東華大學圖書館 |

Designing Electrochemical Solar Fuels to Operate in Real-World, Variable Conditions /

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Designing Electrochemical Solar Fuels to Operate in Real-World, Variable Conditions // Kyra Muk Kam Yap.
作者:	Yap, Kyra Muk Kam,
面頁冊數:	1 electronic resource (334 pages)
附註:	Source: Dissertations Abstracts International, Volume: 86-10, Section: B.
Contained By:	Dissertations Abstracts International86-10B.
標題:	Organic chemicals. -
電子資源:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31974618
ISBN:	9798311960823

Designing Electrochemical Solar Fuels to Operate in Real-World, Variable Conditions /
Yap, Kyra Muk Kam,

Designing Electrochemical Solar Fuels to Operate in Real-World, Variable Conditions /Kyra Muk Kam Yap. - 1 electronic resource (334 pages)

Source: Dissertations Abstracts International, Volume: 86-10, Section: B.

Rising greenhouse gas (GHG) emissions have caused a shift in the energy landscape towards electrification. With this electrification comes the need to decarbonize adjacent, energy-intensive sectors, such as the chemicals industry. Globally, the chemicals industry accounts for ~30% of GHG emissions, due to high energy consumption to drive chemical conversions at elevated temperatures and pressures, transportation of chemical feedstocks to centralized, large-scale processing facilities, and separation processes that occur under harsh operating conditions. Electrochemical technologies have emerged as a potential contender to decarbonize the chemical industry by utilizing electricity drawn directly from renewable energy to drive chemical conversions.Electrochemical solar fuels are a further integrated form of electrochemical conversion where the solar absorber (i.e., photovoltaic) is directly integrated to the electrochemical cell, allowing for decentralized, off-grid operation of chemical conversions. The unique design of solar fuels technologies allows for tackling of GHG emissions associated with long-haul chemical transportation, in addition to reducing the carbon footprint of the chemical conversion step. Additionally, the off-grid nature of electrochemical solar fuels removes the additional electric load and regulatory burden of connecting large-scale electrochemical systems to the electricity grid.Unique challenges arise for the outdoor operation of affordable, efficient, electrochemical solar fuels technology. These challenges include the variable nature of outdoor conditions, including fluctuations in incident irradiation and environmental conditions which can affect the electrochemical performance of the solar fuels device.Additional challenges include generating higher value products from waste feed streams and improving affordability by utilizing impure, accessible water sources. This thesis will begin to tackle some of these challenges by investigating the real-world, outdoor operation of electrochemical solar fuels technology through the lens of two reactions.We employed electrochemical CO2reduction (CO2R) to study diurnal consequences on selectivity and activity, as CO2R systems generate multiple products and have product distributions which are highly dependent on the operating conditions at the electrocatalytic interface (Chapters 2 - 4). CO2R is a valuable electrochemical technology because of its ability to convert waste CO2into valuable products, offering a pathway to circularization of the carbon economy. However, achieving stable CO2R product generation under diurnal conditions is an ongoing challenge, as CO2R is highly sensitive to changes in electrochemical potential, temperature, and the composition of the reaction microenvironment. Beyond the study selectivity and activity under diurnal conditions, we investigated the coupling of solar-driven CO2R reactors in tandem catalytic process for the conversion of larger hydrocarbon products (Chapter 6). Finally, towards the development of affordable CO2R systems, we studied the role of abundant divalent cationic impurities on CO2R performance (Chapter 7).We utilized the hydrogen evolution reaction (HER) to study the effect of diurnal irradiation on the stability of electrocatalytic protective layers for HER photoelectrodes (Chapter 5). Using a mixture of in situcharacterization techniques and spectroscopic electrode analysis, we identified mechanisms of degradation of the electrode surface and electrochemical performance which are observed under simulated diurnal conditions. We proposed methods to prevent this degradation and to design stable photoelectrode protective layers that can be efficiently integrated to semiconductor components.The combination of studies conducted in this thesis provides insight into the realworld operation of electrochemical solar fuels devices. We investigated the unique conditions which arise under diurnal operating conditions and identify methods to engineer resilience in electrochemical solar fuels systems against some of these challenges. Additionally, we provided insight into the design of electrochemical systems for resistance to impure water sources and engineer tandem solar fuels processes for further upgrading of CO2-derived products. This work provides key insights into the future of electrochemical solar fuels as a technology at the forefront of the sustainable chemicals industry.

English

ISBN: 9798311960823Subjects--Topical Terms:

3560375
Organic chemicals.

Designing Electrochemical Solar Fuels to Operate in Real-World, Variable Conditions /
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520 $a Rising greenhouse gas (GHG) emissions have caused a shift in the energy landscape towards electrification. With this electrification comes the need to decarbonize adjacent, energy-intensive sectors, such as the chemicals industry. Globally, the chemicals industry accounts for ~30% of GHG emissions, due to high energy consumption to drive chemical conversions at elevated temperatures and pressures, transportation of chemical feedstocks to centralized, large-scale processing facilities, and separation processes that occur under harsh operating conditions. Electrochemical technologies have emerged as a potential contender to decarbonize the chemical industry by utilizing electricity drawn directly from renewable energy to drive chemical conversions.Electrochemical solar fuels are a further integrated form of electrochemical conversion where the solar absorber (i.e., photovoltaic) is directly integrated to the electrochemical cell, allowing for decentralized, off-grid operation of chemical conversions. The unique design of solar fuels technologies allows for tackling of GHG emissions associated with long-haul chemical transportation, in addition to reducing the carbon footprint of the chemical conversion step. Additionally, the off-grid nature of electrochemical solar fuels removes the additional electric load and regulatory burden of connecting large-scale electrochemical systems to the electricity grid.Unique challenges arise for the outdoor operation of affordable, efficient, electrochemical solar fuels technology. These challenges include the variable nature of outdoor conditions, including fluctuations in incident irradiation and environmental conditions which can affect the electrochemical performance of the solar fuels device.Additional challenges include generating higher value products from waste feed streams and improving affordability by utilizing impure, accessible water sources. This thesis will begin to tackle some of these challenges by investigating the real-world, outdoor operation of electrochemical solar fuels technology through the lens of two reactions.We employed electrochemical CO2reduction (CO2R) to study diurnal consequences on selectivity and activity, as CO2R systems generate multiple products and have product distributions which are highly dependent on the operating conditions at the electrocatalytic interface (Chapters 2 - 4). CO2R is a valuable electrochemical technology because of its ability to convert waste CO2into valuable products, offering a pathway to circularization of the carbon economy. However, achieving stable CO2R product generation under diurnal conditions is an ongoing challenge, as CO2R is highly sensitive to changes in electrochemical potential, temperature, and the composition of the reaction microenvironment. Beyond the study selectivity and activity under diurnal conditions, we investigated the coupling of solar-driven CO2R reactors in tandem catalytic process for the conversion of larger hydrocarbon products (Chapter 6). Finally, towards the development of affordable CO2R systems, we studied the role of abundant divalent cationic impurities on CO2R performance (Chapter 7).We utilized the hydrogen evolution reaction (HER) to study the effect of diurnal irradiation on the stability of electrocatalytic protective layers for HER photoelectrodes (Chapter 5). Using a mixture of in situcharacterization techniques and spectroscopic electrode analysis, we identified mechanisms of degradation of the electrode surface and electrochemical performance which are observed under simulated diurnal conditions. We proposed methods to prevent this degradation and to design stable photoelectrode protective layers that can be efficiently integrated to semiconductor components.The combination of studies conducted in this thesis provides insight into the realworld operation of electrochemical solar fuels devices. We investigated the unique conditions which arise under diurnal operating conditions and identify methods to engineer resilience in electrochemical solar fuels systems against some of these challenges. Additionally, we provided insight into the design of electrochemical systems for resistance to impure water sources and engineer tandem solar fuels processes for further upgrading of CO2-derived products. This work provides key insights into the future of electrochemical solar fuels as a technology at the forefront of the sustainable chemicals industry.
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