A sustainable one-step strategy for highly graphitized capacitive carbons with hierarchical micro-meso-macro porosity.

Large micropore surface area, superior electrical conductivity and suitable pore size are simultaneously desired characteristics for high-performance capacitive carbons. However, these desired features tend to be mutually competing, and are generally difficult to integrate into a single carbon. Considering this challenge, we developed a sustainable, less time-demanding, pollution-free strategy to construct highly graphitized porous carbon (GPC) by one-step heat-treatment. This approach achieves the need of the abovementioned characteristics for capacitive carbons, wherein potassium ferrate works as both an activating agent and graphitization catalyst to achieve synchronous hierarchical porosity and graphitization of wasted natural wood, and the resultant carbon materials possess a large micropore surface area of 870.4 m2 g-1, a highly graphitic carbon skeleton and a well-interconnected micro-meso-macropore structure. The assembled GPC-based symmetrical capacitors exhibited a satisfactory capacitive performance in different aqueous electrolytes (H2SO4, KOH and Na2SO4), including high specific capacitance, prominent rate capability, satisfactory energy density and good cycle stability. Meanwhile, we compared the contributions of porosity and the graphitized structure to capacitive performance, and porosity was dominant in determining capacitance and the graphitized skeleton had a positive effect in enhancing the capacitive performance. In addition, we established the relationship between the structure of GPC and electrochemical capacitive performance in different aqueous electrolytes, providing a valuable reference for GPC-based supercapacitors in different practical applications. More importantly, this strategy holds great promise to sustainably convert biowaste to high-added-value capacitive carbons for advanced energy storage applications in the future.

Copper ions-assisted inorganic dynamic porogen of graphene-like multiscale microporous carbon nanosheets for effective carbon dioxide capture.

The superior ultramicroporosity and enriched surface CO2-philic sites are simultaneously required features for high-efficiency carbon-based CO2 adsorbents. Unfortunately, these characteristics are usually incompatible and difficult to integrate into one porous carbon material. Herein, we report a new copper ions (Cu2+)-assisted dynamic porogen to construct hierarchically microporous carbon nanosheets in a large scale with high heterogeneity for solving such issue. Cu2+ can be equably dispersed in precursor by coordination interactions of COO-Cu and Cu-N, which can anchor more N/O-containing species in final product. The reduced cuprous ions (Cu+) in pyrolysis process functions as a dynamic porogen to tailor uniform ultramicropores. Importantly, copper salt extracted in this synthetic procedure allows cyclic utilization, realizing a green and low-cost process. The obtained carbon sheets possess a graphene-like morphology, a high surface area and a high-proportioned multiscale microporosity, especially a high-density ultramicropores of 0.4-0.7 nm and supermicroproes of 0.8-1.5 nm. The maximized synergistic effect of morphology, high density of multi-sized ultramicroporosity and surface high heterogeneity endow the resultant microporous carbon nanosheets with the remarkable CO2 capture property, including a high uptake, a moderate adsorption heat, a good selectivity and superior recyclability.