Biomass-based N-rich porous carbon materials for CO2 capture and in situ conversion.
Biomass-based N-rich porous carbon materials for CO2 capture and in situ conversion.
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用于二氧化碳捕获和原位转化的生物质基富氮多孔碳材料。
DOI：
10.1002/cssc.202201004
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发表时间：
2022
期刊：
影响因子：
8.4
通讯作者：
Liang‐Nian He
中科院分区：
文献类型：
--
作者：
Weidi Xie;Xiangyang Yao;Heng Li;Hong‐Ru Li;Liang‐Nian He
捕获CO2并随后转化为有价值的化学品引起了广泛的关注。本文以生物质废弃物豆渣为前驱体，制备了一系列具有高比表面积和孔容的生物质基富氮多孔炭材料。氮的含量高达4%，并以吡啶-N、吡咯-N等不同形式存在于碳骨架中。超微孔（孔径< 0.7 nm）和含氮基团的协同作用使材料表现出高的CO2吸附容量，在0 oC和25 oC大气压下分别达到6.3和3.6 mmol g-1。此外，固体核磁共振结果表明，含氮基团与CO2之间存在充分的相互作用，捕获的CO2可能以氨基甲酸酯的形式被活化，这有利于后续的转化。以合成的多孔炭材料为载体，Zn Ⅱ为催化中心，制备了负载型催化剂，并成功地用于CO2与炔丙胺的羧化环化反应，合成了3苄基5亚甲基恶唑烷2酮。结果验证了CO2捕集和原位转化有效地生产高附加值的化学品。在这个过程中，捕获的CO2可以在温和的条件下活化并固定成化学品。更重要的是，可以避免CO2解吸和吸附剂再生过程中的能耗.将固体废物和二氧化碳转化为有价值的化学品提供了一个一石三鸟的绝妙策略。
Capturing CO2 and subsequently converting into valuable chemicals has attracted extensive attention. Herein, a series of biomass-based N-rich porous carbon materials with high specific surface area and pore volume were prepared using biomass waste soybean dregs as precursors. The nitrogen content was up to 4% with different forms in the carbon skeleton such as pyridine-N, pyrrole-N. The synergistic effect of ultra-micropore (pore size < 0.7 nm) and N-containing groups renders the materials exhibit a high CO2 adsorption capacity, reaching 6.3 and 3.6 mmol g-1 at 0 oC and 25 oC under atmosphere pressure respectively. In addition, the sufficient interaction between N-containing groups and CO 2 was demonstrated by solid state NMR, the captured CO 2 was activated in the form of carbamate possibly, which is conducive to subsequent conversion. Therefore, the supported catalyst with the as-synthetic porous carbon material as the carrier and Zn II as catalytic sites was prepared and successfully applied for carboxylative cyclization of propargylic amine with CO 2 to afford the 3-benzyl-5-methyleneoxazolidin-2-one. The results validate CO 2 capture and in situ conversion work effectively to produce highly value-added chemicals. In this process, the captured CO 2 can be activated and fixed into chemicals in mild conditions. More importantly, the energy consumption in CO 2 desorption and adsorbent regeneration can be avoided. The valorization of both solid waste and CO 2 to valuable chemicals provides an elegant strategy of killing three birds with one stone.