Effect of support morphology on the ammonia synthesis activity of Ru/CeO2-based catalysts

IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL International Journal of Hydrogen Energy Pub Date : 2024-11-13 DOI:10.1016/j.ijhydene.2024.11.053
Kiyoshi Yamazaki , Yoshihiro Goto , Masashi Kikugawa , Akinori Sato , Yuichi Manaka , Tetsuya Nanba , Hideyuki Matsumoto , Shinichi Ookawara
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Abstract

We investigate the effect of the support morphology on ammonia (NH3) synthesis activity of Ru/CeO2-based catalysts using supports derived from various CeO2 materials under different treatment temperatures with different SiO2/ZrO2 additions. These supports are classified by peak pore size into three pore structure types: small (3–4 nm), medium (7–20 nm), and large (50–70 nm). The medium-type supports show the highest specific surface area (SSA), which increases with SiO2/ZrO2 addition. The Ru dispersion on each support, regardless of its type and composition, is determined from its SSA. The NH3-synthesis activity of catalysts at 0.1 MPa and a space velocity (SV) of 36000 h−1 exhibits a volcanic trend with respect to the Ru dispersion. This is explained by the fraction of active B5-type sites generated. At SVs >72000 h−1, the activity of catalysts with peak pore size <8 nm is less than the above volcanic trend, possibly owing to increased diffusion resistance in the pore.
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支撑体形态对基于 Ru/CeO2 催化剂的氨合成活性的影响
我们研究了支撑体形态对 Ru/CeO2 基催化剂合成氨 (NH3) 活性的影响,使用的支撑体来自不同处理温度下添加不同 SiO2/ZrO2 的各种 CeO2 材料。这些载体按峰值孔径分为三种孔结构类型:小型(3-4 nm)、中型(7-20 nm)和大型(50-70 nm)。中型支撑物的比表面积(SSA)最大,随着 SiO2/ZrO2 添加量的增加而增大。无论支撑物的类型和组成如何,Ru 在每种支撑物上的分散度都是根据其 SSA 确定的。在 0.1 MPa 和 36000 h-1 的空间速度 (SV) 条件下,催化剂的 NH3 合成活性与 Ru 的分散度有关,呈现出火山爆发的趋势。这可以从生成的活性 B5 型位点的比例得到解释。在 SVs >72000 h-1 条件下,峰值孔径为 8 nm 的催化剂的活性低于上述火山岩趋势,这可能是由于孔中的扩散阻力增加所致。
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来源期刊
International Journal of Hydrogen Energy
International Journal of Hydrogen Energy 工程技术-环境科学
CiteScore
13.50
自引率
25.00%
发文量
3502
审稿时长
60 days
期刊介绍: The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc. The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.
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