<br>高铜分散度的Cu@SiO2催化剂用于对氯硝基苯化学选择加氢,Chemical Engineering Journal

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高铜分散度的Cu@SiO2催化剂用于对氯硝基苯化学选择加氢
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2024-03-26 , DOI: 10.1016/j.cej.2024.150652
Xinhui Li , Ruiheng Zhu , Baoquan Sun , Like Chen , Hongwei Yang , Xiaohui Liu , Yong Guo , Yanqin Wang

对氯硝基苯（p-CNB）的选择性加氢不仅具有重要的工业重要性，而且也是选择性研究的重要模型反应。尽管非贵金属Cu已被证明是双金属催化剂中的有效促进剂，但Cu作为单一活性金属同时实现高转化率和高选择性的报道很少。在这项工作中，通过简单的溶胶制备了具有高比表面积（509.8–694.3 m2/g）、高铜分散度（58.4–69.6%）和小粒径（2.0–3.0 nm）的Cu@SiO2催化剂。凝胶法。该催化剂完全抑制脱氯反应，实现对CNB的完全转化，对氯苯胺(p-CAN)的选择性为99.9%。其微观结构、组成、化学状态、吸附和反应行为已通过催化剂的各种常规非原位表征和对-CNB加氢的原位DRIFT进行了鉴定。有趣的是，即使在高负载量下，催化剂中的Cu也能高度分散，从而表现出良好的催化活性。此外，Cu催化剂对p-CNB表现出独特的吸附性能，这可能是其良好性能的因素之一。这项工作不仅通过简单的方法提供了即使在高负载量下也具有高Cu分散度的选择性加氢催化剂，而且揭示了p-CNB吸附模式的重要性，为未来开发更高效的催化剂提供指导。

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Cu@SiO2 catalyst with high copper dispersion for chemoselective hydrogenation of p-chloronitrobenzene

Selective hydrogenation of p-chloronitrobenzene (p-CNB) is not only of significant industrial importance, but also an important model reaction for selectivity investigation. Despite non-precious metal Cu has been proven to be an effective promoter in bimetallic catalysts, Cu as a single active metal achieving both high conversion and high selectivity are rare reported. In this work, Cu@SiO2 catalysts with high specific surface area (509.8–694.3 m2/g), high Cu dispersion (58.4–69.6 %), and small particle size (2.0–3.0 nm) has been prepared by a simple sol–gel method. The catalysts completely suppress the dechlorination reaction, achieving complete conversion of p-CNB with 99.9 % selectivity for p-chloroaniline (p-CAN). Its microstructure, composition, chemical state, adsorption and reaction behavior have been identified by various conventional ex-situ characterizations of catalysts and in-situ DRIFTs of hydrogenation of p-CNB. Interestingly, even at high loadings, Cu in the catalyst could be highly dispersed, thus exhibiting good catalytic activity. In addition, the Cu catalyst exhibits unique adsorption performance towards p-CNB, which perhaps one of the factors for its good performance. This work not only provides a selective hydrogenation catalyst with high Cu dispersion even at high loading amount by a simple method and but also reveals the importance of the adsorption mode of p-CNB, providing guidance for the development of more efficient catalysts in the future.

更新日期：2024-03-26

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