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  • 2025robertshawphd

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Towards Efficient MXene-based Electrocatalysts for Electrochemical CO2 Reduction

Research output: ThesisDoctoral Thesis

Published
  • Samuel Robertshaw
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Publication date19/04/2025
Number of pages153
QualificationPhD
Awarding Institution
Supervisors/Advisors
Award date30/03/2025
Publisher
  • Lancaster University
<mark>Original language</mark>English

Abstract

The increased utilisation of non-renewable energy sources in recent decades has
had a drastic impact on the Earth’s climate. With significant anthropogenic carbon
dioxide (CO2) emissions causing drastic changes to the Earth’s atmosphere, the
decarbonisation of energy generation alongside renewable energy alternatives to
fossil fuels is crucial. The electrocatalytic reduction of CO2 (eCO2RR) to value-added
chemicals is an attractive and sustainable technology towards achieving a low-
carbon economy. However, current electrocatalysts have been reported to suffer
from low selectivity, poor stability, and high overpotentials, thus limiting their scale-
up potential. There is a critical demand for the development of efficient novel
electrocatalysts with high selectivity towards desired products. A new class of 2-
dimensional materials known as MXenes has gained significant interest in the recent
literature due to their unique structural and electronic properties. Several
computational studies have highlighted Ti3C2Tx to be of significant interest as an
eCO2RR electrocatalyst. This thesis works towards evaluating Ti3C2Tx for the
application of eCO2RR catalysis, with a particular focus on the fabrication of MXene-
modified electrodes using MXene powders. Additionally, the treatment and handling
of Ti3C2Tx powders is reported herein, with the successful -O and -OH surface
functionalisation of a commercial MXene also demonstrated via ozone
modifications. Finally, the design and manufacture of bespoke electrochemical cells
is reported, with the aim of accommodating a wealth of electrode morphologies
while simultaneously optimising and improving current systems for accurate
eCO2RR product quantification.