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Powering the future: understanding mechanistic pathways in electrocatalytic CO2 reduction


Project Description

The University of Bath is inviting applications for the following PhD project supervised by Dr Ulrich Hintermair https://researchportal.bath.ac.uk/en/persons/ulrich-hintermair in the Department of Chemistry.

The electro-catalytic reduction of CO2 and H2O to CO, formaldehyde, formic acid, MeOH or higher alcohols holds great potential to give access to key chemical building blocks with much reduced carbon footprint compared to traditional processes based on fossil resources. When powered by renewable electricity from wind, tidal or solar the process mimics natural photosynthesis that not only saves fossil resources but actively consumes anthropogenic CO2. Because the reaction is not dependent on industrial infrastructures or geologically confined resources, it also offers the prospect of small-to-medium scale decentralised chemical and fuel production. The development of efficient electrocatalysts is key to tuning the selectivity of the reaction and increase its efficiency so that real-world application may become viable.

Promising advances in catalyst design have recently been made, but our understanding of their mode of action is still based on empirical optimisation, ex-situ characterisation and computational modelling. A general complication for detailed in-situ studies of electrocatalysts is that the electrochemical responses are difficult to match with independent characterisation of the chemical transformations occurring in the electrolyte under reaction conditions. An accurate mapping of what products are generated over time at different pH values and potentials applied would greatly enhance our understanding of their electrochemical signatures and allow distinguishing concentred versus consecutive product formation pathways that help to understand the overall mechanism. This is especially important in the case of CO2 reduction, as in addition to the various reduced carbon species that may form, competition with proton reduction to give H2 is crucial to improving the efficiency of the process. Currently no methods exist to capture all of these events under meaningful working conditions.

Bath’s Dynamic Reaction Monitoring (DReaM) Facility offers a unique combination of complementary operando techniques currently comprising multi-nuclear FlowNMR, head-space MS, liquid phase MS, UV-vis, and HPLC. All of these are part of a fully integrated and computer-controlled system that is able to track reaction intermediates and products in real time to give comprehensive insight into complex reaction networks. We have successfully demonstrated in-situ analysis of reactions under similar conditions to electrocatalytic CO2 reduction, and have established the quantitative detection of all relevant reaction products in aqueous solution including H2, CO, H2CO, HCOOH, H3COH and higher alcohols. Fast 2D techniques can complement the 1H NMR analysis, and the use of 13CO2 will make direct 13C NMR monitoring possible. Cross-over experiments with unlabelled CO or CO2 will give further insights into the sequence of higher product formation. This would be the first demonstration of real-time in-situ analysis of an electrocatalytic reaction by high-resolution FlowNMR spectroscopy, and the ability to freely modulate the electrochemical conditions during the analysis will provide unprecedented insights into the reaction network, paving the way to the rational design of improved catalysts and optimized reaction conditions.

Candidate requirements:

Applicants should hold, or expect to receive, a First Class or good Upper Second Class Honours degree, or the equivalent from an overseas university. A master’s level qualification would also be advantageous.

Enquiries and applications:

Informal enquiries are welcomed and should be directed to Dr Ulrich Hintermair, .

Formal applications should be made via the University of Bath’s online application form for a PhD in Chemistry:
https://samis.bath.ac.uk/urd/sits.urd/run/siw_ipp_lgn.login?process=siw_ipp_app&code1=RDUCH-FP01&code2=0014

More information about applying for a PhD at Bath may be found here:
http://www.bath.ac.uk/guides/how-to-apply-for-doctoral-study/

Anticipated start date: 28 September 2020.

Funding Notes

UK and EU citizens, who have been ordinarily resident in the UK since September 2017, may be considered for a studentship funded by the Engineering and Physical Sciences Research Council in conjunction with Catalytic Innovations, Inc. View Website

Funding will cover UK/EU tuition fees, maintenance at the UKRI doctoral stipend rate (£15,009 per annum tax-free in 2019/20, increasing annually in line with the GDP inflator) and a training support grant (£1,000 per annum) for a period of up to 3.5 years.

References

J. Mat. Chem. A 2017, 5, 8230-8246.
Cat. Sci. Tech. 2016, 6, (24), 8406.
ACS Cat. 2019, 9 (3), 2079.

How good is research at University of Bath in Chemistry?

FTE Category A staff submitted: 33.10

Research output data provided by the Research Excellence Framework (REF)

Click here to see the results for all UK universities

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