서브메뉴
검색
Electrifying Chemical Transformations and Separations to Valorize Wastewater Nitrogen
Electrifying Chemical Transformations and Separations to Valorize Wastewater Nitrogen
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211153050
- ISBN
- 9798346387442
- DDC
- 621.48
- 서명/저자
- Electrifying Chemical Transformations and Separations to Valorize Wastewater Nitrogen
- 발행사항
- [Sl] : Stanford University, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 338 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-05, Section: A.
- 주기사항
- Advisor: Tarpeh, William.
- 학위논문주기
- Thesis (Ph.D.)--Stanford University, 2024.
- 초록/해제
- 요약Managing the nitrogen cycle has been identified as one of 14 Grand Challenges for Engineering in the 21st century, as defined by the U.S. National Academy of Engineering. Indeed, the U.S. Environmental Protection Agency considers nitrogen pollution "one of the costliest, most difficult environmental problems we face in the 21stcentury." Humanity has profoundly skewed the natural throughput of the nitrogen cycle through Haber-Bosch ammonia synthesis, which outpaces nitrogen removal rates from wastewater. As a result, nitrogen pollution continues to accumulate in the environment, threatening global water security and human health. However, as global populations continue to grow, humanity will require more ammonia than it ever has before.Electrochemical nitrogen recovery from wastewaters offers an avenue for bringing balance back to the nitrogen cycle by directly recovering ammonia from wastewater nitrogen. Two forms of reactive nitrogen in particular compose the majority of nitrogen pollution in wastewaters: ammonia and nitrate. Targeting these two pollutants for ammonia recovery is a key focus of this dissertation. Whereas ammonia requires a selective separation from other wastewater constituents to be recovered as a pure product, nitrate requires selective reduction to ammonia prior to separation. Thus, the work in this dissertation explores techniques for achieving selective electrochemical separations and selective electrochemical reactions.In Chapter 2 explores the use of electrochemical stripping, a unit process combining electrodialysis and membrane stripping, for ammonium sulfate recovery from ammoniarich influent as a function of electrolyte temperature, gas permeable membrane, and influent concentration (30 to 3000 mg N/L). A mass transfer model for nitrogen movement between reactor chambers is developed to yield both descriptive and predictive insights into the effect of operating parameters on nitrogen recovery. The validation of electrochemical stripping as a platform for selectively separating ammonia forms a bedrock for the remainder of this dissertation.Chapters 3-5 consist of studies into electrochemical nitrate reduction to ammonia, with the idea that synthesized ammonia can be recovered with electrochemical stripping. Chapter 3 examines the use of titanium electrodes for nitrate reduction. Under the protic, reducing conditions of nitrate reduction, titanium forms titanium hydride, which possesses distinct physical, chemical, and electronic properties from titanium. The work in this chapter employs synchrotron X-ray characterization to study how different nitrate reduction conditions (applied potential, duration) impact the formation of near-surface titanium hydride, and the impact this altered surface structure may have on nitrate reduction performance. Chapters 4-5 explore the use of the homogeneous electrocatalyst Co(DIM), a cobalt-centered tetra-aza macrocycle, for selective nitrate reduction to ammonia. In Chapter 4, Co(DIM) is incorporated into electrochemical stripping to simultaneously treat nitrate-rich secondary effluent and ammonium-rich reverse osmosis brine. The work demonstrates successful separation of synthesized ammonia from the catalyst and treated water at performance metrics (energy consumption, recovery rate) that matched or outperformed state-of-the-art nitrogen recovery systems. Chapter 5 investigates the reaction mechanisms and kinetics of Co(DIM) through electroanalytical studies. It is shown that prior to nitrate conversion, Co(DIM) must free its axial sites through bromide dissociation coupled with electron transfer. The kinetics of nitrate conversion, including reaction rate constants, turnover frequencies, kinetic isotope effects, and activation parameters, are quantified to benchmark the performance of Co(DIM)-mediated nitrate reduction.
- 일반주제명
- Reactors
- 일반주제명
- Nitrates
- 일반주제명
- Electrons
- 일반주제명
- Electrodes
- 일반주제명
- Water treatment
- 일반주제명
- Chemistry
- 일반주제명
- 21st century
- 일반주제명
- Voltammetry
- 일반주제명
- Chemists
- 일반주제명
- Ammonia
- 일반주제명
- Catalysis
- 일반주제명
- Effluents
- 일반주제명
- Electrocatalysis
- 일반주제명
- Energy consumption
- 일반주제명
- Nitrogen
- 일반주제명
- Atomic physics
- 일반주제명
- Energy
- 일반주제명
- Industrial engineering
- 일반주제명
- Museum studies
- 일반주제명
- Engineering
- 기타저자
- Stanford University.
- 기본자료저록
- Dissertations Abstracts International. 86-05A.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
008250123s2024 us c eng d■001000017164811
■00520250211153050
■006m o d
■007cr#unu||||||||
■020 ▼a9798346387442
■035 ▼a(MiAaPQ)AAI31643305
■035 ▼a(MiAaPQ)Stanfordfk004hm3141
■040 ▼aMiAaPQ▼cMiAaPQ
■0820 ▼a621.48
■1001 ▼aLiu, Matthew Junjie.
■24510▼aElectrifying Chemical Transformations and Separations to Valorize Wastewater Nitrogen
■260 ▼a[Sl]▼bStanford University▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a338 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-05, Section: A.
■500 ▼aAdvisor: Tarpeh, William.
■5021 ▼aThesis (Ph.D.)--Stanford University, 2024.
■520 ▼aManaging the nitrogen cycle has been identified as one of 14 Grand Challenges for Engineering in the 21st century, as defined by the U.S. National Academy of Engineering. Indeed, the U.S. Environmental Protection Agency considers nitrogen pollution "one of the costliest, most difficult environmental problems we face in the 21stcentury." Humanity has profoundly skewed the natural throughput of the nitrogen cycle through Haber-Bosch ammonia synthesis, which outpaces nitrogen removal rates from wastewater. As a result, nitrogen pollution continues to accumulate in the environment, threatening global water security and human health. However, as global populations continue to grow, humanity will require more ammonia than it ever has before.Electrochemical nitrogen recovery from wastewaters offers an avenue for bringing balance back to the nitrogen cycle by directly recovering ammonia from wastewater nitrogen. Two forms of reactive nitrogen in particular compose the majority of nitrogen pollution in wastewaters: ammonia and nitrate. Targeting these two pollutants for ammonia recovery is a key focus of this dissertation. Whereas ammonia requires a selective separation from other wastewater constituents to be recovered as a pure product, nitrate requires selective reduction to ammonia prior to separation. Thus, the work in this dissertation explores techniques for achieving selective electrochemical separations and selective electrochemical reactions.In Chapter 2 explores the use of electrochemical stripping, a unit process combining electrodialysis and membrane stripping, for ammonium sulfate recovery from ammoniarich influent as a function of electrolyte temperature, gas permeable membrane, and influent concentration (30 to 3000 mg N/L). A mass transfer model for nitrogen movement between reactor chambers is developed to yield both descriptive and predictive insights into the effect of operating parameters on nitrogen recovery. The validation of electrochemical stripping as a platform for selectively separating ammonia forms a bedrock for the remainder of this dissertation.Chapters 3-5 consist of studies into electrochemical nitrate reduction to ammonia, with the idea that synthesized ammonia can be recovered with electrochemical stripping. Chapter 3 examines the use of titanium electrodes for nitrate reduction. Under the protic, reducing conditions of nitrate reduction, titanium forms titanium hydride, which possesses distinct physical, chemical, and electronic properties from titanium. The work in this chapter employs synchrotron X-ray characterization to study how different nitrate reduction conditions (applied potential, duration) impact the formation of near-surface titanium hydride, and the impact this altered surface structure may have on nitrate reduction performance. Chapters 4-5 explore the use of the homogeneous electrocatalyst Co(DIM), a cobalt-centered tetra-aza macrocycle, for selective nitrate reduction to ammonia. In Chapter 4, Co(DIM) is incorporated into electrochemical stripping to simultaneously treat nitrate-rich secondary effluent and ammonium-rich reverse osmosis brine. The work demonstrates successful separation of synthesized ammonia from the catalyst and treated water at performance metrics (energy consumption, recovery rate) that matched or outperformed state-of-the-art nitrogen recovery systems. Chapter 5 investigates the reaction mechanisms and kinetics of Co(DIM) through electroanalytical studies. It is shown that prior to nitrate conversion, Co(DIM) must free its axial sites through bromide dissociation coupled with electron transfer. The kinetics of nitrate conversion, including reaction rate constants, turnover frequencies, kinetic isotope effects, and activation parameters, are quantified to benchmark the performance of Co(DIM)-mediated nitrate reduction.
■590 ▼aSchool code: 0212.
■650 4▼aReactors
■650 4▼aNitrates
■650 4▼aElectrons
■650 4▼aElectrodes
■650 4▼aWater treatment
■650 4▼aChemistry
■650 4▼a21st century
■650 4▼aVoltammetry
■650 4▼aChemists
■650 4▼aAmmonia
■650 4▼aCatalysis
■650 4▼aEffluents
■650 4▼aElectrocatalysis
■650 4▼aEnergy consumption
■650 4▼aNitrogen
■650 4▼aAtomic physics
■650 4▼aEnergy
■650 4▼aEnvironmental engineering
■650 4▼aIndustrial engineering
■650 4▼aMuseum studies
■650 4▼aEngineering
■690 ▼a0485
■690 ▼a0748
■690 ▼a0791
■690 ▼a0775
■690 ▼a0546
■690 ▼a0730
■690 ▼a0537
■71020▼aStanford University.
■7730 ▼tDissertations Abstracts International▼g86-05A.
■790 ▼a0212
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17164811▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.


