文献类型：期刊文献

中文题名：Ni-MgO/CaO中空微球受限空间强化CO_(2)捕集与原位转化制合成气

英文题名：Confinement-enhanced integrated CO_(2)capture and in-situ conversion from high-temperature flue gas to syngas over Ni-MgO/CaO hollow microsphere

作者：贾中昊[1];邵斌[1];谢志成[1];胡军[1]

机构：[1]华东理工大学化学与分子工程学院,上海200237

年份：2025

卷号：31

期号：6

起止页码：25

中文期刊名：洁净煤技术

外文期刊名：Clean Coal Technology

收录：;北大核心:【北大核心2023】；

基金：国家自然科学基金资助项目(22278126,22408095,22250005);国家重点研发计划资助项目(2024YFA1509801);中国博士后科学基金资助项目(BX20240116,2023M741170)。

语种：中文

中文关键词：中空微球;受限空间;双功能材料;CO_(2)捕集与原位转化;合成气

外文关键词：hollow microspheres;confined space;dual-functional materials;CO_(2)capture and in-situ conversion;syngas

摘要：CO_(2)捕集与原位转化(iCCC)技术是解决全球气候变暖的有效技术路径,将iCCC技术应用于工业高温烟气CO_(2)捕集与原位逆水煤气变换(RWGS)反应过程,可以充分利用高温烟气的热能,在同一装置下实现CO_(2)原位转化为合成气。双功能材料理性设计是实现高效iCCC技术的关键。以NaOH活化的多孔碳球为硬模板,通过Ca、Mg、Ni金属离子的共吸附和煅烧去碳模板,得到了具有中空微球结构的系列xNi-MgO/CaO双功能材料。其中空微球结构不仅降低了CO_(2)吸附过程的扩散阻力、同时还提供了CaO/CaCO_(3)在吸附过程中体积膨胀的缓冲空间;在中空微球受限空间上形成的NiO-MgO固溶体作为物理屏障分隔催化位点Ni^(0)颗粒,有效抑制活性金属在高温下的烧结。通过筛选Ni/Mg比例和反应温度、H_(2)体积分数等反应条件,考察了xNi-MgO/CaO双功能材料的等温CO_(2)捕集和原位加氢转化性能。在优化反应条件下,反应温度为650℃、氢气体积分数为10%时,10Ni-MgO/CaO在10次吸附?转化循环中材料的CO_(2)吸附量保持在10 mmol/g,CO_(2)转化率维持在94%以上,CO选择性稳定在100%。动力学研究进一步证明了Ni-MgO/CaO中空微球受限空间结构对CO_(2)捕集与加氢反应速率的强化作用。
CO_(2)capture and in-situ conversion(iCCC)technology can play a crucial role in mitigating global climate change.When the iCCC technology is applied to the CO_(2)capture from the high-temperature flue gas,its thermo-energy can be directly converted CO_(2)into the syngas during CO_(2)conversion at the same fixed bed.The rational design of efficient dual functional materials(DFMs)is key to achieve high-efficiency iCCC processes.Here,we synthesized a series of xNi-MgO/CaO DFMs with varying Ni/Mg ratios by a hard template method using NaOH-activated porous carbon spheres.The structure of the hollow microsphere not only reduces the diffusion resistance during CO_(2)adsorption but also provides buffer space to accommodate the volume expansion of CaO/CaCO_(3)during the iCCC process.In addition,the NiO-MgO solid solution formed within the confined space of the hollow microspheres acts as a physical barrier,isolating the catalytic Ni^(0) particles and effectively preventing the sintering of Ni nanoparticle at high temperatures.By optimizing the Ni/Mg ratio,reaction temperature,and H_(2) concentration,the iCCC performance of the xNi-MgO/CaO DFMs were evaluated.Under the optimal reaction temperature of 650℃and H_(2) concentration of 10%,the 10Ni-MgO/CaO DFM exhibited a CO_(2)adsorption capacity of 10 mmol/g,a CO_(2)conversion efficiency above 94%with a 100%CO selectivity after 10 adsorption-conversion cycles.Kinetic studies further demonstrated that the confined space in the Ni-MgO/CaO DFM significantly enhances the reaction rates of iCCC to syngas.