Atomic tuning of 3D printed carbon surface chemistry for electrocatalytic nitrite oxidation and reduction to ammonia

Gao, Wanli; Michalička, Jan; Pumera, Martin

Atomic tuning of 3D printed carbon surface chemistry for electrocatalytic nitrite oxidation and reduction to ammonia

Files

d4ta06800a.pdf(2.29 MB)

Date

2024-11-26

Authors

Gao, Wanli

Michalička, Jan

Pumera, Martin

ORCID

0000-0001-7879-2253

0000-0001-6231-0061

0000-0001-5846-2951

Publisher

ROYAL SOC CHEMISTRY

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Abstract

Nitrite contamination in agricultural and industrial wastewater presents a critical impact on environmental sustainability, demanding efficient strategies for monitoring and remediation. This study addresses this challenge by developing cost-effective electrocatalysts for both nitrite detection and conversion to value-added ammonia. 3D printed carbon materials are explored as bifunctional platforms for the electrochemical nitrite oxidation reaction (NO2OR) and nitrite reduction reaction (NO2RR). Benefiting from the inherent Ti-dominated metallic impurities and intrinsic surface features of carbon nanotubes, 3D printed carbon electrodes exhibit electrocatalytic activity for both reactions. To enhance this activity, we further introduce an effective fabrication methodology that combines 3D printing of carbon substrates with precise surface modification using atomic layer deposition (ALD) of TiO2. The resulting TiO2-coated carbon electrode demonstrates significantly improved electrocatalytic properties. For NO2OR, it exhibits a peak current density of 0.75 mA cm-2 at 1.53 V vs. RHE, while for NO2RR, it achieves a yield rate of 630.5 mu g h-1 cm-2 with a faradaic efficiency of 81.9% at -1.06 V vs. RHE. This enhancement in electrocatalytic activity is primarily attributed to the formation of abundant interfaces between the conductive carbon and ALD-coated TiO2. The developed methodology not only enables precise modification of 3D printed carbon surface chemistry but also presents a scalable method for electrocatalyst production.

Keywords

Bioremediation, Carbon electrodes, Electrochemical oxidation, Electrolysis, Nitrogen oxides, Oxygen reduction reaction, Surface chemistry, Titanium dioxide, Titanium nitride

Citation

Journal of Materials Chemistry A. 2024, vol. 12, issue 46, p. 32458-32470.
https://pubs.rsc.org/en/content/articlelanding/2024/ta/d4ta06800a

Document type

Peer-reviewed

Document version

Published version

Language of document

en