Villalgordo-Hernández David, Grau-Atienza Aida, García-Marín Antonio A, Ramos-Fernández Enrique V, Narciso Javier
Laboratorio de Materiales Avanzados, Departamento de Química Inorgánica, Instituto Universitario de Materiales de Alicante, Universidad de Alicante, Apartado 99, 03080 Alicante, Spain.
Instituto de Investigación Sanitaria y Biomédica de Alicante (ISABIAL), 03010 Alicante, Spain.
Materials (Basel). 2022 Mar 25;15(7):2415. doi: 10.3390/ma15072415.
Nowadays one of the biggest challenges for carbon materials is their use in CO capture and their use as electrocatalysts in the oxygen reduction reaction (ORR). In both cases, it is necessary to dope the carbon with nitrogen species. Conventional methods to prepare nitrogen doped carbons such as melamine carbonization or NH treatment generate nitrogen doped carbons with insufficient nitrogen content. In the present research, a series of activated carbons derived from MOFs (ZIF-8, ZIF-67) are presented. Activated carbons have been prepared in a single step, by pyrolysis of the MOF in an inert atmosphere, between 600 and 1000 °C. The carbons have a nitrogen content up to 20 at.% and a surface area up to 1000 m/g. The presence of this nitrogen as pyridine or pyrrolic groups, and as quaternary nitrogen are responsible for the great adsorption capacity of CO, especially the first two. The presence of Zn and Co generates very different carbonaceous structures. Zn generates a greater porosity development, which makes the doped carbons ideal for CO capture. Co generates more graphitized doped carbons, which make them suitable for their use in electrochemistry.
如今，碳材料面临的最大挑战之一是其在二氧化碳捕获中的应用以及作为氧还原反应（ORR）中的电催化剂的应用。在这两种情况下，都需要用氮物种对碳进行掺杂。制备氮掺杂碳的传统方法，如三聚氰胺碳化或氨处理，所产生的氮掺杂碳的氮含量不足。在本研究中，展示了一系列源自金属有机框架（ZIF-8、ZIF-67）的活性炭。通过在惰性气氛中于600至1000°C之间对金属有机框架进行热解，一步制备出了活性炭。这些碳的氮含量高达20原子百分比，表面积高达1000平方米/克。这种以吡啶或吡咯基团形式存在的氮以及季氮的存在，是二氧化碳具有高吸附容量的原因，尤其是前两者。锌和钴的存在产生了非常不同的碳质结构。锌产生了更大的孔隙发展，这使得掺杂碳成为二氧化碳捕获的理想材料。钴产生了更多石墨化的掺杂碳，这使得它们适用于电化学领域。
