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Mechanistic Studies of Catalytic Activity in Electrochemical CO2 Reduction Reaction by Operando Surface Enhanced Raman Spectroscopy Coupled with Electrochemical Mass Spectrometry

Periodic Reporting for period 1 - ESRS-EMS for CO2RR (Mechanistic Studies of Catalytic Activity in Electrochemical CO2 Reduction Reaction by Operando Surface Enhanced Raman Spectroscopy Coupled with Electrochemical Mass Spectrometry)

Reporting period: 2021-01-01 to 2022-12-31

The project has achieved the majority of its objectives and milestones for the period, with some changes and modifications of the goals with considerations over the technical challenges and unprecedented situations. In overall, I successfully developed operando spectroscopic techniques to study the electrochemical reaction mechanisms governing the electrocatalysis reactions related to clean energy applications including electrochemical CO2 reduction, nitrogen reduction, and hydrogen production. I also developed electrochemical approaches to reduce CO2 release through production of on-demand CO2-intensive chemicals and commodities from industrial wastes and side-products using clean and CO2-free electrical energy.
Due to COVID pandemic and restrictions upon traveling and on-site laboratory working, substantial delays and limitations were experienced in establishing planned spectroscopic facilities and experimental parts of the proposal. Out of the WPs, WP1, WP3 and WP4 have been fulfilled while WP2 was modified according to the experimental limitations mainly imposed by special situations of COVID pandemic.
The Work Packages, Milestones, and Deliverables of the project are outlined below. The project achieved and surpassed the planned objectives in WP1, WP3, and WP4. A secondment had been planned in WP2 to synthesize a variety of electrocatalysts for application in operando studies which could not be accomplished due the travel restrictions as a result of COVID pandemic. Therefore, the activities in WP2 was modified and replanned to cover collaboration with local research groups working on different aspects of electrochemical reactions for clean energy applications. In this regard, I started collaborative research to apply operando Raman spectroscopy in other areas including nitrogen reduction reaction, hydrogen production, and electrochemical energy storage devices such as Na/Li-ion batteries.
List of my published publications:

1) Yadegari, H.; Zhou, Y.; and Ryan, M. P.; Section 2: What is the future of CO2 capture for CO2 utilization?, J. Phys. Materials 2022, 5, 032001.
2) Barrio, J.; Pedersen, A.; Feng, J.; Sarma, S. C.; Wang, M.; Li, A. Y.; Yadegari, H.; Luo, H.; Ryan, M. P.; Titirici, M.-M. Metal coordination in C 2 N-like materials towards dual atom catalysts for oxygen reduction. Journal of Materials Chemistry A 2022, 10 (11), 6023-6030.
3) Xu, Z.; Wang, J.; Guo, Z.; Xie, F.; Liu, H.; Yadegari, H.; Tebyetekerwa, M.; Ryan, M. P.; Hu, Y. S.; Titirici, M. M., The role of hydrothermal carbonization in sustainable sodium‐ion battery anodes. Adv. Energy Mater. 2022, 12 (18), 2200208.
4) Zhang, H.; Diao, J.; Ouyang, M.; Yadegari, H.; Mao, M.; Wang, J.; Henkelman, G.; Xie, F.; Riley, D. J., Enhancing the Performance of Bi2S3 in Electrocatalytic and Supercapacitor Applications by Controlling Lattice Strain. Adv. Funct. Mater. 2022, 32 (48), 2205974.
5) Zhang, H.; Geng, S.; Ouyang, M.; Yadegari, H.; Xie, F.; Riley, D. J., A Self‐Reconstructed Bifunctional Electrocatalyst of Pseudo‐Amorphous Nickel Carbide@ Iron Oxide Network for Seawater Splitting. Advanced Science 2022, 9 (15), 2200146.
6) Westhead, O.; Spry, M.; Bagger, A.; Shen, Z.; Yadegari, H.; Favero, S.; Tort, R.; Titirici, M.; Ryan, M. P.; Jervis, R., The role of ion solvation in lithium mediated nitrogen reduction. Journal of Materials Chemistry A 2023.
7) Zhang, H.; Diao, J.; Ouyang, M.; Yadegari, H.; Mao, M.; Wang, M.; Henkelman, G.; Xie, F.; Riley, D. J., Heterostructured Core–Shell Ni–Co@ Fe–Co Nanoboxes of Prussian Blue Analogues for Efficient Electrocatalytic Hydrogen Evolution from Alkaline Seawater. Acs Catal 2023, 13, 1349-1358.

Another publication is being prepared and expected to be submitted in 1-2 months.
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