Developing non‐noble metal catalysts with excellent NH3 synthesis activity under mild conditions is a long‐term goal. The best catalysts reported to date often require laborious fabrication methods and controlled environments to fabricate the catalysts or high temperatures and long times to activate the catalysts. This work introduces a facile one‐pot method to fabricate carbon (C)‐based, barium (Ba)‐promoted cobalt (Co) catalysts via the citric acid sol–gel method with metal nitrates as precursors and water as the solvent. This approach ensures the homogeneous incorporation of metal ions into the carbon framework. The resulting (Ba/Co)0.3/C catalyst demonstrates an outstanding NH3 synthesis activity of 34 mmol gcat−1 h−1 (350 °C, 1.0 MPa) with excellent stability. In‐depth characterizations reveal that Ba exists as barium oxide (BaO), uniformly distributed on the carbon framework and around the Co nanoparticles. It is uncovered that retarding barium carbonate (BaCO3) formation in the fresh catalyst significantly reduces the reduction temperature and time (485 °C/4 h), which is a fundamental advantage of this method. Density functional theory and molecular dynamics simulations indeed support the experimental observations. It is anticipated that this simple and economical strategy will resolve the issues in a broad field of heterogeneous catalyst research.

中文翻译：

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通过与 Co 同时掺入氨合成催化剂的碳保护框架中实现理想的 Ba 启动子状态


在温和条件下开发具有优异 NH3 合成活性的非贵金属催化剂是一个长期目标。迄今为止报道的最佳催化剂通常需要费力的制造方法和受控环境来制造催化剂，或者需要高温和长时间来激活催化剂。这项工作介绍了一种简单的一锅法，以金属硝酸盐为前驱体，以水为溶剂，通过柠檬酸溶胶-凝胶法制备碳 （C） 基钡 （Ba） 促进的钴 （Co） 催化剂。这种方法可确保金属离子均匀地掺入碳框架中。所得的 （Ba/Co）0.3/C 催化剂表现出出色的 NH3 合成活性，为 34 mmol gcat−1 h−1（350 °C，1.0 MPa），具有优异的稳定性。深入的表征表明，Ba 以氧化钡 （BaO） 的形式存在，均匀分布在碳框架上和 Co 纳米颗粒周围。结果表明，延缓新催化剂中碳酸钡 （BaCO3） 的形成可显著降低还原温度和时间 （485 °C/4 h），这是该方法的一个基本优势。密度泛函理论和分子动力学模拟确实支持实验观察结果。预计这种简单而经济的策略将解决非均相催化剂研究的广泛领域中的问题。