Events Calendar

19 Aug
PhD Dissertation Final Defense- Anantha Venkataraman Nagarajan
Event Type

Defenses

Topic

Research

Target Audience

Graduate Students

University Unit
Department of Chemical and Petroleum Engineering
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PhD Dissertation Final Defense- Anantha Venkataraman Nagarajan

 

Chair:

Prof. Giannis Mpourmpakis, Chemical and Petroleum Engineering Department, University of Pittsburgh

 

Committee:

Prof. John A. Keith, Chemical and Petroleum Engineering Department, University of Pittsburgh

 

Prof. James R. McKone, Chemical and Petroleum Engineering Department, University of Pittsburgh

 

Prof. Guofeng Wang, Mechanical Engineering and Materials Science Department, University of Pittsburgh

 

Dr. Douglas R. Kauffman, National Energy Technology Lab, Pittsburgh, PA

 

Title:

Investigation of atomically precise nanostructures for electrocatalytic conversion of CO2

 

Abstract:

In order to alleviate the high concentrations of CO2 while meeting increasing demands for chemicals and fuels, electrochemical CO2 reduction reaction (CO2RR) has gained tremendous interest. A vast array of nanomaterials have been investigated as electrocatalysts that can reliably convert CO2 to valuable fuels and chemicals. However, understanding the atomic-level behavior of nanomaterials during CO2RR remains a complex challenge. Overcoming this challenge will result in the rapid, targeted development of nanomaterials that can significantly promote circular economy. Ligand-protected metal nanoclusters (LPNCs) are a remarkable class of nanomaterials (1-3 nm in diameter) with unique physicochemical proper-ties that can outperform larger, conventional nanoparticles (NPs) for CO2RR. Importantly, their atomically precise structures provide a platform to unravel accurate mechanistic insight into CO2RR through accurate computational methods such as Density Functional Theory (DFT).

 

This work elucidates the detailed behavior of LPNCs during CO2RR while also building a foundation for the rapid discovery of new, highly active LPNCs for electrocatalytic applications. First, we showcased the stability of a range of LPNCs during CO2RR through the Thermodynamic Stability Model (TSM). Importantly, we rationalized the experimentally observed stability of the well-known Au25 LPNC during CO2RR. Next, we expanded the nanomaterials domain of interest and elucidated the experimentally observed higher CO2RR performance of Au-based LPNCs modified via heterometal doping and ligand engineering. At the same time, we uncovered the nature of catalytically active sites on LPNCs during CO2RR. Lastly, we provided a descriptor-based framework for the accelerated screening of electrocatalytically active alloy LPNCs. Overall, this dissertation provides important insights into the electrocatalytic behavior of LPNCs and their applicability towards sustainable fuels and chemicals production.

Dial-In Information

Virtual:

Zoom Link: https://pitt.zoom.us/j/94315648877

Meeting ID: 943 1564 8877

Password: 206041

Friday, August 19 at 10:00 a.m. to 12:00 p.m.

Benedum Hall, 702 Benedum Hall
3700 O'Hara Street, Pittsburgh, PA 15261

PhD Dissertation Final Defense- Anantha Venkataraman Nagarajan

 

Chair:

Prof. Giannis Mpourmpakis, Chemical and Petroleum Engineering Department, University of Pittsburgh

 

Committee:

Prof. John A. Keith, Chemical and Petroleum Engineering Department, University of Pittsburgh

 

Prof. James R. McKone, Chemical and Petroleum Engineering Department, University of Pittsburgh

 

Prof. Guofeng Wang, Mechanical Engineering and Materials Science Department, University of Pittsburgh

 

Dr. Douglas R. Kauffman, National Energy Technology Lab, Pittsburgh, PA

 

Title:

Investigation of atomically precise nanostructures for electrocatalytic conversion of CO2

 

Abstract:

In order to alleviate the high concentrations of CO2 while meeting increasing demands for chemicals and fuels, electrochemical CO2 reduction reaction (CO2RR) has gained tremendous interest. A vast array of nanomaterials have been investigated as electrocatalysts that can reliably convert CO2 to valuable fuels and chemicals. However, understanding the atomic-level behavior of nanomaterials during CO2RR remains a complex challenge. Overcoming this challenge will result in the rapid, targeted development of nanomaterials that can significantly promote circular economy. Ligand-protected metal nanoclusters (LPNCs) are a remarkable class of nanomaterials (1-3 nm in diameter) with unique physicochemical proper-ties that can outperform larger, conventional nanoparticles (NPs) for CO2RR. Importantly, their atomically precise structures provide a platform to unravel accurate mechanistic insight into CO2RR through accurate computational methods such as Density Functional Theory (DFT).

 

This work elucidates the detailed behavior of LPNCs during CO2RR while also building a foundation for the rapid discovery of new, highly active LPNCs for electrocatalytic applications. First, we showcased the stability of a range of LPNCs during CO2RR through the Thermodynamic Stability Model (TSM). Importantly, we rationalized the experimentally observed stability of the well-known Au25 LPNC during CO2RR. Next, we expanded the nanomaterials domain of interest and elucidated the experimentally observed higher CO2RR performance of Au-based LPNCs modified via heterometal doping and ligand engineering. At the same time, we uncovered the nature of catalytically active sites on LPNCs during CO2RR. Lastly, we provided a descriptor-based framework for the accelerated screening of electrocatalytically active alloy LPNCs. Overall, this dissertation provides important insights into the electrocatalytic behavior of LPNCs and their applicability towards sustainable fuels and chemicals production.

Dial-In Information

Virtual:

Zoom Link: https://pitt.zoom.us/j/94315648877

Meeting ID: 943 1564 8877

Password: 206041

Friday, August 19 at 10:00 a.m. to 12:00 p.m.

Benedum Hall, 702 Benedum Hall
3700 O'Hara Street, Pittsburgh, PA 15261

Event Type

Defenses

Topic

Research

Target Audience

Graduate Students

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