Mixed-Valence Single-Atom Catalyst Derived from Functionalized Graphene

Advanced Materials
Aristides BakandritsosRadek Zbořil

Abstract

Single-atom catalysts (SACs) aim at bridging the gap between homogeneous and heterogeneous catalysis. The challenge is the development of materials with ligands enabling coordination of metal atoms in different valence states, and preventing leaching or nanoparticle formation. Graphene functionalized with nitrile groups (cyanographene) is herein employed for the robust coordination of Cu(II) ions, which are partially reduced to Cu(I) due to graphene-induced charge transfer. Inspired by nature's selection of Cu(I) in enzymes for oxygen activation, this 2D mixed-valence SAC performs flawlessly in two O2 -mediated reactions: the oxidative coupling of amines and the oxidation of benzylic CH bonds toward high-value pharmaceutical synthons. High conversions (up to 98%), selectivities (up to 99%), and recyclability are attained with very low metal loadings in the reaction. The synergistic effect of Cu(II) and Cu(I) is the essential part in the reaction mechanism. The developed strategy opens the door to a broad portfolio of other SACs via their coordination to various functional groups of graphene, as demonstrated by successful entrapment of FeIII /FeII single atoms to carboxy-graphene.

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Citations

Oct 2, 2019·Chemical Society Reviews·Huilong FeiXiangfeng Duan
Feb 7, 2020·Chemistry : a European Journal·Antonios KouloumpisMichal Otyepka
Dec 5, 2020·Advanced Materials·Kolleboyina JayaramuluRoland A Fischer
Mar 18, 2021·Nanoscale·Philippe Serp
Mar 26, 2021·Advanced Materials·Haifeng XiongYong Wang
Mar 31, 2021·Small·Ravishankar G KadamManoj B Gawande
Feb 25, 2021·Nanotechnology·Jan NavrátilMichal Otyepka
Apr 14, 2021·Chemistry : a European Journal·Mingzhu JiangHongpeng Jia
Jan 1, 2020·ACS Applied Materials & Interfaces·Xin LuoChengzhou Zhu
Jul 7, 2021·Small·Yu WuChengzhou Zhu
Apr 4, 2020·Chemical Reviews·Shufang JiYadong Li
Oct 22, 2020·Chemical Reviews·Selina K KaiserJavier Pérez-Ramírez
Oct 1, 2021·Proceedings of the National Academy of Sciences of the United States of America·Yan YanZhiqun Lin
Oct 14, 2021·Chemical Reviews·Baljeet SinghRadek Zbořil

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