Ordered macroporous graphenic carbon-based framework materials and their low-temperature co-sacrificial template synthesis mechanism

Ordered porous functional materials such as microporous metal-organic frameworks and mesoporous silica series have been widely explored from both science and engineering perspectives due to their unique physiochemical merits and broad potential applications. However, there is still a lack of ordered macroporous materials, particularly with high crystallinity that can effectively extend these ordering-based advantages to a larger scale. Through a facile co-sacrificial template sequential pyrolysis process using metal salts and colloidal crystals as precursors, here we have developed a three-dimensionally ordered macroporous framework material constructed by well-crystallized graphenic carbon and uniformly dispersed metallic nanocrystals down to subnanometer size, denoted as OMGCs. Through systematic experimental and theoretical verification by using various metal nitrate precursors, a unique atom-casting mechanism occurring on specific crystal surfaces of metallic salts is further revealed to explain its low-temperature formation mechanism at 290°C–300°C. These OMGCs may greatly expand the family of ordered porous framework materials for emerging applications.