A recyclable heterogeneous-homogeneous-heterogeneous NiO/AlOOH catalysis system for hydrocarboxylation of acetylene to acrylic acid.

A recyclable heterogeneous-homogeneous-heterogeneous NiO/AlOOH catalysis system for hydrocarboxylation of acetylene to acrylic acid.
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一种可回收的多相-均相-多相NiO/AlOOH催化体系,用于乙炔加氢羧化制丙烯酸

DOI:
10.1039/c9ra09737f
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发表时间:
2020-01-07
期刊:
影响因子:
3.9
通讯作者:
--
中科院分区:
化学3区
文献类型:
--
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对以煤和天然气为基础的乙炔的高价值利用的担忧为探索通过一步加氢羧化反应生产丙烯酸(AA)提供了特别的动力。在催化剂的简单回收、再循环和再利用的推动下,我们报道了一种高性能 NiO/AlOOH 催化剂,其 AA 时空产率为 412 gAA gcat.−1 h−1,可通过简单的初湿浸渍法获得。详细的动力学和控制实验证实,这种固体催化剂上的镍物质提供了非均相-均相-非均相催化循环,其中CO和浸出的镍之间形成的螯合物充当活性物质。浸出镍物质的彻底回收大大提高了催化剂的稳定性。这些初步发现进一步表明了传统均相催化体系中新型多相催化剂设计的前景。 NiO/AlOOH 催化剂上乙炔加氢羧化为丙烯酸过程中的多相-均相-多相催化循环。
Concerns about the high-valued utilization of coal- and natural gas-based acetylene has provided particular impetus for exploration of acrylic acid (AA) production via one-step hydrocarboxylation reaction. Motivated by simple recovery, recycling and reuse of the catalyst, we report a high-performance NiO/AlOOH catalyst with AA space-time-yield of 412 gAA gcat.−1 h−1, obtainable by a simple incipient wetness impregnation method. Detailed kinetic and controlled experiments confirmed that nickel species on such a solid catalyst provide a heterogeneous–homogeneous–heterogeneous catalytic cycle where the chelates formed between CO and leached nickel act as the active species. The thorough recovery of leached nickel species improves the catalyst stability greatly. These preliminary findings indicate further prospects for new heterogeneous catalyst design in traditional homogeneous catalytic systems. The heterogeneous–homogeneous–heterogeneous catalytic cycle during the hydrocarboxylation of acetylene to acrylic acid over a NiO/AlOOH catalyst.
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