Chemical looping hydrogen (CLH) production is a promising pathway that can offer both use of renewable resources and efficient CO₂ capture capabilities. Here, we use the CALculation of PHase Diagrams (CALPHAD) thermodynamic database to study the water conversion capability of metal oxides (MO_x) for CLH. We report the discovery of iron-based oxides with theoretical hydrogen yields up to 8 times higher than those of state-of-the-art oxides (e.g., ceria and ferrites). More specifically, Fe_0.4Co_0.6O_x is found to have a theoretical conversion efficiency capability > 50% at 700°C. Experimental results are presented, and a technoeconomic model quantifies the importance of MO_x oxygen capacity and water conversion in this process. This reflects the potential of CLH production with a hydrogen cost of $1.25 ± $0.38/kg at a scale of 50 tons per day. This is comparable to steam methane reforming but with the added benefit of producing a stream of pure CO₂.

化学循环制氢（CLH）生产是一种有前途的途径，既可以提供可再生资源的利用，又可以提供有效的CO ₂捕集能力。在这里，我们使用相图计算（CALPHAD）热力学数据库来研究金属氧化物（MO _x）对CLH的水转化能力。我们报告发现理论上氢产率比最先进的氧化物（例如二氧化铈和铁氧体）高8倍的铁基氧化物的发现。更具体地，发现Fe _0.4 Co _0.6 O _x在700℃下具有大于50％的理论转化效率能力。提出了实验结果，并建立了一个技术经济模型来量化MO _x的重要性此过程中的氧气容量和水转化率。这反映出每天生产50吨规模的氢气成本为1.25美元±0.38美元/公斤的CLH生产潜力。这可与蒸汽甲烷重整相媲美，但具有产生纯CO _2料流的额外好处。