福州大学Yu Luo研究小组近日取得一项新成果，他们的最新研究通过构建金属氧化物界面促进了氨分解产氢。相关论文于2024年1月23日发表在《结构化学》杂志上。

在这项工作中，通过在Ni纳米颗粒(NPs)上涂覆铈，该课题组发现Ni-CeO₂界面产生了一种特殊的效果，与原始Ni相比，它可以将氨的催化分解提高10倍以上。动力学分析表明，重组N₂脱附是反应的速率决定步骤(RDS)， Ni-CeO₂界面的加入大大提高了反应的速率决定步骤。

在此基础上，研究团队采用一锅溶胶-凝胶法制备了具有丰富Ni-Ce-O界面的Ni/CeO₂催化剂(简称s-Ni/CeO₂)。s-Ni/CeO₂催化剂表现出较高的氨分解活性，在550℃下H₂生成速率为10.5 mmol gcat^-1 min^-1。结合一系列表征，团队研究了催化剂结构与性能的关系，以进一步了解金属-氧化物界面对催化剂性能的影响。

据了解，氨分解制无碳氢引起了广泛的关注，但由于其动力学缓慢，仍然存在挑战，因此精确设计高效的低温氨分解催化剂至关重要。构建金属-载体相互作用和界面是促进催化剂的重要策略之一。

附：英文原文

Title: Boosting hydrogen production of ammonia decomposition via the construction of the metal-oxide interfaces

Author: anonymous

Issue&Volume: 2024-01-23

Abstract: The ammonia decomposition for the production of carbon–free hydrogen has triggered great attentions yet still remains challenging due to its sluggish kinetics, posting the importance of precise design of the efficient catalysts for ammonia decomposition under low temperatures. Constructing the metal–support interaction and interface is one of the most important strategies for promoting catalysts. In this work, by coating ceria onto the Ni nanoparticles (NPs), we discover that the Ni–CeO2 interfaces create an exceptional effect to enhance the catalytic decomposition of ammonia by over 10 folds, compared with the pristine Ni. The kinetic analysis demonstrates that the recombinative N2 desorption is the rate–determining step (RDS) and the Ni–CeO2 interface greatly increase the RDS. Based on these understandings, a strategy to fabricate the Ni/CeO2 catalyst with abundant Ni–Ce–O interfaces via one–pot sol–gel method was employed (hereafter denoted to s-Ni/CeO2). The s–Ni/CeO2 catalyst show a high activity for ammonia decomposition, achieving a H2 formation rate of 10.5 mmol gcat–1 min–1 at 550 °C. Combined with a series of characterizations, the relationship between the catalyst structure and the performance was investigate for further understanding the effect of the metal–oxide interfaces.

DOI: 10.1016/j.cjsc.2024.100236

Source: http://cjsc.ac.cn/cms/issues/556