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- Title
- Developing Advanced Materials for Carbon Dioxide Electroreduction to Value-Added Chemicals and Fuels
- Creator
- Esmaeilirad, Mohammadreza
- Date
- 2023
- Description
-
Developing highly efficient electrocatalysts for the carbon dioxide reductionreaction (CO2RR) to value-added fuels and chemicals offers a...
Show moreDeveloping highly efficient electrocatalysts for the carbon dioxide reductionreaction (CO2RR) to value-added fuels and chemicals offers a feasible pathway for renewable energy storage and could help mitigate the ever-increasing carbon dioxide (CO2) emissions from human activities. Different catalysts are known to catalyze CO2RR in aqueous solutions. Most known catalysts are only capable of transferring 2 electrons with needed protons to CO2 producing either carbon monoxide (CO) or formic acid (HCOOH). Copper (Cu) is the only electrocatalytic material that converts CO2 into different types of hydrocarbon products. Additionally, owing to Cu’s natural abundance and low cost, it has been intensively studied for CO2RR for decades. However, the required high input energy (overpotential), low product selectivity towards valuable fuel products, and the lack of long-term stability remain major challenges for Cu-based catalysts. This work aims to develop new materials that produce hydrocarbons at lower overpotentials with higher rates and greater selectivity than current copper catalysts. By implementing a process referred to as the electrocatalyst discovery cycle iterations between predications, catalyst testing, and active site characterization allow for the rational design and discovery of new and improved electrocatalysts for CO2RR. This methodology led to the discovery of different heteroatomic catalysts as low overpotential catalysts for electroreduction of CO2 high energy density hydrocarbon products.
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- Title
- High-Entropy Stabilization as a Designing Tool for Li-Ion Electrodes
- Creator
- Bandeira Jovino Marques, Otavio Jose
- Date
- 2023
- Description
-
High-Entropy oxides (HEOs) form a new class of materials where the configurational entropy plays the stabilizing role of multicomponent...
Show moreHigh-Entropy oxides (HEOs) form a new class of materials where the configurational entropy plays the stabilizing role of multicomponent systems at high temperatures. Recently, it raised much attention for energy storage applications, especially on Li-ion batteries, where the combination of several different elements in a single solid solution can synergistically act to overcome some of its main drawbacks, improving the battery’s performance. The entropy stabilization opens new boundaries on electrode’s design by increasing the compositional space available for different structures and compounds. Not long ago, the high-entropy oxide (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O demonstrated a big potential as anode material in Li-ion batteries. Its high capacity and long cycling stability raised a lot of questions about the role of the transition metals in the conversion reaction, and the configurational entropy contribution to the electrochemical reaction, further supporting the electrode’s stability. In order to investigate the structural evolution, the role of the multicomponent oxides and structures on the battery’s performance, and the entropic contribution to the electrode’s stability, this research proposes a systematic and robust methodology around the (Mg0.2Co0.2Ni0.2Cu0.2Zn0.2)O high-entropy oxide (HEO). The project heavily relies on the EXAFS ability to determine the short-range structure and the chemical sensitivity to isolate the elemental contribution of the compound at different cycling and charging states. First, the role of different metallic cations on the electrochemical reaction mechanism of the HEO was analyzed by the change in local structure during different charging steps of a Li-ion battery (Chapter 3). Secondly, the entropy contribution and tunability effects on electrochemical performance were tested in a series of medium and high-entropy oxides derived from the seminal HEO. Mg, Co, Ni, Cu, and Zn were individually removed from the HEO’s composition at a time and tested as Li-ion electrode. Fe was also added to the HEO’s composition (HEO+Fe) in order to prove the tunability effects and entropy contribution (Chapter 4). Operando x-ray absorption spectroscopy (XAS) was used to capture the short lived phases and the transient nature of the conversion reaction, to explain the origins of the extra storage capacity encountered on entropy stabilized systems (Chapter 5). Finally, the role of the high-entropy oxide initial structure was investigated and compared, to check versatility of the elements that can be used on a high-entropy system (Chapter 6).
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