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Peer-reviewedCC BYInorganic chemistry

Tailoring Reactivity of Molecular Gallium Hydroxides via Chalcogen Bridging.

  • Erandi Bernabé-Pablo1,2
  • Alfonso Gallardo-Garibay1,2
  • Vojtech Jancik1,2
  • Diego Martínez-Otero1,2
  • Roman Neufeld3
  • Uvaldo Hernández-Balderas1,2
  • Dietmar Stalke3
  • Mónica Moya-Cabrera1,2
  1. 1Universidad Nacional Autónoma de México, Instituto de Química , Ciudad Universitaria, Ciudad de México04510, México.
  2. 2Centro Conjunto de Investigación en QuímicaSustentable UAEM-UNAM, Carretera Toluca-Atlacomulco Km 14.5, Toluca, Estado de México50200, México.
  3. 3Institut für Anorganische Chemie, Georg-August Universität Göttingen, Tammannstrasse 4, 37077Göttingen, Germany.
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Abstract

We studied the influence of bridging chalcogen atoms (μ-E; E = S, Se) on the structure and reactivity of digallium dihydroxide complexes [{MeLGa(OH)}2(μ-E)] [E = S (4), Se (5); MeL = CH{CMe(NAr)}2-, Ar = 2,4,6-Me3C6H2]. Compounds 4 and 5 were synthesized from MeLGaCl2 and sodium chalcogenide (Na2E) in THF-NH3(l), followed by controlled hydrolysis. For the sulfur system, the intermediates [{MeLGa(Cl)}2(μ-S)] (2) and [{MeLGa(NH2)}2(μ-S)] (3) were isolated and characterized, whereas the corresponding selenium derivatives proved too reactive for isolation. The reactivity of 4 and 5 toward Group 4 metal amides, M(NR2)4 (M = Ti, R = Me; M = Zr, Hf, R = Et), revealed a chalcogen effect, affording both monocyclic and spirocyclic complexes from 4, while 5 selectively yielded spirocyclic complexes. Likewise, the milder amide Me2Si(NMe2)2 reacted exclusively with 5 to produce a siloxide-bridged derivative. Distinct borane-dependent pathways were also observed. Treatment of 4 and 5 with BH3·THF resulted in the Ga-OH protonolysis to form cyclic borates, whereas BH3·SMe2 promoted hydride attack at gallium, yielding gallium hydrides. These results provide an insight into the ambiphilic character of 4 and 5 and establish chalcogen bridging as a strategy for tuning their bonding and reactivity.

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Cite

BibTeXRIS
BibTeX
@article{bernabepablo2026tailoring,
  title = {{Tailoring Reactivity of Molecular Gallium Hydroxides via Chalcogen Bridging.}},
  author = {Erandi Bernabé-Pablo and Alfonso Gallardo-Garibay and Vojtech Jancik and Diego Martínez-Otero and Roman Neufeld and Uvaldo Hernández-Balderas and Dietmar Stalke and Mónica Moya-Cabrera},
  journal = {Inorganic chemistry},
  year = {2026},
  month = oct,
  doi = {10.1021/acs.inorgchem.6c03433},
  url = {https://europepmc.org/article/MED/42895374},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Tailoring Reactivity of Molecular Gallium Hydroxides via Chalcogen Bridging.
AU  - Erandi Bernabé-Pablo
AU  - Alfonso Gallardo-Garibay
AU  - Vojtech Jancik
AU  - Diego Martínez-Otero
AU  - Roman Neufeld
AU  - Uvaldo Hernández-Balderas
AU  - Dietmar Stalke
AU  - Mónica Moya-Cabrera
PY  - 2026
DA  - 2026/10/01
JO  - Inorganic chemistry
DO  - 10.1021/acs.inorgchem.6c03433
UR  - https://europepmc.org/article/MED/42895374
AB  - We studied the influence of bridging chalcogen atoms (μ-E; E = S, Se) on the structure and reactivity of digallium dihydroxide complexes [{MeLGa(OH)}2(μ-E)] [E = S (4), Se (5); MeL = CH{CMe(NAr)}2-, Ar = 2,4,6-Me3C6H2]. Compounds 4 and 5 were synthesized from MeLGaCl2 and sodium chalcogenide (Na2E) in THF-NH3(l), followed by controlled hydrolysis. For the sulfur system, the intermediates [{MeLGa(Cl)}2(μ-S)] (2) and [{MeLGa(NH2)}2(μ-S)] (3) were isolated and characterized, whereas the corresponding selenium derivatives proved too reactive for isolation. The reactivity of 4 and 5 toward Group 4 metal amides, M(NR2)4 (M = Ti, R = Me; M = Zr, Hf, R = Et), revealed a chalcogen effect, affording both monocyclic and spirocyclic complexes from 4, while 5 selectively yielded spirocyclic complexes. Likewise, the milder amide Me2Si(NMe2)2 reacted exclusively with 5 to produce a siloxide-bridged derivative. Distinct borane-dependent pathways were also observed. Treatment of 4 and 5 with BH3·THF resulted in the Ga-OH protonolysis to form cyclic borates, whereas BH3·SMe2 promoted hydride attack at gallium, yielding gallium hydrides. These results provide an insight into the ambiphilic character of 4 and 5 and establish chalcogen bridging as a strategy for tuning their bonding and reactivity.
SN  - 0020-1669
SN  - 1520-510X
ER  -