Highly enhanced CO2 and H2 adsorption properties were achieved with a series of phenolic resin-based carbon spheres (resorcinol–formaldehyde carbon (RFC) and phenol–formaldehyde carbon (PFC)) by carbonization of RF and PF polymer (RFP and PFP) spheres synthesized via a sol–gel reaction and subsequent activation with hot CO2 or NH3 treatment. Monodisperse and size-tunable (100–600 nm) RFC and PFC spheres had intrinsic nitrogen contents (ca. 1.5 wt %), which are attributed to the synthesis conditions that utilized NH3 as a basic catalyst as well as nitrogen precursor. A series of CO2-activated and N-doped RFC and PFC spheres showed almost perfect correlation (R 2 = 0.99) between CO2 adsorption capacities and accumulated pore volumes of fine micropores (ultramicropore <1 nm) obtained using the nonlocal density functional theory (NLDFT) model. Interestingly, NH3 activation served not only as an effective method for heteroatom doping (i.e., nitrogen) into the carbon framework but also as an excellent activation process to fine-tune the surface area and pore size distribution (PSD). Increased nitrogen doping levels up to ca. 2.8 wt % for NH3-activated RFC spheres showed superior CO2 adsorption capacities of 4.54 (1 bar) and 7.14 mmol g–1 (1 bar) at 298 and 273 K, respectively. Compared to CO2-activated RFC spheres with similar ultramicropore volume presenting CO2 uptakes of 4.41 (1 bar) and 6.86 mmol g–1 (1 bar) at 298 and 273 K, respectively, NH3-activated nitrogen-enriched RFC was found to have elevated chemisorption ability. Moreover, prolonged activation of RFC and PFC spheres provided ultrahigh surface areas, one of which reached 4079 m2g–1 with an unprecedented superb H2 uptake capacity of 3.26 wt % at 77 K (1 bar), representing one of the best H2 storage media among carbonaceous materials and metal–organic frameworks (MOFs).

The electrochemical performance of MOFs for supercapacitor and oxygen reduction reaction applications is significantly improved when conjugated with conductive and 3D connected nanoporous carbon matrices.

Polyimide is one of the most important high-performance polymers, which is widely used due to its excellent mechanical performance and thermal stability. Unlike the conventional synthetic approach, hydrothermal polymerization enables the synthesis of polyimides without any toxic solvent and catalyst. Herein, we report the synthesis of polyimide-based microparticles (PIMs) through one-pot hydrothermal polymerization using precursors of mellitic acid (MA) and three isomers of phenylenediamine (PDA) (o-, m-, and p-PDA). Interestingly, the chemical composition of PIMs was highly tunable with the choice of the PDA isomers, leading to considerable morphological differences between PIMs. The molecular dynamics simulation and density functional theory calculation of the polymeric segment of the respective PIMs suggested that the relative ratio of amide to imide influenced the rotational freedom of the polymeric chains and number of hydrogen bonds, resulting in the well-defined structures of respective PIMs. Considering the highly tunable nature of PIMs coupled with the facile synthetic protocol, we anticipate prospective potentials of PIMs in materials, energy, and composite applications.

ORR activity of Fe, Si, and N co-doped carbons (FeSiNCs) is first reported that DFT calculations reveal the origin of the ORR activity of FeSiNC, presenting excellent ORR activity and single-cell performances in Zn–air battery and AEMFC.

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Ionic liquids (ILs) or solidified ionic liquids, known as ionogels, have been actively employed in supercapacitors (SCs) owing to their superior electrochemical stabilities to aqueous and organic electrolytes. However, initial efforts of using ILs and ionogels in SCs were not successful because bulky and sluggish ions cannot effectively access tiny pores of conventional microporous carbons. To address this, a strategy is developed to optimize the electrochemically active surfaces of carbonaceous electrodes and thus to improve the energy storage performance by incorporating 3D ordered/interconnected large mesoporous carbons with ionogel electrolytes. Precisely designed large mesopores interconnected via windows promote mass transport of the electrolyte ions within the solid ionogel electrolytes and effectively utilize the surface of the carbon electrodes for capacitive energy storage, giving rise to record‐high energy storage performance that surpasses the upper bound of the Ragone plots of the current state‐of‐the‐art SCs. In addition, all‐solid‐state SCs with outstanding bending/folding durability are successfully demonstrated. Overall, these results provide critical insight into surface utilization of carbon electrodes as well as capacitive energy storage, when viscous and bulky ILs or ionogels are used as electrolytes.