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

• Published in: Angewandte Chemie International Edition Vol. 59; no. 49; pp. 21885 - 21889
• Main Authors: Jin, Song, Ni, Youxuan, Hao, Zhimeng, Zhang, Kai, Lu, Yong, Yan, Zhenhua, Wei, Yajuan, Lu, Ying‐Rui, Chan, Ting‐Shan, Chen, Jun
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 01.12.2020
• Edition: International ed. in English
• Subjects: Absorption spectra; Carbon; Carbon dioxide; Carbon nanotubes; Catalysts; Chemical synthesis; Chromium; CO2 electrochemical reduction; Copper; Graphene; Iron; Manganese; Metal ions; Metals; Nanospheres; Nickel; Quantum dots; Selectivity; Single atom catalysts; Strategy; Tethering; Transmission electron microscopy; Zinc
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.202008422

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 CO2 reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications. A graphene quantum dot tethering design strategy is developed for the synthesis of single‐atom catalysts, which is applicable to a wide variety of metals and carbon supports. Furthermore, the prepared carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO2 reduction with nearly 100 % CO selectivity.