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Synergistically Catalytic Hydrochlorination of Acetylene over the Highly Dispersed Ru Active Species Embedded in P-Containing Ionic Liquids
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2020-06-17 , DOI: 10.1021/acssuschemeng.0c02329
Jian Li 1 , Haiyang Zhang 1 , Linfeng Li 1 , Ming Cai 1 , Yanqin Li 1 , Dongyang Xie 1 , Jinli Zhang 1, 2
Affiliation  

With the objective of achieving long-term sustainable development of an effective approach for acetylene hydrochlorination, green and efficient mercury-free catalysts are urgently needed. Based on the coordination or interaction between heteroatoms and metal ions, catalysts with carbon-supported ruthenium active species embedded in ionic liquids (Ru-ILx/AC) were prepared with structural phosphorus-containing ILs. The experimental results showed that Ru species were embedded in ILs and the interaction between the central Ru ions and ILs guaranteed the successful anchoring and high dispersion of active species on the host. The incorporation of ILs with alkyl branched chains having strong electron-donating ability augmented the relative content of the active Run+ species, which synergistically enhanced the adsorption and activation ability of the catalysts toward both the HCl and C2H2 reactants. This resulted in a significant improvement in the catalytic activity, with a 386% relative increment over the 1Ru-5IL5/AC catalyst with respect to its counterpart. Furthermore, the additives discouraged the coke deposition and Ru species agglomeration and stabilized the Ru species in a high-valent state, thus significantly slowing down the deactivation of the catalyst. The 1Ru-5IL5/AC catalyst exhibited an impressive stability and provides an important reference for potential industrial application.

中文翻译:

嵌入P离子液体中的高分散Ru活性物种对乙炔的协同催化氯化氢处理

为了长期可持续发展一种有效的乙炔氢氯化方法,迫切需要绿色高效的无汞催化剂。基于杂原子与金属离子之间的配位或相互作用,用结构性含磷离子液体制备了嵌入碳离子液体(Ru-IL x / AC)中的碳载钌活性物种催化剂。实验结果表明,Ru物种被包埋在ILs中,中心Ru离子与ILs之间的相互作用确保了活性物种在宿主上的成功锚定和高度分散。IL与具有强电子给体能力的烷基支链的结合增加了活性Ru n +的相对含量物种,它们协同增强了催化剂对HCl和C 2 H 2反应物的吸附和活化能力。这导致催化活性的显着改善,相对于其对应物,其相对于1Ru-5IL 5 / AC催化剂具有386%的相对增量。此外,添加剂阻止了焦炭沉积和Ru物质的团聚并使Ru物质稳定在高价态,从而显着减慢了催化剂的失活。1Ru-5IL 5 / AC催化剂显示出令人印象深刻的稳定性,并为潜在的工业应用提供了重要的参考。
更新日期:2020-07-13
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