Large specific surface area (SSA) carbons have been demonstrated to be effective active materials and conductive substrates for energy storage devices, such as supercapacitors and batteries, due to their designable pore structures and buffering frameworks, as well as excellent electrical conductivity and chemical stability. Recently, tremendous efforts have been made in the design and preparation of large SSA carbons as electrode materials for energy storage devices, which can significantly enhance their capacitance, power and energy density, lifespan, and preeminent safety. In this review, recent advances in the development of large SSA carbons from structures and properties, porous carbon classifications, and preparation strategies to energy storage applications in supercapacitors, lithium-ion batteries, lithium-sulfur batteries, and zinc-air batteries are discussed. Finally, current challenges, future research directions, and prospects in the development of large SSA carbons for energy storage applications are highlighted.

Platinum (Pt)-based electrocatalysts remain the only practical cathode catalysts for proton exchange membrane water electrolysis (PEMWE), due to their excellent catalytic activity for acidic hydrogen evolution reaction (HER), but are greatly limited by their low reserves and high cost. Here, we report an interfacial engineering strategy to obtain a promising low-Pt loading catalyst with atomically Pt-doped molybdenum carbide quantum dots decorated on conductive porous carbon (Pt-MoC_x@C) for high-rate and stable HER in PEMWE. Benefiting from the strong interfacial interaction between Pt atoms and the ultra-small MoC_x quantum dots substrate, the Pt-MoC_x catalyst exhibits a high mass activity of 8.00 A·mg_Pt⁻¹, 5.6 times higher than that of commercial 20 wt.% Pt/C catalyst. Moreover, the strong interfacial coupling of Pt and MoC_x substrate greatly improves the HER stability of the Pt-MoC_x catalyst. Density functional theory studies further confirm the strong metal-support interaction on Pt-MoC_x, the critical role of MoC_x substrate in the stabilization of surface Pt atoms, as well as activation of MoC_x substrate by Pt atoms for improving HER durability and activity. The optimized Pt-MoC_x@C catalyst demonstrates > 2000 h stability under a water-splitting current of 1000 mA·cm⁻² when applied to the cathode of a PEM water electrolyzer, suggesting the potential for practical applications.

Metal–organic frameworks (MOFs) with redox-active metal sites and controllable crystalline structures make it possible to access the merits of highly-efficient electrode materials in electrochemical energy storage systems. However, most MOFs suffer from low capacitance and poor cycling stability that largely thwart their application. Herein, we present the holey graphene oxide (HGO) template strategy to prepare nano two-dimensional Ni(BDC) with HGO as both template and capping agent (denoted as Ni(BDC)-HGOx, x = 10, 20, 30, and 40 according to the added HGO amount). Structural analyses reveal that HGO can significantly inhibit the Ni(BDC) agglomeration, thus offering a high ion-accessible surface area. Ni(BDC)-HGO30 with well-exposed active sites exhibits a high capacitance of 1,115.6 F·g⁻¹ at 1 A·g⁻¹ in 6 M KOH aqueous, 1.8 times that of bulk Ni(BDC). An asymmetric supercapacitor with Ni(BDC)-HGO30 as a positive electrode and activated carbon as the opposing electrode delivers an energy density of 52.5 W·h·kg⁻¹ and a power density up to 18.0 kW·kg⁻¹, with 92.5% capacitance retention after 10,000 cycles. Galvanostatic intermittent titration technique and in situ electrochemical–Raman measurements were exploited to elucidate the electrochemical behavior of Ni(BDC)-HGO30. These results pave the way for the development of rationally tuned MOF materials for enhancing supercapacitor performances.

Supercapacitors (SCs) have attracted extensive attention due to their ultrahigh power density, fast charging/discharging rate, excellent electrochemical stability and environmental friendliness. Currently, the main commercial electrode materials for SCs are carbon materials in term of low cost, excellent conductivity, large specific surface area and good electrochemical stability. Recently, various dimensional carbon materials including zero dimensional (0D) carbon materials (nanosphere, dot etc.), 1D carbon materials (nanotube, nanofiber etc.), 2D carbon materials (nanosheet) as well as 3D carbon materials have been developed for SCs. Carbon materials with different spatial dimensions have their unique properties when used as the electrode materials for SCs. In this review, recent advances in the fabrication of different dimensional carbons for SCs are summarized. Several key issues for enhancing the electrochemical properties of carbon-based SCs and some mutual relationships among various influence parameters are reviewed, and challenges and perspectives in this field are also discussed.