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Ammonia recently has gained increasing attention as a carrier for the efficient and safe usage of hydrogen to further advance the hydrogen economy. However, there is a pressing need to develop new ammonia synthesis techniques to overcome the problem of intense energy consumption associated with the widely used Haber–Bosch process. Chemical looping ammonia synthesis (CLAS) is a promising approach to tackle this problem, but the ideal redox materials to drive these chemical looping processes are yet to be discovered. Here, by mining the well-established MP database, the reaction free energies for CLAS involving 1699 bicationic inorganic redox pairs are screened to comprehensively investigate their potentials as efficient redox materials in four different CLAS schemes. A state-of-the-art machine learning strategy is further deployed to significantly widen the chemical space for discovering the promising redox materials from more than half a million candidates. Most importantly, using the three-step H2O-CL as an example, a new metric is introduced to determine bicationic redox pairs that are “cooperatively enhanced” compared to their corresponding monocationic counterparts. It is found that bicationic compounds containing a combination of alkali/alkaline-earth metals and transition metal (TM)/post-TM/metalloid elements are compounds that are particularly promising in this respect.
中文翻译：
最近，氨作为高效和安全使用氢以进一步推动氢经济的载体而受到越来越多的关注。然而，迫切需要开发新的氨合成技术，以克服与广泛使用的 Haber-Bosch 工艺相关的高能耗问题。化学链氨合成 (CLAS) 是解决这一问题的一种有前途的方法，但驱动这些化学链过程的理想氧化还原材料尚未被发现。在这里，通过挖掘完善的 MP 数据库，筛选了涉及 1699 个双阳离子无机氧化还原对的 CLAS 的反应自由能，以全面研究它们在四种不同 CLAS 方案中作为高效氧化还原材料的潜力。进一步部署了最先进的机器学习策略，以显着扩大化学空间，以从超过 50 万个候选者中发现有前途的氧化还原材料。最重要的是，使用三步 H2 O-CL 作为一个例子，引入了一个新的度量来确定与其相应的单阳离子对应物相比“协同增强”的双阳离子氧化还原对。发现包含碱金属/碱土金属和过渡金属(TM)/后TM/准金属元素的组合的双阳离子化合物是在这方面特别有前途的化合物。 |
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