碳氧双缺陷强化钌基氨分解催化剂，这一成果由北京工业大学邓积光小组经过不懈努力而取得。相关论文发表在2025年3月27日出版的《德国应用化学》杂志上。

虽然氨被广泛认为是最有前途的氢储存和转化候选者之一，但涉及氨分解的催化机制仍然不够清楚，催化剂的稳定性仍然存在重大挑战。在本研究中，采用简单的方法合成了具有双缺陷位的Ru/CeO₂-CNTs催化剂，在500°C下的产氢速率达到2230 mmol/gRu/min，优于大多数Ru基催化剂。实验表征和理论计算表明，CeO₂-CNT界面通过碳氧相互作用促进氧空位（Ov）和碳缺陷（Cd）的形成。这些缺陷增强了载体向钌纳米粒子（NPs）的电子转移，调节了NH₃的吸附和活化，以及吸附的N种（N*）的重组和解吸。

此外，CeO₂涂层显著提高了CNTs的稳定性，从而减弱了在高温和富氢条件下的不良反应。该研究提出了一种合理的设计策略，通过构建双缺陷位点来增强NH₃分解的多个初级阶段，为在恶劣环境下设计高效耐用的催化剂提供了新的见解。

附：英文原文

Title: Carbon and Oxygen Double Defects Enhanced Ru-based Catalyst for Ammonia Decomposition

Author: Likang Lv, Peiqi Chu, Tong Han, Yunpeng Jiang, Zhiwei Wang, Yuxi Liu, Hongxing Dai, Lu Wei, Jiguang Deng

Issue&Volume: 2025-03-27

Abstract: Although ammonia is widely recognized as one of the most promising candidates for hydrogen storage and transformation, the catalytic mechanisms involved in ammonia decomposition remain insufficiently understood, and the stability of catalysts continues to present significant challenges. In this study, Ru/CeO2-CNTs catalysts with double defect sites were synthesized by a straightforward method, achieving an outstanding hydrogen production rate of 2,230 mmol/gRu/min at 500 °C, outperforming most Ru-based catalysts. Experimental characterization and theoretical calculations revealed that the CeO2-CNT interface promotes the formation of oxygen vacancies (Ov) and carbon defects (Cd) through carbon-oxygen interactions. These defects enhance electron transfer from the support to Ru nanoparticles (NPs), modulate NH3 adsorption and activation, as well as the recombination and desorption of adsorbed N species (N*). Moreover, the coating of CeO2 significantly improved the stability of CNTs, which weakens undesired reaction under high temperature and hydrogen-rich conditions. The study introduced a rational design strategy that enhance the multiple elementary stages of the NH3 decomposition by constructing double defect sites, and offering new insights into the design of efficient and durable catalysts under harsh environment.

DOI: 10.1002/anie.202501898

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202501898