Zheng Jialin, Wang Xiaojian, Zi Xin, Zhang Hang, Chen Heping, Pensa Evangelina, Liu Kang, Fu Junwei, Lin Zhang, Chai Liyuan, Cortés Emiliano, Liu Min
Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, School of Physics, Central South University, Changsha, Hunan, 410083, P. R. China.
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083, P. R. China.
Adv Sci (Weinh). 2025 Mar;12(9):e2413203. doi: 10.1002/advs.202413203. Epub 2025 Jan 10.
Perfluorinated compounds (PFCs) are emerging environmental pollutants characterized by their extreme stability and resistance to degradation. Among them, tetrafluoromethane (CF) is the simplest and most abundant PFC in the atmosphere. However, the highest C─F bond energy and its highly symmetrical structure make it particularly challenging to decompose. In this work, a yolk-shell AlO micro-reactor is developed to enhance the catalytic hydrolysis performance of CF by creating a local autothermic environment. Finite element simulations predict that the yolk-shell AlO micro-reactor captures the heat released during the catalytic hydrolysis of CF, resulting in a local autothermic environment within the yolk-shell structure that is 50 °C higher than the set temperature. The effectiveness of this local autothermic environment is experimentally confirmed by in situ Raman spectroscopy. As a result, the obtained yolk-shell AlO micro-reactor achieves 100% CF conversion at a considerably low temperature of 580 °C for over 150 h, while hollow and solid AlO structures required higher temperatures of 610 and 630 °C, respectively, to achieve the same conversion rate, demonstrating the potential of yolk-shell AlO micro-reactor to significantly reduce the energy requirements for PFCs degradation and contribute to more sustainable and effective environmental remediation strategies.
全氟化合物（PFCs）是一类新兴的环境污染物，其特点是具有极高的稳定性和抗降解性。其中，四氟甲烷（CF）是大气中最简单且含量最丰富的全氟化合物。然而，其极高的碳氟键能及其高度对称的结构使其分解极具挑战性。在这项工作中，开发了一种蛋黄壳结构的AlO微反应器，通过营造局部自热环境来提高CF的催化水解性能。有限元模拟预测，蛋黄壳结构的AlO微反应器能捕获CF催化水解过程中释放的热量，从而在蛋黄壳结构内部形成一个比设定温度高50°C的局部自热环境。原位拉曼光谱实验证实了这种局部自热环境的有效性。结果，所制备的蛋黄壳结构AlO微反应器在580°C的相当低的温度下，超过150小时实现了100%的CF转化率，而空心和实心AlO结构分别需要610°C和630°C的更高温度才能达到相同的转化率，这表明蛋黄壳结构AlO微反应器具有显著降低全氟化合物降解所需能量的潜力，并有助于实现更可持续、更有效的环境修复策略。
