CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis
CC3 porous organic cage crystals and membranes for the non-thermal plasma catalytic ammonia synthesis
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DOI：
10.1016/j.ceja.2022.100340
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发表时间：
2022-08-15
影响因子：
--
通讯作者：
Carreon, Maria L.
中科院分区：
文献类型：
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作者：
Gorky, Fnu;Nguyen, Hoang M.;Carreon, Maria L.
氨被认为是肥料的基本组成部分。此外，它是一种经济高效且技术适用的能源储存和运输解决方案。非热等离子体驱动的可再生能源驱动的催化剂被认为是传统哈伯-博世氨合成工艺的一种绿色替代方案。在这种电子介导的途径中的主要挑战是低氨合成产量，考虑到在反应期间等离子体诱导的新鲜产生的氨的分解。在这里，我们报告的等离子体辅助氨合成在介质阻挡放电反应器填充与CC 3晶体，一个原型的多孔有机笼，和分子筛膜从相同的CC 3材料制成。与其他微孔催化剂（例如沸石（SAPO-34）和金属有机骨架（ZIF-8、ZIF-67）（低于0.02 μ mol min-1 m-2）相比，CC 3晶体提供了最高的氨合成速率（0.06 μ mol min-1 m-2）。具有良好定义的八面体晶体几何形状的CC 3多孔笼提供了部分保护，而CC 3膜提供了吸附和分离效果的新鲜形成的氨从其原位分解，确保优良的氨合成率为20.3 μ mol min-1 m- 2。该研究结果为等离子体驱动催化氨合成中先进多孔催化剂和膜的合理设计提供了新的见解。
Ammonia is considered a basic building block for fertilizers. Also, it is an economically efficient and technologically suitable solution for energy storage and transportation. Non-thermal plasma-driven catalysis powered by renewable energy is considered as a green alternative to the conventional Haber-Bosch process for ammonia synthesis. The main challenge in this electron-mediated route is the low ammonia synthesis production, given the plasma-induced decomposition of the freshly generated ammonia during the reaction. Herein we report the plasma-assisted ammonia synthesis in a dielectric barrier discharge reactor packed with CC3 crystals, a prototypical porous organic cage, and a molecular-sieve membrane fabricated from the same CC3 material. The CC3 crystals delivered the highest ammonia synthesis rate (0.06 & mu;mol min-1 m-2) compared to other microporous catalysts such as zeolite (SAPO-34) and metal-organic frameworks (ZIF-8, ZIF-67) (below 0.02 & mu;mol min-1 m-2). The CC3 porous cage with well-defined octahedral crystal geometry provides partial protection while the CC3 membrane offers both adsorption and separation effects for the freshly formed ammonia from its in-situ decomposition, securing an excellent ammonia synthesis rate of 20.3 & mu;mol min-1 m- 2. The findings from this work unfolds novel insights into rational designs of advanced porous catalyst and membrane for plasma-driven catalytic ammonia synthesis in a sustainable and efficient way.