分级Fe/ZSM-5催化剂上N2O氧化苯制苯酚

IF 10.7 1区 工程技术 Q1 CHEMISTRY, PHYSICAL
Cui Ouyang , Jianwei Li , Yaqi Qu , Song Hong , Songbo He
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引用次数: 2

摘要

在连续固定床反应器中,研究了分级微孔Fe/ZSM-5基催化剂上N2O催化苯氧化制苯酚的反应。废催化剂通过使用N2O的氧化处理原位再生,总共进行了10次反应再生循环。在新的分级Fe/ZSM-5-H2.8催化剂上,获得了100%的N2O转化率、93.3%的苯酚选择性、16.49±0.06 mmol g催化剂−1 h−1的高初始苯酚形成率和147.06 mmol c催化剂−1的良好苯酚产率。在反应再生循环中,N2O转化率在3小时的TOS内完全恢复,此外,苯酚生产率下降约2.2±0.8%,导致总苯酚生产率约为0.44吨苯酚kgcatalyst−1,估计300次循环。催化剂表征表明,焦炭在3小时的初始TOS(0.28 mgc g催化剂−1分钟−1)中快速沉积在催化剂表面,并在30小时的TOS中逐渐变为石墨化,形成速率为0.06 mgc c g催化剂–1分钟−2。除其他外(例如,结构性质和酸度的降低),焦炭几乎完全覆盖活性Fe-O-Al位点是主要催化剂失活的原因。除了这些与焦化有关的可逆失活特性外,反应再生循环也观察到催化剂的不可逆失活。后者反映为活性Fe-O-Al位点的进一步减少,其随着循环而聚集在催化剂表面,可能与再生未完全去除的硬焦残留物有关。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Oxidation of benzene to phenol with N2O over a hierarchical Fe/ZSM-5 catalyst

Oxidation of benzene to phenol with N2O over a hierarchical Fe/ZSM-5 catalyst

Catalytic oxidation of benzene with N2O to phenol over the hierarchical and microporous Fe/ZSM-5-based catalysts in a continuous fixed-bed reactor was investigated. The spent catalyst was in-situ regenerated by an oxidative treatment using N2O and in total 10 reaction-regeneration cycles were performed. A 100% N2O conversion, 93.3% phenol selectivity, and high initial phenol formation rate of 16.49 ± 0.06 mmolphenol gcatalyst−1 h−1 at time on stream (TOS) of 5 min, and a good phenol productivity of 147.06 mmolphenol gcatalyst−1 during catalyst life-time of 1800 min were obtained on a fresh hierarchical Fe/ZSM-5-Hi2.8 catalyst. With the reaction-regeneration cycle, N2O conversion is fully recovered within TOS of 3 h, moreover, the phenol productivity was decreased ca. 2.2 ± 0.8% after each cycle, leading to a total phenol productivity of ca. 0.44 tonphenol kgcatalyst−1 estimated for 300 cycles. Catalyst characterizations imply that the coke is rapidly deposited on catalyst surface in the initial TOS of 3 h (0.28 mgc gcatalyst−1 min−1) and gradually becomes graphitic during the TOS of 30 h with a slow formation rate of 0.06 mgc gcatalyst−1 min−1. Among others (e.g., the decrease of textural property and acidity), the nearly complete coverage of the active Fe-O-Al sites by coke accounts for the main catalyst deactivation. Besides these reversible deactivation characteristics related to coking, the irreversible catalyst deactivation is also observed with the reaction-regeneration cycle. The latter is reflected by a further decreased amount of the active Fe-O-Al sites, which agglomerate on catalyst surface with the cycle, likely associated with the hard coke residue that is not completely removed by the regeneration.

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来源期刊
Green Energy & Environment
Green Energy & Environment Energy-Renewable Energy, Sustainability and the Environment
CiteScore
16.80
自引率
3.80%
发文量
332
审稿时长
12 days
期刊介绍: Green Energy & Environment (GEE) is an internationally recognized journal that undergoes a rigorous peer-review process. It focuses on interdisciplinary research related to green energy and the environment, covering a wide range of topics including biofuel and bioenergy, energy storage and networks, catalysis for sustainable processes, and materials for energy and the environment. GEE has a broad scope and encourages the submission of original and innovative research in both fundamental and engineering fields. Additionally, GEE serves as a platform for discussions, summaries, reviews, and previews of the impact of green energy on the eco-environment.
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