深入了解作为高效稳定的 CO2 吸附剂的大量孔隙支撑在聚乙烯亚胺功能化中的关键作用,ACS Applied Materials & Interfaces

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深入了解作为高效稳定的 CO2 吸附剂的大量孔隙支撑在聚乙烯亚胺功能化中的关键作用
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-11-03 , DOI: 10.1021/acsami.1c17132
Yuan Meng ₁ , Tongyao Ju ₁ , Fanzhi Meng ₁ , Siyu Han ₁ , Mengzhu Song ₁ , Jianguo Jiang ₁

Affiliation

新兴的聚乙烯亚胺 (PEI) 功能化固体吸附剂由于其良好的吸附能力、可回收性和可扩展性，在实施 CO ₂捕获和分离方面取得了重大进展。作为不可缺少的底物，选择多孔固体载体在 CO _{2 的}PEI 功能化中的重要性吸附在许多以前的研究中通常被忽视，而是强调筛选胺类型或开发复杂的多孔材料。为此，我们在本研究中仔细研究了不同商业多孔载体（二氧化硅、氧化铝、活性炭和聚合物树脂）在 PEI 浸渍中的关键作用，同时考虑了多个方面。在此，目前的结果表明，丰富的较大孔结构和表面官能团有利于加载大量 PEI 分子。PEI 功能化后的各种载体在吸附容量、胺效率和相应的最佳温度方面存在很大差异。此外，更多关注多孔载体在连续吸附 - 再生循环中的长期稳定性中的作用，₂和 CO ₂净化分别作为再生策略。尤其是，在基于 SiO ₂的吸附剂中，由于尿素物质的形成而导致CO ₂诱导的降解被特别识别，这将引起对 CO ₂循环捕获的严重关注。另一方面，我们还证实采用传统的多孔载体，例如 HP20，可以实现优于合成的吸附性能（高于 4 mmol CO ₂ /g）和循环稳定性（30 次循环后损失约 1%）通过复杂的方法，确保了 PEI 功能化 CO ₂吸附剂的可用性和可扩展性。

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Insights into the Critical Role of Abundant-Porosity Supports in Polyethylenimine Functionalization as Efficient and Stable CO2 Adsorbents

The emerging polyethylenimine (PEI)-functionalized solid adsorbents have witnessed significant development in the implementation of CO₂ capture and separation because of their decent adsorption capacity, recyclability, and scalability. As an indispensable substrate, the importance of selecting porous solid supports in PEI functionalization for CO₂ adsorption was commonly overlooked in many previous investigations, which instead emphasized screening amine types or developing complex porous materials. To this end, we scrutinized the critical role of different commercial porous supports (silica, alumina, activated carbon, and polymeric resins) in PEI impregnation in this study, taking into account multiple perspectives. Hereinto, the present results identified that abundant larger pore structures and surface functional groups were conducive to loading a considerable amount of PEI molecules. Various supports after PEI functionalization had great differences in adsorption capacities, amine efficiencies, and the corresponding optimal temperatures. In addition, more attention was paid to the role of porous supports in long-term stability during the consecutive adsorption–regeneration cycles, while N₂ and CO₂ purging as regeneration strategies, respectively. Especially, CO₂-induced degradation due to urea species formation was specifically recognized in a SiO₂-based adsorbent, which would induce serious concerns in CO₂ cyclic capture. On the other side, we also confirmed that adopting conventional porous supports, for example, HP20, could achieve superior adsorption performance (above 4 mmol CO₂/g) and cyclic stability (around 1% loss after 30 cycles) rather than the ones synthesized through complex approaches, which ensured the availability and scalability of PEI-functionalized CO₂ adsorbents.

更新日期：2021-11-17

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