Solar methane dry reforming (MDR) reaction is a highly promising technology for long‐term energy storage due to its eco‐friendly nature and high‐value‐added product. Numerous present works mainly focused on the photo‐thermal catalysts, few of them discussed photo‐thermal coupled kinetics. Therefore, this article proposed a light‐dependent kinetic model for MDR. In the model, not only the effect of temperature and species concentration were included, but also the radiation was considered, which is different from the conventional kinetic model. Solar radiation is divided into thermal‐effect and light‐promoted‐effect part and coupled with the heat and mass transportation and chemical reaction. The average relative error of established model is only 0.97% under dark condition, and 13.2% under light condition. Then, the impacts of operating condition in a cavity reactor were investigated by established coupled optical‐photo‐thermal dynamics–computational fluid dynamic model to improve the efficiency of chemical conversion. The results show that when GHSV is 48.21 h−1, light increased the reaction rate by 1.59 times and thermochemical energy storage efficiency by 18.5%. When CH4/CO2 = 1, the formation rates of syngas and thermochemical energy storage efficiency are the highest. This work provides a highly coupled photo‐thermal kinetic model and a method for modeling and condition optimization.

中文翻译：

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甲烷干重整光依赖光热动力学模型的建立及空腔反应器性能优化

太阳能甲烷干重整（MDR）反应因其环保性和高附加值产品而成为一种极具前景的长期储能技术。目前的许多工作主要集中在光热催化剂上，很少讨论光热耦合动力学。因此，本文提出了MDR的光依赖性动力学模型。该模型不仅考虑了温度和物质浓度的影响，还考虑了辐射，这与传统的动力学模型不同。太阳辐射分为热效应和光促效应部分，并与热质传输和化学反应耦合。建立的模型在黑暗条件下平均相对误差仅为0.97%，在光照条件下平均相对误差为13.2%。然后，通过建立光学-光热动力学-计算流体动力学耦合模型，研究空腔反应器中操作条件的影响，以提高化学转化效率。结果表明，当 GHSV 为 48.21 h 时−1，光反应速率提高1.59倍，热化学储能效率提高18.5%。当CH4/CO2=1时，合成气生成率和热化学储能效率最高。这项工作提供了高度耦合的光热动力学模型以及建模和条件优化的方法。