Leppänen, E., Aarva, A., Sainio, S., Caro, M. A., & Laurila, T. (2021). Connection between the physicochemical characteristics of amorphous carbon thin films and their electrochemical properties. Journal of Physics: Condensed Matter, 33(43), 434002. https://doi.org/10.1088/1361-648X/ac1a2e
Connection between the physicochemical characteristics of amorphous carbon thin films and their electrochemical properties
|Author:||Leppänen, Elli1; Aarva, Anja1; Sainio, Sami2,3;|
1Department of Electrical Engineering and Automation, School of Electrical Engineering, Aalto University, Tietotie 3, 02150 Espoo, Finland
2Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA
3Microelectronics Research Unit, Faculty of Information Technology and Electrical Engineering, University of Oulu, P.O. Box. 4500, 90570 Oulu, Finland
4Department of Chemistry and Materials Science, Aalto University, Kemistintie 1, 02150 Espoo, Finland
|Persistent link:|| http://urn.fi/urn:nbn:fi-fe2022020918263
|Publish Date:|| 2022-08-18
Connecting a material's surface chemistry with its electrocatalytic performance is one of the major questions in analytical electrochemistry. This is especially important in many sensor applications where analytes from complex media need to be measured. Unfortunately, today this connection is still largely missing except perhaps for the most simple ideal model systems. Here we present an approach that can be used to obtain insights about this missing connection and apply it to the case of carbon nanomaterials. In this paper we show that by combining advanced computational techniques augmented by machine learning methods with x-ray absorption spectroscopy (XAS) and electrochemical measurements, it is possible to obtain a deeper understanding of the correlation between local surface chemistry and electrochemical performance. As a test case we show how by computationally assessing the growth of amorphous carbon (a-C) thin films at the atomic level, we can create computational structural motifs that may in turn be used to deconvolute the XAS data from the real samples resulting in local chemical information. Then, by carrying out electrochemical measurements on the same samples from which x-ray spectra were measured and that were further characterized computationally, it is possible to gain insight into the interplay between the local surface chemistry and electrochemical performance. To demonstrate this methodology, we proceed as follows: after assessing the basic electrochemical properties of a-C films, we investigate the effect of short HNO3 treatment on the sensitivity of these electrodes towards an inner sphere redox probe dopamine to gain knowledge about the influence of altered surface chemistry to observed electrochemical performance. These results pave the way towards a more general assessment of electrocatalysis in different systems and provide the first steps towards data driven tailoring of electrode surfaces to gain optimal performance in a given application.
Journal of physics. Condensed matter
|Type of Publication:||
A1 Journal article – refereed
|Field of Science:||
116 Chemical sciences
This project has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement no. 841621.
|EU Grant Number:||
(841621) TACOMA - Towards Application specific tailoring of CarbOn nanoMAterials
© 2021 IOP Publishing Ltd. The final authenticated version is available online at https://doi.org/10.1088/1361-648X/ac1a2e.