低氧化态碱土金属有机化学概述

doi:10.6023/A24100325

化学学报 ›› 2025, Vol. 83 ›› Issue (2): 139-151.DOI: 10.6023/A24100325 上一篇下一篇

综述

低氧化态碱土金属有机化学概述

陈荣, 魏保生^*()

中南大学化学化工学院长沙 410083

投稿日期:2024-10-28 发布日期:2024-12-24

作者简介:

陈荣, 2023年获延安大学学士学位, 同年保送至中南大学化学化工学院攻读硕士学位, 师从魏保生副教授, 目前主要研究主族金属有机化学.

魏保生, 副教授, 博士生导师. 2012年获山东大学学士学位, 2017年获北京大学博士学位(导师: 席振峰院士、张文雄教授), 2018~2021年在德国慕尼黑大学化学系从事博士后研究(合作导师: Paul Knochel教授), 2022年起加入中南大学化学化工学院开展教学科研工作. 主要研究金属有机化学、有机合成与催化化学, 近年来在Acc. Chem. Res.、J. Am. Chem. Soc.、Angew. Chem. Int. Ed.等国内外权威期刊发表论文20余篇, 应邀撰写1个英文专著章节, 现担任国际学术期刊Chem. Synth.青年编委, 入选中南大学首批升华学者计划和湖南省高层次人才引进项目.

基金资助:
国家自然科学基金(22271312); 中南大学启动基金和中南大学创新驱动计划项目(2023CXQD047)

Overview on Low-oxidation-state Alkaline Earth Organometallic Chemistry

Rong Chen, Baosheng Wei()

College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China

Received:2024-10-28 Published:2024-12-24
Contact: *E-mail: bswei@csu.edu.cn
Supported by:
National Natural Science Foundation of China(22271312); start-up funds of Central South University and the Central South University Innovation-Driven Research Programme(2023CXQD047)

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摘要/Abstract

低氧化态主族元素化学在主族化学中占据重要地位, 该领域的研究成果不仅可以丰富化学键理论内涵, 而且在金属有机及催化、小分子活化与转化等方面都具有重要意义. 相比于低氧化态p区元素化学, s区中碱土金属元素因电负性较低极易失去两个价电子形成稳定的＋2氧化态化合物, 但较难形成具有高活性和强还原性的低氧化态物种, 因此低氧化态碱土金属有机化学的研究充满挑战. 本文概述了低氧化态碱土金属有机化学的发展历程, 简要描述了已发展较为成熟的低氧化态镁化学, 全面介绍了近期取得显著进展的低氧化态铍化学, 重点强调了亟待突破的低氧化态钙、锶和钡化学.

关键词: 低氧化态, 碱土金属, 金属有机化学, 铍, 镁, 钙

The chemistry of main group elements with low oxidation states occupies an important position in main group chemistry. Research results in this field can not only enrich the theoretical connotation of chemical bonding, but also have great significance in organometallic chemistry and catalysis, small molecule activation and transformation, etc. Compared with the chemistry of low-oxidation-state p-block elements, the s-block alkaline earth metal elements with low electronegativity can easily lose two valence electrons to form stable ＋2 oxidation state compounds, but it is more difficult to form low-oxidation-state species with relatively low stability and strong reducing property. Therefore, the study on low-oxidation-state alkaline earth organometallic chemistry is full of challenges. This review outlines the development history of low-oxidation-state alkaline earth organometallic chemistry, briefly describes the relatively mature low-oxidation-state magnesium chemistry, comprehensively introduces the low-oxidation-state beryllium chemistry that has recently made significant progress, highlights the low-oxidation-state calcium, strontium, and barium chemistry that still needs urgent breakthrough.

Key words: low oxidation state, alkaline earth metal, organometallic chemistry, beryllium, magnesium, calcium

引用此文

陈荣, 魏保生. 低氧化态碱土金属有机化学概述[J]. 化学学报, 2025, 83(2): 139-151.

Rong Chen, Baosheng Wei. Overview on Low-oxidation-state Alkaline Earth Organometallic Chemistry[J]. Acta Chimica Sinica, 2025, 83(2): 139-151.

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图/表 32

图1. 首例可稳定分离的Mg(I)配合物

Figure 1. The first stable and isolable magnesium(I) complex

图2. 双阴离子配体支持的Mg(I)二聚体的合成

Figure 2. Synthesis of the dianionic magnesium(I) dimers

图3. 常见还原剂的氧化还原电位

Figure 3. Redox potentials of common reductants

图4. Mg(I)二聚体对有机底物的双电子还原

Figure 4. Two-electron reduction of organic substrates by magnesium(I) dimers

图5. Mg(I)二聚体对有机底物的单电子还原

Figure 5. One-electron reduction of organic substrates by magnesium(I) dimers

图6. Mg(I)配合物催化醛酮的硅氰化反应

Figure 6. Magnesium(I)-catalyzed cyanosilylation of ketones or aldehydes

图7. 新型配体支持的Mg(I)二聚体配合物的合成及反应性

Figure 7. Synthesis and reactivity of magnesium(I) complex with a new ligand

图8. 镁-偶氮阴离子自由基配合物的合成及反应性

Figure 8. Synthesis and reactivity of magnesium-azobenzenyl anion radical complex

图9. Mg(I)自由基化合物的原位合成及反应性

Figure 9. In situ synthesis and reactivity of magnesium(I) radical compound

图10. Mg(II)-自由基双阴离子配合物的合成

Figure 10. Synthesis of magnesium(II)-radical dianion complex

图11. 球磨法制备不稳定的Mg(I)自由基化合物

Figure 11. Preparation of unstable magnesium(I) free radical compounds by ball milling

图12. 首例Mg(0)配合物的合成及反应性研究

Figure 12. Synthesis and reactivity of the first magnesium(0) complex

图13. 首例镁-氮气配合物的合成

Figure 13. Synthesis of the first Mg-N2 complex

图14. 首例Be(0)配合物的合成及反应性研究

Figure 14. Synthesis and reactivity of the first beryllium(0) complex

图15. Be(I)-Al配合物的合成

Figure 15. Synthesis of beryllium(I)-aluminum complexes

图16. 正离子型Be(I)自由基化合物的合成及反应性研究

Figure 16. Synthesis and reactivity of beryllium radical cation compounds

图17. 中性Be(I)自由基化合物的合成及反应性研究

Figure 17. Synthesis and reactivity of neutral beryllium(I) radical compounds

图18. 经历Be(I)自由基中间体的反应

Figure 18. A reaction via the beryllium(I) radical intermediate

图19. 双茂双铍化合物的合成及反应性研究

Figure 19. Synthesis and reactivity of diberyllocene

图20. 杂双金属Mg-Be配合物的合成及反应性研究

Figure 20. Synthesis and reactivity of heterobimetallic Mg-Be complexes

图21. 反三明治型双Ca(I)配合物的合成及其争议

Figure 21. Synthesis and controversy of inverse sandwich dicalcium(I) complexes

图22. 大位阻BDI*配体支持的Ca(I)配合物的合成探索

Figure 22. Attempts on the synthesis of calcium(I) complexes supported by bulky BDI* ligands

图23. 大位阻BDI*配体支持的首例钙-氮气配合物的合成

Figure 23. Synthesis of the first Ca-N2 complex supported by a bulky BDI* ligand

图24. 大位阻BDI*配体支持的钙-氮气配合物的反应性研究

Figure 24. Reactivity of a Ca-N2 complex supported by a bulky BDI* ligand

图25. 大位阻氧杂蒽双氮配体支持的钙-氮气配合物的合成

Figure 25. Synthesis of Ca-N2 complex supported by an extremely bulky diamide ligand

图26. 联苯-双钙配合物的合成

Figure 26. Syntheses of biphenyl-dicalcium complexes

图27. 偶氮苯自由基钙配合物的合成及反应性研究

Figure 27. Synthesis and reactivity of azobenzene radical calcium complexes

图28. 2,2'-联吡啶自由基钙配合物的合成及反应性研究

Figure 28. Synthesis and reactivity of calcium complexes with 2,2'-bipyridyl radical

图29. 杂双金属Mg-Ae (Ae=Ca/Sr/Ba)配合物的合成及反应性研究

Figure 29. Synthesis and reactivity of heterobimetallic Mg-Ae complexes

图30. 联苯-双锶配合物的合成

Figure 30. Syntheses of biphenyl-distrontium complexes

图31. Ba(0)/BaH2在催化氢化反应中的应用

Figure 31. The application of Ba(0)/BaH2 in catalytic hydrogenation

图32. 金属蒸气法合成Ba(0)金属有机合成子

Figure 32. Metal vapour synthesis (MVS) of an organometallic Ba(0) synthon

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低氧化态碱土金属有机化学概述

Overview on Low-oxidation-state Alkaline Earth Organometallic Chemistry

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