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Catalytic Reduction of Carbon Dioxide Using Cationic Organoaluminum and -Gallium Compounds
Organometallics ( IF 2.5 ) Pub Date : 2017-12-07 00:00:00 , DOI: 10.1021/acs.organomet.7b00716
Mahmoud Saleh 1 , Douglas R. Powell 2 , Rudolf J. Wehmschulte 1
Affiliation  

Ethide abstraction from Et3M (M = Al and Ga), (2,6-Ph2C6H3)AlEt2, 1, and (2,6-Dipp2C6H3)GaEt2, 2 (Dipp = 2,6-iPr2C6H3), using the silylium ion [Et3Si][CHB11Cl11] afforded crystalline ion-like compounds [Et2M][CHB11Cl11] (M = Al, 3; Ga, 5) and [(2,6-Ph2C6H3)AlEt][CHB11Cl11], 4, and the likely solvent-separated ion pair [(2,6-Dipp2C6H3)GaEt][CHB11Cl11], 6. Crystalline compounds 35 feature cation···anion contacts in the solid state, and their solubility in low polarity benzene indicates that these contacts are maintained in solution. All compounds catalyze the reduction of CO2 with Et3SiH, but the activity of the gallium compound 5 is significantly lower due to its polymeric structure and the lower Lewis acidity of gallium. Whereas the reduction products from the reactions catalyzed by compounds 35 are mostly methane and toluene (from Friedel–Crafts alkylation of the benzene solvent), catalysis by 6 led mostly to Et3SiOCH3.

中文翻译:

阳离子有机铝和镓化合物催化还原二氧化碳

从Et Ethide抽象3 M(M = Al和Ga),(2,6-PH 2 ç 6 ħ 3)ALET 21,和(2,6-卜先生2 ç 6 ħ 3)GaEt 22(迪普=2,6 - i Pr 2 C 6 H 3),使用甲硅烷基离子[Et 3 Si] [CHB 11 Cl 11 ]得到结晶离子状化合物[Et 2 M] [CHB 11 Cl 11 ](M = Al ,3 ; Ga,5)和[(2,6-Ph 2 C 6 H 3)AlEt] [CHB 11 Cl 11 ],4和可能的溶剂分离离子对[(2,6-Dipp 2 C 6 H 3)GaEt] [ CHB 11 Cl 11 ],6。结晶化合物3 - 5个在固体状态特征阳离子...阴离子接触,并且其在低极性苯溶解度表明这些触头被保持在溶液中。所有化合物都可以用Et 3 SiH催化CO 2的还原,但是镓化合物5的活性由于其聚合物结构和较低的镓路易斯酸度,因此其明显较低。化合物35催化反应的还原产物主要是甲烷和甲苯(苯溶剂的Friedel-Crafts烷基化反应),而6催化则主要生成Et 3 SiOCH 3
更新日期:2017-12-07
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