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IF 3.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2025-03-10 DOI:10.1016/j.mcat.2025.115008

Gang Cheng , Junhua Zou , Xinjie Song , Hongmei Tang , Qing Gong , Hongxian Liu , Wenxin Dai

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引用次数: 0

摘要

将 NO 向上循环转化为 NH3 为 NO 净化和 NH3 生产提供了一种双赢策略。在这项工作中，我们报告了一种在低温常压下通过光助热催化 CO 还原 NO 和 H2O 生产 NH3 的方法。在该研究中，我们使用了一种具有电子富集钯和氧空位双活性位点的钯/二氧化钛模型催化剂。结果表明，只有在 120 ℃ 时才能实现氮氧化物的完全转化，而在 180 ℃ 以下，Pd/TiO2 可获得超过 55.0% 的 NH3 选择性。一系列的光谱和理论研究表明，吸附在钯位点上的 CO 和界面氧空位上离解的 H2O 首先会相互作用，在原位生成活性 *H 物种，然后同样吸附在界面氧空位上的 NO 会逐渐被 *H 加氢生成 NH3。光照射通过促进氧空位的形成和电子传递来增强 CO 和 NO 的活化和 H2O 的解离，从而进一步强化了这一过程。这项工作为通过光热催化 CO 还原 NO 和 H2O 生成 NH3 提供了宝贵的见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

NH3 synthesis via photo-assisted thermalcatalytic NO and H2O reduction by CO over Pd/TiO2: Synergistic effects of Pd and oxygen vacancies

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NH3 synthesis via photo-assisted thermalcatalytic NO and H2O reduction by CO over Pd/TiO2: Synergistic effects of Pd and oxygen vacancies

Upcycling of NO into NH₃ provided a win-win strategy for NO purification and NH₃ production. In this work, we reported an approach for NH₃ production via photo-assisted thermalcatalytic NO and H₂O reduction by CO at low temperature and atmospheric pressure. Herein, a Pd/TiO₂ model catalyst with electron-enriched Pd and oxygen vacancies dual active sites was applied. The results showed that full NO conversion was realized only at 120 °C, and a beyond 55.0% NH₃ selectivity could be obtained below 180 °C over Pd/TiO₂. A series of collective spectroscopic and theoretical investigations revealed that CO adsorbed at Pd site and H₂O dissociated at interfacial oxygen vacancies would first interact to in situ generate active *H species, and then NO also adsorbed at interfacial oxygen vacancies was gradually hydrogenated by *H to produce NH₃. Light irradiation further reinforced this process by promoting oxygen vacancies formation and electron transfer for enhancing CO and NO activation and H₂O dissociation. This work provides a valuable insight into NH₃ production via photothermal catalytic NO and H₂O reduction by CO.

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods