金属离子的丰富含氧基团和用于掺入氮的丰富缺陷位点对于实现SACs的合成至关重要。此外，碳纳米管负载的Ni SACs对CO还原表现出高电催化活性，CO选择性接近100%。这种通用策略有望为生产用于各种电催化应用的SACs开辟新的研究途径。