Selective semi-hydrogenation of alkynes plays a pivotal role in the field of chemical production but still suffers from low selectivity and catalyst stability. Herein, an aminoclay-derived nickel catalyst was constructed by replacing part of Mg by Niin the skeleton and coordinating Ni with aminopropyl groups via a self-assembly synthetic strategy. The introduction of Ni facilitated the exfoliation of lamellar structure, resulting in highly exposed and uniformly dispersed Ni nanoparticles. The optimal catalyst showed an excellent catalytic performance with 99.9 % conversion and 98.9 % regio- selectivity to alkene (/ = 94:6) in diphenylacetylene semi-hydrogenation. Experimental data and theoretical calculations validated that the aminopropyl groups on NiMg-AC improved the activity and selectivity to alkene by tuning the adsorption/desorption energies of substrate/product. Furthermore, this non-precious metal catalyst showed stable activity and selectivity during cyclic testing, thanks to the strong interaction between Ni and the aminopropyl groups. This "self-assembly" synthetic strategy provides valuable guidance for the preparation of aminoclay-derived Ni catalysts for selective semi-hydrogenation.

中文翻译：

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用于炔烃选择性半氢化的氨基粘土镍纳米颗粒的制备和第一性原理计算：氨基丙基的影响

炔烃选择性半加氢在化工生产领域发挥着关键作用，但仍然存在选择性和催化剂稳定性较低的问题。在此，通过自组装合成策略，通过用 Ni 取代骨架中的部分 Mg，并通过 Ni 与氨丙基基团配位，构建了氨基粘土衍生的镍催化剂。 Ni的引入促进了层状结构的剥离，产生高度暴露且均匀分散的Ni纳米颗粒。优化的催化剂在二苯乙炔半加氢反应中表现出优异的催化性能，转化率达到 99.9%，烯烃区域选择性达到 98.9%（/= 94:6）。实验数据和理论计算验证了 NiMg-AC 上的氨丙基通过调节底物/产物的吸附/解吸能提高了烯烃的活性和选择性。此外，由于镍和氨丙基之间的强相互作用，这种非贵金属催化剂在循环测试中表现出稳定的活性和选择性。这种“自组装”合成策略为制备用于选择性半加氢的氨基粘土衍生镍催化剂提供了有价值的指导。