Realization of Ideal Ba Promoter State by Simultaneous Incorporation with Co into Carbon-protective Framework for Ammonia Synthesis Catalyst

IF 24.4 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
K. Kanishka H. De Silva, Katsutoshi Sato, Takahiro Naito, Takaaki Toriyama, Tomokazu Yamamoto, Ryotaro Aso, Yasukazu Murakami, Pradeep R. Varadwaj, Ryoji Asahi, Koji Inazu, Katsutoshi Nagaoka
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Abstract

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.

Abstract Image

Abstract Image

在氨合成催化剂的碳保护框架中同时掺入Co以实现理想的Ba促进剂态
开发在温和条件下具有优异NH3合成活性的非贵金属催化剂是一个长期的目标。迄今为止报道的最好的催化剂通常需要费力的制造方法和可控的环境来制造催化剂,或者需要高温和长时间来激活催化剂。本文介绍了一种以金属硝酸盐为前驱体,水为溶剂,采用柠檬酸溶胶-凝胶法制备碳(C)基钡(Ba)促进型钴(Co)催化剂的简易一锅法。这种方法确保金属离子均匀地结合到碳框架中。得到的(Ba/Co)0.3/C催化剂的NH3合成活性为34 mmol gcat−1 h−1(350℃,1.0 MPa),稳定性良好。深入表征表明,Ba以氧化钡(BaO)的形式存在,均匀分布在碳骨架上和Co纳米颗粒周围。研究发现,在新鲜催化剂中延缓碳酸钡(BaCO3)的形成,显著降低了还原温度和还原时间(485℃/4 h),这是该方法的一个根本优势。密度泛函理论和分子动力学模拟确实支持实验观察。这种简单、经济的方法有望解决多相催化剂研究领域的广泛问题。
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来源期刊
Advanced Energy Materials
Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
41.90
自引率
4.00%
发文量
889
审稿时长
1.4 months
期刊介绍: Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.
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