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Issue 31, 2018
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Monitoring surface transformations of metal carbodiimide water oxidation catalysts by operando XAS and Raman spectroscopy

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Abstract

Transition metal carbodiimides MNCN (M = Co, Ni, Co0.9Ni0.1, Mn and Cu), were studied by simultaneous operando Raman and X-ray absorption spectroscopy (XAS) with focus on surface oxide detection during electrocatalytic water oxidation. As a proof of concept, easily modifiable screen-printed electrodes were used in this unified operando synchrotron setup for a trade-off between convenience of electrochemical anodization and spectroscopic data acquisition. Monitoring of chemical and structural transformations at the electrode surface during initial anodic electrode polarization shows stability for MNCN with M = Co, Ni, Co0.9Ni0.1 and Mn. While MnNCN is inactive, CoNCN emerges as the most active representative of the series. CuNCN displays pronounced side reactions and the formation of a surface copper oxide layer leading to lower current density attributed to water oxidation, as evident from an irreversible variation of the CuNCN redox behaviour in rotating ring-disc voltammetry. Furthermore, the accompanying structural and vibrational spectroscopy properties of the different MNCN compounds were explored with complementary ex situ analytical methods.

Graphical abstract: Monitoring surface transformations of metal carbodiimide water oxidation catalysts by operando XAS and Raman spectroscopy

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Article information


Submitted
20 Apr 2018
Accepted
26 Jun 2018
First published
06 Jul 2018

Dalton Trans., 2018,47, 10759-10766
Article type
Paper

Monitoring surface transformations of metal carbodiimide water oxidation catalysts by operando XAS and Raman spectroscopy

R. J. Müller, J. Lan, K. Lienau, R. Moré, C. A. Triana, M. Iannuzzi and G. R. Patzke, Dalton Trans., 2018, 47, 10759
DOI: 10.1039/C8DT01587B

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