Self-organized Ruthenium-Barium Core-Shell Nanoparticles on a Mesoporous Calcium Amide Matrix for Efficient Low-Temperature Ammonia Synthesis

Self-organized Ruthenium-Barium Core-Shell Nanoparticles on a Mesoporous Calcium Amide Matrix for Efficient Low-Temperature Ammonia Synthesis
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DOI:
10.1002/anie.201712398
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发表时间:
2018-03-01
影响因子:
16.6
通讯作者:
Hosono, Hideo
Hosono, Hideo
中科院分区:
化学1区
文献类型:
--
作者:
Kitano, Masaaki;Inoue, Yasunori;Hosono, Hideo

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现场合成需要低温氨合成工艺。在低于300 ℃的温度下,钡掺杂的氨基化钙(Ba-Ca(NH 2)(2))将由Ru和Co介导的氨合成的效率提高了2个数量级以上。此外,所提出的催化剂比已知在低温和低压下具有高活性的工业催化剂的基于浮氏体的Fe催化剂优越上级。在H_2预处理过程中,Ru-Ba纳米核壳结构在Ba-Ca(NH_2)(2)载体上自组装,同时载体材料转化为具有高比表面积(> 100 m2·g ~(-1))的介孔结构。这些自组织纳米结构解释了低温氨合成中的高催化性能。
A low-temperature ammonia synthesis process is required for on-site synthesis. Barium-doped calcium amide (Ba-Ca(NH2)(2)) enhances the efficacy of ammonia synthesis mediated by Ru and Co by 2 orders of magnitude more than that of a conventional Ru catalyst at temperatures below 300 degrees C. Furthermore, the presented catalysts are superior to the wustite-based Fe catalyst, which is known as a highly active industrial catalyst at low temperatures and pressures. Nanosized Ru-Ba core-shell structures are self-organized on the Ba-Ca(NH2)(2) support during H-2 pretreatment, and the support material is simultaneously converted into a mesoporous structure with a high surface area (>100m(2)g(-1)). These self-organized nanostructures account for the high catalytic performance in low-temperature ammonia synthesis.