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用红外光谱考察了氢甲酰化反应过程中铑膦催化剂结构的变化,讨论了可能的催化活性物种和失活的原因。结果表明,氧的存在对氢甲酰化反应直接产生抑制作用,但在我们的实验条件下,催化剂的失活不能归因于三苯膦的氧化和碳膦键的断裂。失活可能主要是由于原位生成的活性物种在反应过程中不断缔合,生成了非活性的膦取代的铑原子簇。
The structure of the rhodium phosphine catalyst during the hydroformylation reaction was investigated by infrared spectroscopy. Possible catalytic species and reasons for inactivation were discussed. The results showed that the presence of oxygen directly inhibited the hydroformylation reaction, but under our experimental conditions, the catalyst deactivation could not be attributed to the oxidation of triphenylphosphine and the cleavage of the carbon-carbon bond. Inactivation may be mainly due to the continuous association of the in situ generated active species during the reaction, resulting in the formation of an inactive phosphine-substituted rhodium cluster.