碳相互作用的 AlF3 簇作为脱氟化氢反应的鲁棒催化剂，具有增强的配位不足和稳定性,ACS Catalysis

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碳相互作用的 AlF3 簇作为脱氟化氢反应的鲁棒催化剂，具有增强的配位不足和稳定性
ACS Catalysis ( IF 11.3 ) Pub Date : 2024-01-31 , DOI: 10.1021/acscatal.3c05921
Yiwei Sun ₁ , Xiaoli Wei ₁ , Wei Zhang ₁ , Zhen Wang ₁ , Jianhai Jiang ₁ , Fangcao Liu ₁ , Bing Liu ₁ , Wenfeng Han _{1,

2}

Affiliation

将强效温室气体氢氟碳化物 (HFC) 转化为增值氢氟烯烃 (HFO) 非常重要。 AlF ₃催化剂在此过程中发挥着重要作用。配位铝的形成和维持是制备高效催化剂的关键。在此，以SAPO-5分子筛为前驱体，通过热解和原位氟化，有效地实现了碳相互作用的AlF ₃纳米团簇催化剂（AlF ₃ –SAPO-5）。该过程导致碳质材料和活性铝（Al）物质之间产生强烈的相互作用。结果表明AlF ₃ –SAPO-5具有较高的活性和热稳定性。对于1,1-二氟乙烷(HFC-152a)脱氟化氢，在350℃的反应温度下转化率可以达到95%。反应速率比传统热解法制备的AlF _{3 (AlF}₃ -py)高出近4倍。这意味着限域效应有助于形成具有丰富的 4 和 5 配位 Al 物种的 AlF ₃纳米团簇，并由 F-Al-O-C 结构稳定。此外，碳相互作用的AlF ₃纳米团簇表现出优异的耐烧结性。鉴于其出色的活性和热稳定性，碳相互作用的AlF ₃纳米团簇在氟化烷烃的催化脱氟化氢方面显示出巨大的潜力。

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Carbon-Interacted AlF3 Clusters as Robust Catalyst for Dehydrofluorination Reaction with Enhanced Undercoordination and Stability

Conversion of potent greenhouse gases, hydrofluorocarbons (HFCs), to value-added hydrofluoroolefins (HFOs) is of great importance. AlF₃ catalysts play a major role in this process. Formation and maintenance under coordinated Al are the key to prepare efficient catalysts. Herein, carbon interacted AlF₃ nanoclusters catalyst (AlF₃–SAPO-5) was effectively achieved with SAPO-5 molecular sieves as precursors via pyrolysis followed by in situ fluorination. This process results in a strong interaction between the carbonaceous material and active aluminum (Al) species. The results show that AlF₃–SAPO-5 possesses both high activity and thermal stability. For 1,1-difluoroethane (HFC-152a) dehydrofluorination, the conversion can reach up to 95% at a reaction temperature of 350 °C. The reaction rate is almost 4 times higher than that of AlF₃ prepared by traditional pyrolysis (AlF₃-py). It implies that the confinement effect contributes to the formation of AlF₃ nanoclusters with abundant 4- and 5-coordinated Al species stabilized by the F–Al–O–C structure. In addition, the carbon-interacted AlF₃ nanoclusters exhibit superb sintering resistance. Given its fantastic activity and thermal stability, the carbon-interacted AlF₃ nanoclusters show great potential for the catalytic dehydrofluorination of fluorinated alkanes.

更新日期：2024-01-31

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