國立高雄大學圖資館 |

Electrifying Chemicals, Fuels, and Building Materials Production: Catalyst Design, Operation Optimization, and Application Expansion /

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Electrifying Chemicals, Fuels, and Building Materials Production: Catalyst Design, Operation Optimization, and Application Expansion /Xiao Kun Lu.
作者:	Lu, Xiao Kun,
面頁冊數:	1 electronic resource (413 pages)
附註:	Source: Dissertations Abstracts International, Volume: 86-09, Section: B.
附註:	Advisors: Seitz, Linsey C. Committee members: Notestein, Justin M.; Sargent, Edward H.; Schweitzer, Neil M.
Contained By:	Dissertations Abstracts International86-09B.
標題:	Chemical engineering.
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31839600
ISBN:	9798310150089

Electrifying Chemicals, Fuels, and Building Materials Production: Catalyst Design, Operation Optimization, and Application Expansion /
Lu, Xiao Kun,

Electrifying Chemicals, Fuels, and Building Materials Production: Catalyst Design, Operation Optimization, and Application Expansion /Xiao Kun Lu. - 1 electronic resource (413 pages)

Source: Dissertations Abstracts International, Volume: 86-09, Section: B.

Increasing energy demand in the midst of climate crisis caused by anthropogenic greenhouse gas emissions calls for rapid technological advances towards energy transition to renewable sources. Development and integration of efficient energy storage mechanisms such as Power-to-X addresses intermittency of renewable energy sources such as wind and solar. Electrocatalysis is a Power-to-X technology that converts electrical energy to chemical energy and is capable of valorizing abundant small molecules to fuels and chemical commodities. Currently, barriers to commercialization of electrocatalytic processes include inadequate performance, stability, and integration. This dissertation focuses on electrolyzer engineering, operational method optimization, catalyst design, and technological expansion to improve the performance, stability, and ultimately, scalability of electrocatalytic processes.First, a literature review of recent progress in understanding and tuning the effects of electrolyzer operating parameters on performance and stability of electrochemical CO(2) reduction (ECR) is presented to provide a comprehensive assessment of the complexity and interplay of operating parameters. I selected the most impactful parameters, including (1) electrolyzer geometry, (2) reactant availability, (3) electrolyte choice, (4) hydrophobicity treatments, (5) conductivity modifications, (6) operating temperature, and (7) electrochemical protocols, and provided insights on the origin of interconnectedness between these parameters. Finally, I offered perspectives on the future research directions of the field for development of ECR technologies.Following this overview and discussion of electrochemical protocols for reactor testing, I tested the enhancement effect of pulsed electrolysis (PE) for ECR at industrially relevant current density (>200 mA/cm2) in a zero-gap membrane electrode assembly (MEA) electrolyzer. Three types of binders, including cationic ionomer, anionic ionomer, and hydrophobic fluoropolymer were tested under PE operations. In situ surface enhanced Raman spectroscopy was performed using a gas diffusion electrode (GDE)-based spectroelectrochemical cell to understand the local reaction environment during PE operation. Lastly, the effect of PE operation on the iridium-based anode was assessed through a durability test.Next, I turn to catalyst design to improve the performance of ECR. The best catalyst for ECR towards multi-carbon products, copper, has been previously modified by oxide-derived methods to expose highly active undercoordinated sites. However, due to the highly reductive alkaline conditions of GDE flow cells, undercoordinated sites are typically reduced to the common 12-coordinated sites of face center cubic metallic copper. I synthesized strontium copper oxide catalysts and probed the chemical coordination of copper with ex situ and in situ X-ray absorption spectroscopy, which proves the stabilization of undercoordinated sites due to the presence of strontium in correlation with its enhanced production of desired multi-carbon products.Applying similar principles to the 2e- oxygen reduction reaction (ORR), we performed electrolyzer engineering to reach 400 mA/cm2 in a dual MEA solid electrolyte electrolyzer to understand the effect of reactor design and electrode structure. We study the transport of O2 and water to the electrode by varying the catalyst layer thickness, surface hydrophobicity, and O2 feed concentration. We also consider the transport of our product species in the solid electrolyte layer with varying flow rates and operational modes. By correlating the changes in reactant/product mass transport to performance and stability, we provide suggestions on operation at high current density in pre-industrial scale electrolyzers.In addition to electrolyzer engineering, catalyst design for 2e- ORR could significantly improve performance and bring down the cost of electrocatalytic H2O2 production. Carbon-based materials have been extensively studied for electrocatalytic processes due to their low cost, tunability, and abundance. The structural-functional relationship of heteroatom-doped carbon-based catalysts for 2e- ORR in neutral conditions remain largely unexplored. We control the functional groups of synthesized carbon-based catalysts by varying the pyrolysis temperature and characterize them with a suite of laser-based and X-ray based techniques to draw conclusions on the desired carbon, boron, and nitrogen composition and functional groups.Finally, integration of electrocatalytic systems into existing industrial processes enables decarbonization of various sectors, as well as increasing the economic feasibility of electrocatalytic processes. We utilize the water dissociation of alkaline hydrogen and oxygen evolution reactions (HER and OER) to produce acid and base for production of carbon-negative supplementary cementitious materials. Current production of Portland cement produces 0.9 kg-CO2/kg-cement due to limestone decomposition and combustion of fossil fuels. By weathering and mineralizing CO2 to calcium silicates electrochemically, we produce carbon-negative CaCO3, SiO2, H2, and O2 that can replace limestone, coal fly ash, and fossil fuels during cement production for decarbonization of this gigatons scale industry.In summary, this dissertation presents studies aimed at accelerating the commercialization of electrocatalytic processes by improving their performance, stability, and adoptability.

English

ISBN: 9798310150089Subjects--Topical Terms:

206267
Chemical engineering.
Subjects--Index Terms:

Electrocatalysis

Electrifying Chemicals, Fuels, and Building Materials Production: Catalyst Design, Operation Optimization, and Application Expansion /
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This dissertation focuses on electrolyzer engineering, operational method optimization, catalyst design, and technological expansion to improve the performance, stability, and ultimately, scalability of electrocatalytic processes.First, a literature review of recent progress in understanding and tuning the effects of electrolyzer operating parameters on performance and stability of electrochemical CO(2) reduction (ECR) is presented to provide a comprehensive assessment of the complexity and interplay of operating parameters. I selected the most impactful parameters, including (1) electrolyzer geometry, (2) reactant availability, (3) electrolyte choice, (4) hydrophobicity treatments, (5) conductivity modifications, (6) operating temperature, and (7) electrochemical protocols, and provided insights on the origin of interconnectedness between these parameters. Finally, I offered perspectives on the future research directions of the field for development of ECR technologies.Following this overview and discussion of electrochemical protocols for reactor testing, I tested the enhancement effect of pulsed electrolysis (PE) for ECR at industrially relevant current density (>200 mA/cm2) in a zero-gap membrane electrode assembly (MEA) electrolyzer. Three types of binders, including cationic ionomer, anionic ionomer, and hydrophobic fluoropolymer were tested under PE operations. In situ surface enhanced Raman spectroscopy was performed using a gas diffusion electrode (GDE)-based spectroelectrochemical cell to understand the local reaction environment during PE operation. Lastly, the effect of PE operation on the iridium-based anode was assessed through a durability test.Next, I turn to catalyst design to improve the performance of ECR. The best catalyst for ECR towards multi-carbon products, copper, has been previously modified by oxide-derived methods to expose highly active undercoordinated sites. However, due to the highly reductive alkaline conditions of GDE flow cells, undercoordinated sites are typically reduced to the common 12-coordinated sites of face center cubic metallic copper. I synthesized strontium copper oxide catalysts and probed the chemical coordination of copper with ex situ and in situ X-ray absorption spectroscopy, which proves the stabilization of undercoordinated sites due to the presence of strontium in correlation with its enhanced production of desired multi-carbon products.Applying similar principles to the 2e- oxygen reduction reaction (ORR), we performed electrolyzer engineering to reach 400 mA/cm2 in a dual MEA solid electrolyte electrolyzer to understand the effect of reactor design and electrode structure. We study the transport of O2 and water to the electrode by varying the catalyst layer thickness, surface hydrophobicity, and O2 feed concentration. We also consider the transport of our product species in the solid electrolyte layer with varying flow rates and operational modes. By correlating the changes in reactant/product mass transport to performance and stability, we provide suggestions on operation at high current density in pre-industrial scale electrolyzers.In addition to electrolyzer engineering, catalyst design for 2e- ORR could significantly improve performance and bring down the cost of electrocatalytic H2O2 production. Carbon-based materials have been extensively studied for electrocatalytic processes due to their low cost, tunability, and abundance. The structural-functional relationship of heteroatom-doped carbon-based catalysts for 2e- ORR in neutral conditions remain largely unexplored. We control the functional groups of synthesized carbon-based catalysts by varying the pyrolysis temperature and characterize them with a suite of laser-based and X-ray based techniques to draw conclusions on the desired carbon, boron, and nitrogen composition and functional groups.Finally, integration of electrocatalytic systems into existing industrial processes enables decarbonization of various sectors, as well as increasing the economic feasibility of electrocatalytic processes. We utilize the water dissociation of alkaline hydrogen and oxygen evolution reactions (HER and OER) to produce acid and base for production of carbon-negative supplementary cementitious materials. Current production of Portland cement produces 0.9 kg-CO2/kg-cement due to limestone decomposition and combustion of fossil fuels. By weathering and mineralizing CO2 to calcium silicates electrochemically, we produce carbon-negative CaCO3, SiO2, H2, and O2 that can replace limestone, coal fly ash, and fossil fuels during cement production for decarbonization of this gigatons scale industry.In summary, this dissertation presents studies aimed at accelerating the commercialization of electrocatalytic processes by improving their performance, stability, and adoptability.
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