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重新定义氧化钴在乙烷脱氢芳构化中的作用:对增强催化活性和稳定性的见解。

Redefining the Role of Cobalt Oxide in Ethane Dehydroaromatization: Insights into Enhanced Catalytic Activity and Stability.

作者信息

Ju Na Yeong, Lee Seok-Ho, Kim Sang Yun, Park Ye Rim, Lee Byung Jin, Kim Jinseong, Choi Jungkyu, Kim Do Heui, Lee Kwan-Young

机构信息

Department of Chemical and Biological Engineering, Korea University, 145 Anam-ro, Seongbuk-gu, Seoul 02841, Republic of Korea.

School of Chemical and Biological Engineering, Institute of Chemical Processes, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, South Korea.

出版信息

ACS Appl Mater Interfaces. 2025 Jan 8;17(1):823-834. doi: 10.1021/acsami.4c13379. Epub 2024 Dec 25.

DOI:10.1021/acsami.4c13379
PMID:39720877
Abstract

Cobalt is recognized as an active catalyst in ethane dehydroaromatization (EDA) reactions due to its efficient ethane cracking capability. In order to optimize cobalt's strong ethane cracking capability, it was loaded onto HZSM-5 zeolite through impregnation. This study was conducted with Co-loaded HZSM-5 catalysts with an incipient wetness impregnation method and witnessed an increase of catalytic activity with a long induction period. We elucidated the prior reduction of external CoO before BTX synthesis and the novel roles of external CoO in suppressing deactivation─an aspect not extensively explored in previous studies utilizing single Co catalysts. The utilization of CoO as a catalyst on external zeolites promotes the generation of carbon nanotubes (CNTs) while inhibiting the formation of graphite, thereby suppressing the deactivation of the catalyst. Furthermore, experimental comparisons with Co catalysts synthesized via ion exchange and physical mixing underscore the role of Co ions anchored to internal zeolite as active sites for BTX synthesis as well as emphasize the importance of external CoO in enhancing catalyst stability.

摘要

钴因其高效的乙烷裂解能力而被认为是乙烷脱氢芳构化(EDA)反应中的活性催化剂。为了优化钴强大的乙烷裂解能力,通过浸渍法将其负载到HZSM-5沸石上。本研究采用初湿浸渍法制备了负载钴的HZSM-5催化剂,观察到催化活性有所提高,但有较长的诱导期。我们阐明了在BTX合成之前外部CoO的预还原以及外部CoO在抑制失活方面的新作用——这是以往使用单一Co催化剂的研究中未广泛探讨的一个方面。在外部沸石上使用CoO作为催化剂促进了碳纳米管(CNT)的生成,同时抑制了石墨的形成,从而抑制了催化剂的失活。此外,与通过离子交换和物理混合合成的Co催化剂进行的实验比较,强调了锚定在内部沸石上的Co离子作为BTX合成活性位点的作用,同时也强调了外部CoO在提高催化剂稳定性方面的重要性。

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