可恒温的 NiO/CeO2 异质界面结构在低温催化 CO-NO 反应中的活性

IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Bulletin of the Chemical Society of Japan Pub Date : 2024-07-23 DOI:10.1093/bulcsj/uoae081
Zannatul Mumtarin Moushumy, Hiroshi Yoshida, Kaori Tokusada, Ai Kuraoka, Sota Sakamoto, Masayuki Tsushida, Masato Machida
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摘要

NiO 表面接枝到 CeO2 纳米晶上会产生异质界面结构,为 CO-NO 反应生成 N2 和 CO2 提供有效的活性位点。在本研究中,我们研究了高温热老化对 NiO/CeO2 催化剂活性和纳米结构的影响。在 900 °C 高温老化后,催化剂保持了较高的催化活性,而参考催化剂则由于大量固态反应和烧结而丧失了催化活性。新制备的 NiO/CeO2 催化剂(600 ℃ 煅烧)在 CeO2 晶粒中含有大量分散的 NiO 物种。相反,经过热老化的催化剂由生长的 NiO 和 CeO2 结晶体组成,它们紧密接触形成热稳定性界面,附近的周边提供了 Ni2+ 并入的 CeO2 表面,用于去除和填充催化循环中的氧物种,从而促进 CO-NO 反应。根据原位傅立叶变换红外分析和平行同位素反应分析,我们确认了以下可能的途径:(i) 吸附的 CO 清除表面氧,形成氧空位 (VO);(ii) 吸附的 NO 与 VO 相互作用;(iii) N-O 键裂解,与 CO 反应生成异氰酸酯,然后与 NO 反应生成 N2。
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The activity of thermostable NiO/CeO2 heterointerface structure toward low-temperature catalytic CO–NO reaction
The surface grafting of NiO onto CeO2 nanocrystallites generates heterointerface structures, providing efficient active sites for CO–NO reactions toward forming N2 and CO2. In this study, we investigated the effects of high-temperature thermal aging on the activity and nanostructure of the NiO/CeO2 catalyst. After thermal aging at 900 °C, the catalyst retained a high catalytic activity, whereas the reference catalysts lost theirs owing to considerable solid-state reactions and sintering. The as-prepared fresh NiO/CeO2 catalyst (calcined at 600 °C) contained high dispersions of NiO species in CeO2 crystallites. Conversely, the thermally aged catalyst comprised grown NiO and CeO2 crystallites were allowed to contact intimately to form thermostable interfaces, where the perimeter in the vicinity provided the Ni2+-incorporated CeO2 surface for removing and filling the oxygen species in the catalytic cycle toward facilitating CO–NO reactions. Based on in situ Fourier transform infrared and parallel isotopic reaction analyses, we confirmed the following as possible pathways: (i) the removal of the surface oxygen by the adsorbed CO to form an oxygen vacancy (VO), (ii) the interaction between the adsorbed NO with VO, and (iii) the N–O bond cleavage and the reaction with CO to form isocyanate, followed by the reaction with NO to produce N2.
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来源期刊
CiteScore
6.40
自引率
5.00%
发文量
194
审稿时长
3-8 weeks
期刊介绍: The Bulletin of the Chemical Society of Japan (BCSJ) is devoted to the publication of scientific research papers in the fields of Theoretical and Physical Chemistry, Analytical and Inorganic Chemistry, Organic and Biological Chemistry, and Applied and Materials Chemistry. BCSJ appears as a monthly journal online and in advance with three kinds of papers (Accounts, Articles, and Short Articles) describing original research. The purpose of BCSJ is to select and publish the most important papers with the broadest significance to the chemistry community in general. The Chemical Society of Japan hopes all visitors will notice the usefulness of our journal and the abundance of topics, and welcomes more submissions from scientists all over the world.
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