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Synthesis and Crystal Growth of 2D Layered Metal Chalophosphate Materials Using P2Q5 Reactive Fluxes
Synthesis and Crystal Growth of 2D Layered Metal Chalophosphate Materials Using P2Q5 Reactive Fluxes
상세정보
- 자료유형
- 학위논문 서양
- 최종처리일시
- 20250211152714
- ISBN
- 9798384016434
- DDC
- 540
- 저자명
- Qian, Eric Kun.
- 서명/저자
- Synthesis and Crystal Growth of 2D Layered Metal Chalophosphate Materials Using P2Q5 Reactive Fluxes
- 발행사항
- [Sl] : Northwestern University, 2024
- 발행사항
- Ann Arbor : ProQuest Dissertations & Theses, 2024
- 형태사항
- 300 p
- 주기사항
- Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
- 주기사항
- Advisor: Kanatzidis, Mercouri G.
- 학위논문주기
- Thesis (Ph.D.)--Northwestern University, 2024.
- 초록/해제
- 요약This thesis explores 2D layered chalcophosphates, with a focus on synthetic strategy. This class of materials has a particularly wide compositional flexibility in the metal cations that can be accommodated; as such, mastering the synthetic strategies required to unlock its full compositional range will in turn allow the synthesis and study of many fascinating electronically and magnetically active members of the family.To begin, a systematic study of the known monometallic and bimetallic 2D layered selenophosphates was done, to investigate the crystal growth behavior of each of these compounds synthesized in a high-concentration, high-temperature P2Se5 reactive flux. It was found that not only do most of the known compounds rapidly grow crystals in such a flux, but that the P2Se5 reactive flux significantly enhanced the incorporation of multiple metal centers into the material, unlocking the potential for new bimetallic selenophosphate discovery.This insight was then applied towards the synthesis of LiGaP2Se6. Prior to this discovery, only one other Li-containing 2D layered selenophosphate had been reported. Additionally, Ga had already been designated as a problem cation to work with; attempts to synthesize CuGaP2Se6 had been reported as failure, and β-AgGaP2Se6 was found to be thermodynamically unstable. By pre-synthesizing a metal alloy Li-Ga precursor, then dissolving that Li-Ga alloy in a reactive P2Se5 reactive flux, crystals of LiGaP2Se6 were grown and characterized. This was then followed by the synthesis of LiCrP2Se6. CuCrP2Se6, AgCrP2Se6, and CuInP2Se6 were already identified as fascinating compounds that underwent ferrielectric, antiferroelectric, or antiferromagnetic ordering. The successful syntheses of LiInP2Se6 and LiGaP2Se6 indicated that Li-based analogues of these electronically and magnetically active materials could be synthesized and studied for further elucidation of structure-property relationships. Crystals of LiCrP2Se6 were grown in a reactive P2Se5 flux and magnetically characterized.Lastly, these studies concluded with the crystallographic refinement of LiInP2S6. Multiple crystal growth methods were explored and documented, including polycrystalline stoichiometric synthesis, large crystal synthesis using P2S5 reactive flux, and self-transport by reaction at increased temperatures. Although previously reported as centrosymmetric, second harmonic generation and exhaustive refinement of a single crystal data set pointed towards a chiral growth habit. These materials were then explored for ion exchange capabilities - with potential applications in wastewater remediation - and found to fully exchange all alkali cation content within the course of 30 minutes.Overall, this journey demonstrated the importance of using thorough experimentation, exploration, and intuition to triumph over synthetic obstacles. By discovering and developing synthetic tools, fascinating new materials can be discovered and studied for future technological innovations.
- 일반주제명
- Chemistry
- 일반주제명
- Applied physics
- 일반주제명
- Engineering
- 일반주제명
- Materials science
- 키워드
- Crystal growth
- 키워드
- Reactive fluxes
- 기타저자
- Northwestern University Chemistry
- 기본자료저록
- Dissertations Abstracts International. 86-04B.
- 전자적 위치 및 접속
- 로그인 후 원문을 볼 수 있습니다.
MARC
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■006m o d
■007cr#unu||||||||
■020 ▼a9798384016434
■035 ▼a(MiAaPQ)AAI31488918
■040 ▼aMiAaPQ▼cMiAaPQ
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■1001 ▼aQian, Eric Kun.▼0(orcid)0000-0003-2314-7569
■24510▼aSynthesis and Crystal Growth of 2D Layered Metal Chalophosphate Materials Using P2Q5 Reactive Fluxes
■260 ▼a[Sl]▼bNorthwestern University▼c2024
■260 1▼aAnn Arbor▼bProQuest Dissertations & Theses▼c2024
■300 ▼a300 p
■500 ▼aSource: Dissertations Abstracts International, Volume: 86-04, Section: B.
■500 ▼aAdvisor: Kanatzidis, Mercouri G.
■5021 ▼aThesis (Ph.D.)--Northwestern University, 2024.
■520 ▼aThis thesis explores 2D layered chalcophosphates, with a focus on synthetic strategy. This class of materials has a particularly wide compositional flexibility in the metal cations that can be accommodated; as such, mastering the synthetic strategies required to unlock its full compositional range will in turn allow the synthesis and study of many fascinating electronically and magnetically active members of the family.To begin, a systematic study of the known monometallic and bimetallic 2D layered selenophosphates was done, to investigate the crystal growth behavior of each of these compounds synthesized in a high-concentration, high-temperature P2Se5 reactive flux. It was found that not only do most of the known compounds rapidly grow crystals in such a flux, but that the P2Se5 reactive flux significantly enhanced the incorporation of multiple metal centers into the material, unlocking the potential for new bimetallic selenophosphate discovery.This insight was then applied towards the synthesis of LiGaP2Se6. Prior to this discovery, only one other Li-containing 2D layered selenophosphate had been reported. Additionally, Ga had already been designated as a problem cation to work with; attempts to synthesize CuGaP2Se6 had been reported as failure, and β-AgGaP2Se6 was found to be thermodynamically unstable. By pre-synthesizing a metal alloy Li-Ga precursor, then dissolving that Li-Ga alloy in a reactive P2Se5 reactive flux, crystals of LiGaP2Se6 were grown and characterized. This was then followed by the synthesis of LiCrP2Se6. CuCrP2Se6, AgCrP2Se6, and CuInP2Se6 were already identified as fascinating compounds that underwent ferrielectric, antiferroelectric, or antiferromagnetic ordering. The successful syntheses of LiInP2Se6 and LiGaP2Se6 indicated that Li-based analogues of these electronically and magnetically active materials could be synthesized and studied for further elucidation of structure-property relationships. Crystals of LiCrP2Se6 were grown in a reactive P2Se5 flux and magnetically characterized.Lastly, these studies concluded with the crystallographic refinement of LiInP2S6. Multiple crystal growth methods were explored and documented, including polycrystalline stoichiometric synthesis, large crystal synthesis using P2S5 reactive flux, and self-transport by reaction at increased temperatures. Although previously reported as centrosymmetric, second harmonic generation and exhaustive refinement of a single crystal data set pointed towards a chiral growth habit. These materials were then explored for ion exchange capabilities - with potential applications in wastewater remediation - and found to fully exchange all alkali cation content within the course of 30 minutes.Overall, this journey demonstrated the importance of using thorough experimentation, exploration, and intuition to triumph over synthetic obstacles. By discovering and developing synthetic tools, fascinating new materials can be discovered and studied for future technological innovations.
■590 ▼aSchool code: 0163.
■650 4▼aChemistry
■650 4▼aApplied physics
■650 4▼aEngineering
■650 4▼aMaterials science
■653 ▼aCrystal growth
■653 ▼aReactive fluxes
■653 ▼aStructure-property relationships
■653 ▼aStoichiometric synthesis
■690 ▼a0485
■690 ▼a0794
■690 ▼a0537
■690 ▼a0215
■71020▼aNorthwestern University▼bChemistry.
■7730 ▼tDissertations Abstracts International▼g86-04B.
■790 ▼a0163
■791 ▼aPh.D.
■792 ▼a2024
■793 ▼aEnglish
■85640▼uhttp://www.riss.kr/pdu/ddodLink.do?id=T17163484▼nKERIS▼z이 자료의 원문은 한국교육학술정보원에서 제공합니다.
