Expanding Reductive Chemistry and Oxidation State Diversity within the Synthetic Chemistry of the Rare-Earth Metals

扩大稀土金属合成化学中的还原化学和氧化态多样性

• 批准号: 1855328
• 负责人: William Evans
• 金额: $ 59.4万
• 依托单位: University of California-Irvine
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-08-01 至 2022-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1855328&HistoricalAwards=false
• 关键词: Expanding; Reductive; Chemistry; Oxidation; State

Professor William J. Evans at the University of California, Irvine, is supported by the Chemical Synthesis Program of the Chemistry Division at NSF. This research addresses chemical reactions of rare-earth elements. Rare-earth elements have been designated critical national resources due to their many technological applications. They are important in magnetism and quantum computing - technologies that have broad potential applications. The project also pursues applications including the development of the smallest, most efficient, magnets, called single-molecule magnets. In addition, students are trained in the use and applications of strategic resources. A component of the project also involves an outreach program to middle and high schools to expose students to rare earths elements, their applications, and the value of scientific research. The chemistry of praseodymium(II), gadolinium(II), terbium(II), holmium(II), erbium(II), and lutetium(II), is being explored to evaluate the special chemical reactions that can arise from their unexpected 4fn5d1 electron configurations. These electron configurations differ from traditional +2 oxidation states of the lanthanide metals (4fn+1 configurations) and could form the basis for new fundamental types of redox chemistry. The chemistry of the new rare earth ion, yttrium(II) (4d1 configuration) is also being studied for comparison. New series of complexes of these +2 ions are synthesized and their reactivity and magnetic and spectroscopic properties are investigated. As these compounds are photoactive diradicals, they present intriguing new options in synthesis, magnetism, and small molecule activation. Among other applications, the development of quantum bits, or qubits, is being pursued.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

加利福尼亚大学尔湾分校的威廉·J·埃文斯教授得到了NSF化学分部的化学合成计划的支持。这项研究解决了稀土元件的化学反应。 由于其许多技术应用，稀有地球元素已被指定为重要的国家资源。它们在具有广泛潜在应用的磁性和量子计算中很重要。该项目还追求应用程序，包括开发最小，最有效的磁铁，称为单分子磁铁。 此外，对学生进行了战略资源的使用和应用培训。该项目的一个组成部分还涉及向中学和高中进行推广计划，以使学生了解稀土元素，其应用以及科学研究的价值。 正在探索praseodymium（II），Gadolinium（II），Terbium（II），Holmium（ii），Erbium（ii）和Lutetium（ii）的化学，以评估其意外的4FN5D1电子配置可能引起的特殊化学反应。 这些电子构型不同于传统+2金属的+2氧化态（4fn +1构型），并且可能构成新型氧化还原化学类型的基础。 还研究了新稀土离子YTTrium（II）（4D1构型）的化学性质进行比较。 这些+2离子的新复合物已合成，并研究了它们的反应性以及磁性和光谱特性。由于这些化合物是光活性的，因此它们提出了合成，磁性和小分子激活方面有趣的新选择。 除其他应用外，还将追求量子位或量子位的开发。该奖项反映了NSF的法定任务，并使用基金会的知识分子优点和更广泛的影响评估标准，被认为值得通过评估来获得支持。

项目成果

2.2.2-Cryptand as a bidentate ligand in rare-earth metal chemistry

2.2.2-稀土金属化学中作为双齿配体的穴状配体

• DOI: 10.1039/d0qi00746c
• 发表时间: 2020
• 期刊: Inorganic Chemistry Frontiers
• 影响因子: 7
• 作者: Chung, Amanda B.;Huh, Daniel N.;Ziller, Joseph W.;Evans, William J.
• 通讯作者: Evans, William J.

Reductive cleavage of N , N ′-di- tert -butylcarbodiimide generates tert -butylcyanamide ligands, (Me 3 CNCN) − , that bind potassium both end-on and side-on in the same single crystal

N , N α-二叔丁基碳二亚胺的还原裂解生成叔丁基氰酰胺配体 (Me 3 CNCN) α ，该配体在同一单晶中以端接和侧接方式结合钾

• DOI: 10.1107/s205698902000732x
• 发表时间: 2020
• 期刊: Acta Crystallographica Section E Crystallographic Communications
• 作者: Chung, Amanda B.;Ziller, Joseph W.;Evans, William J.
• 通讯作者: Evans, William J.

Optimizing Alkali Metal (M) and Chelate (L) Combinations for the Synthesis and Stability of [M(L)][(C 5 H 4 SiMe 3 ) 3 Y] Yttrium(II) Complexes

优化碱金属 (M) 和螯合物 (L) 组合以促进 [M(L)][(C 5 H 4 SiMe 3 ) 3 Y] 钇(II) 配合物的合成和稳定性

• DOI: 10.1021/acs.organomet.1c00379
• 发表时间: 2021
• 期刊: Organometallics
• 影响因子: 2.8
• 作者: Moore, William N.;Ziller, Joseph W.;Evans, William J.
• 通讯作者: Evans, William J.

Evaluating electrochemical accessibility of 4f n 5d 1 and 4f n+1 Ln( ii ) ions in (C 5 H 4 SiMe 3 ) 3 Ln and (C 5 Me 4 H) 3 Ln complexes

评估 (C 5 H 4 SiMe 3 ) 3 Ln 和 (C 5 Me 4 H) 3 Ln 配合物中 4f n 5d 1 和 4f n 1 Ln( ii ) 离子的电化学可达性

• DOI: 10.1039/d1dt02427b
• 发表时间: 2021
• 期刊: Dalton Transactions
• 影响因子: 4
• 作者: Trinh, Michael T.;Wedal, Justin C.;Evans, William J.
• 通讯作者: Evans, William J.

A 9.2-GHz clock transition in a Lu(II) molecular spin qubit arising from a 3,467-MHz hyperfine interaction

• DOI: 10.1038/s41557-022-00894-4
• 发表时间: 2022-03-14
• 期刊: NATURE CHEMISTRY
• 影响因子: 21.8
• 作者: Kundu, Krishnendu;White, Jessica R. K.;Hill, Stephen
• 通讯作者: Hill, Stephen