Final published version, 5.96 MB, PDF document
Available under license: CC BY-NC-ND: Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License
Research output: Thesis › Doctoral Thesis
Research output: Thesis › Doctoral Thesis
}
TY - BOOK
T1 - Towards Efficient MXene-based Electrocatalysts for Electrochemical CO2 Reduction
AU - Robertshaw, Samuel
PY - 2025/4/19
Y1 - 2025/4/19
N2 - The increased utilisation of non-renewable energy sources in recent decades hashad a drastic impact on the Earth’s climate. With significant anthropogenic carbondioxide (CO2) emissions causing drastic changes to the Earth’s atmosphere, thedecarbonisation of energy generation alongside renewable energy alternatives tofossil fuels is crucial. The electrocatalytic reduction of CO2 (eCO2RR) to value-addedchemicals is an attractive and sustainable technology towards achieving a low-carbon economy. However, current electrocatalysts have been reported to sufferfrom low selectivity, poor stability, and high overpotentials, thus limiting their scale-up potential. There is a critical demand for the development of efficient novelelectrocatalysts with high selectivity towards desired products. A new class of 2-dimensional materials known as MXenes has gained significant interest in the recentliterature due to their unique structural and electronic properties. Severalcomputational studies have highlighted Ti3C2Tx to be of significant interest as aneCO2RR electrocatalyst. This thesis works towards evaluating Ti3C2Tx for theapplication of eCO2RR catalysis, with a particular focus on the fabrication of MXene-modified electrodes using MXene powders. Additionally, the treatment and handlingof Ti3C2Tx powders is reported herein, with the successful -O and -OH surfacefunctionalisation of a commercial MXene also demonstrated via ozonemodifications. Finally, the design and manufacture of bespoke electrochemical cellsis reported, with the aim of accommodating a wealth of electrode morphologieswhile simultaneously optimising and improving current systems for accurateeCO2RR product quantification.
AB - The increased utilisation of non-renewable energy sources in recent decades hashad a drastic impact on the Earth’s climate. With significant anthropogenic carbondioxide (CO2) emissions causing drastic changes to the Earth’s atmosphere, thedecarbonisation of energy generation alongside renewable energy alternatives tofossil fuels is crucial. The electrocatalytic reduction of CO2 (eCO2RR) to value-addedchemicals is an attractive and sustainable technology towards achieving a low-carbon economy. However, current electrocatalysts have been reported to sufferfrom low selectivity, poor stability, and high overpotentials, thus limiting their scale-up potential. There is a critical demand for the development of efficient novelelectrocatalysts with high selectivity towards desired products. A new class of 2-dimensional materials known as MXenes has gained significant interest in the recentliterature due to their unique structural and electronic properties. Severalcomputational studies have highlighted Ti3C2Tx to be of significant interest as aneCO2RR electrocatalyst. This thesis works towards evaluating Ti3C2Tx for theapplication of eCO2RR catalysis, with a particular focus on the fabrication of MXene-modified electrodes using MXene powders. Additionally, the treatment and handlingof Ti3C2Tx powders is reported herein, with the successful -O and -OH surfacefunctionalisation of a commercial MXene also demonstrated via ozonemodifications. Finally, the design and manufacture of bespoke electrochemical cellsis reported, with the aim of accommodating a wealth of electrode morphologieswhile simultaneously optimising and improving current systems for accurateeCO2RR product quantification.
U2 - 10.17635/lancaster/thesis/2729
DO - 10.17635/lancaster/thesis/2729
M3 - Doctoral Thesis
PB - Lancaster University
ER -