Redox-dependent spatially resolved electrochemistry at graphene and graphite step edges.

ACS Nano
Aleix G GüellPatrick R Unwin

Abstract

The electrochemical (EC) behavior of mechanically exfoliated graphene and highly oriented pyrolytic graphite (HOPG) is studied at high spatial resolution in aqueous solutions using Ru(NH3)6(3+/2+) as a redox probe whose standard potential sits close to the intrinsic Fermi level of graphene and graphite. When scanning electrochemical cell microscopy (SECCM) data are coupled with that from complementary techniques (AFM, micro-Raman) applied to the same sample area, different time-dependent EC activity between the basal planes and step edges is revealed. In contrast, other redox couples (ferrocene derivatives) whose potential is further removed from the intrinsic Fermi level of graphene and graphite show uniform and high activity (close to diffusion-control). Macroscopic voltammetric measurements in different environments reveal that the time-dependent behavior after HOPG cleavage, peculiar to Ru(NH3)6(3+/2+), is not associated particularly with any surface contaminants but is reasonably attributed to the spontaneous delamination of the HOPG with time to create partially coupled graphene layers, further supported by conductive AFM measurements. This process has a major impact on the density of states of graphene and graphite edges...Continue Reading

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Citations

Feb 4, 2016·Nano Letters·Matěj VelickýRobert A W Dryfe
Dec 3, 2015·Analytical Chemistry·Stephen M OjaBo Zhang
Mar 10, 2016·ACS Applied Materials & Interfaces·Guohui ZhangPatrick R Unwin
Oct 20, 2015·Physical Chemistry Chemical Physics : PCCP·Concha Bosch-NavarroNeil R Wilson
Jun 20, 2015·Physical Chemistry Chemical Physics : PCCP·Matěj VelickýRobert A W Dryfe
Jul 12, 2016·Langmuir : the ACS Journal of Surfaces and Colloids·Minkyung KangPatrick R Unwin
Jul 14, 2016·Langmuir : the ACS Journal of Surfaces and Colloids·Guohui ZhangPatrick R Unwin
Jul 20, 2016·Chemical Communications : Chem Comm·Elizabeth E OselandPatrick R Unwin
Aug 9, 2016·Accounts of Chemical Research·Patrick R UnwinGuohui Zhang
Oct 16, 2016·ACS Applied Materials & Interfaces·Sharel P EPatrick R Unwin
Dec 10, 2016·Accounts of Chemical Research·Andrew KozbialLei Li
Apr 6, 2017·Journal of the American Chemical Society·Michal WojcikKe Xu
Jun 18, 2017·Chemical Society Reviews·Amir KaplanMichael S Strano
Nov 30, 2016·Advanced Materials·Wangyang FuGrégory F Schneider
Jan 27, 2016·Physical Chemistry Chemical Physics : PCCP·Anatolii S CuharucPatrick R Unwin
Jul 13, 2018·Faraday Discussions·Cameron L Bentley, Patrick R Unwin
Jun 3, 2020·Nanotechnology·Tilmann J NeubertKannan Balasubramanian
May 10, 2017·Proceedings. Mathematical, Physical, and Engineering Sciences·Ashley PagePatrick R Unwin
Dec 6, 2019·Chemical Communications : Chem Comm·Xuan LiuDongping Zhan
Jul 28, 2019·Nanoscale·Michel WehrholdKannan Balasubramanian
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Jul 10, 2020·Analytical Chemistry·Waldemir J PaschoalinoJanine Mauzeroll
Jan 21, 2017·Analytical Chemistry·Yasufumi TakahashiTomokazu Matsue
Feb 15, 2019·Nano Letters·Gyeongwon KangRichard P Van Duyne
Nov 15, 2018·Analytical Chemistry·Jingshu HuiJoaquín Rodríguez-López

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