Adsorption Behavior of the Coenzyme NADH at the Carbon/Electrolyte Interface Determined by Neutron Reflectometry

Mary H. Wood; Juan Rubio-Lara; Alexander J. Armstrong; Rebecca J.L. Welbourn

doi:10.1021/acs.langmuir.2c03026

Adsorption Behavior of the Coenzyme NADH at the Carbon/Electrolyte Interface Determined by Neutron Reflectometry

Mary H. Wood, Juan Rubio-Lara, Alexander J. Armstrong, Rebecca J.L. Welbourn

Research output: Contribution to journal › Article › peer-review

Abstract

The adsorption behavior of β-nicotinamide adenine dinucleotide (NADH) at the carbon/electrolyte interface has been studied using a combination of neutron reflectometry (NR) and solution depletion isotherms. Coupling the NR technique with an electrochemical cell allowed in situ observation of the reversible adsorption and desorption of the molecule at the electrode surface over a range of applied potentials. The overall surface coverage was low (30-50%), suggesting adsorption only at specific defect sites on the surface. Isotherms conducted over a range of temperatures were used to extract thermodynamic parameters, which implied strong physisorption via electrostatic interactions. In addition, changes in the outermost layer of the carbon electrode were observed as the applied potential was varied, which were confirmed with ex situ X-ray reflectivity measurements (XRR). X-ray photoelectron spectroscopy (XPS) measurements of the carbon surface demonstrated the majority of carbon atoms were in an sp² state.

Original language	English
Pages (from-to)	668-678
Number of pages	11
Journal	Langmuir
Volume	39
Issue number	1
DOIs	https://doi.org/10.1021/acs.langmuir.2c03026
State	Published - Jan 10 2023
Externally published	Yes

Funding

We thank Professor Paul Bowen at the EPFL for conducting the BET surface area measurements and Thomas Charleston, Andy Church, and Jos Cooper at the ISIS Neutron Source for development of the NR electrochemical cell. NR data were collected at the ISIS Neutron and Muon Source; we are grateful for the allocation of beamtime (RB1820189) from the Science and Technology Facilities Council (data doi:10.5286/ISIS.E.RB1820189) and for access to the XRR diffractometer at the Materials Characterisation Laboratory for the ISIS Neutron source. We are also grateful for funding from the Human Frontiers Science Programme (HFSP, Grant LT000307/2019). We thank Professor Paul Bowen at the EPFL for conducting the BET surface area measurements and Thomas Charleston, Andy Church, and Jos Cooper at the ISIS Neutron Source for development of the NR electrochemical cell. NR data were collected at the ISIS Neutron and Muon Source; we are grateful for the allocation of beamtime (RB1820189) from the Science and Technology Facilities Council (data doi:10.5286/ISIS.E.RB1820189 ) and for access to the XRR diffractometer at the Materials Characterisation Laboratory for the ISIS Neutron source. We are also grateful for funding from the Human Frontiers Science Programme (HFSP, Grant LT000307/2019).

Funders	Funder number
Human Frontier Science Program	LT000307/2019
Science and Technology Facilities Council	:10.5286/ISIS.E.RB1820189
École Polytechnique Fédérale de Lausanne	RB1820189

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title = "Adsorption Behavior of the Coenzyme NADH at the Carbon/Electrolyte Interface Determined by Neutron Reflectometry",

abstract = "The adsorption behavior of β-nicotinamide adenine dinucleotide (NADH) at the carbon/electrolyte interface has been studied using a combination of neutron reflectometry (NR) and solution depletion isotherms. Coupling the NR technique with an electrochemical cell allowed in situ observation of the reversible adsorption and desorption of the molecule at the electrode surface over a range of applied potentials. The overall surface coverage was low (30-50%), suggesting adsorption only at specific defect sites on the surface. Isotherms conducted over a range of temperatures were used to extract thermodynamic parameters, which implied strong physisorption via electrostatic interactions. In addition, changes in the outermost layer of the carbon electrode were observed as the applied potential was varied, which were confirmed with ex situ X-ray reflectivity measurements (XRR). X-ray photoelectron spectroscopy (XPS) measurements of the carbon surface demonstrated the majority of carbon atoms were in an sp2 state.",

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AB - The adsorption behavior of β-nicotinamide adenine dinucleotide (NADH) at the carbon/electrolyte interface has been studied using a combination of neutron reflectometry (NR) and solution depletion isotherms. Coupling the NR technique with an electrochemical cell allowed in situ observation of the reversible adsorption and desorption of the molecule at the electrode surface over a range of applied potentials. The overall surface coverage was low (30-50%), suggesting adsorption only at specific defect sites on the surface. Isotherms conducted over a range of temperatures were used to extract thermodynamic parameters, which implied strong physisorption via electrostatic interactions. In addition, changes in the outermost layer of the carbon electrode were observed as the applied potential was varied, which were confirmed with ex situ X-ray reflectivity measurements (XRR). X-ray photoelectron spectroscopy (XPS) measurements of the carbon surface demonstrated the majority of carbon atoms were in an sp2 state.

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Adsorption Behavior of the Coenzyme NADH at the Carbon/Electrolyte Interface Determined by Neutron Reflectometry

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