Aqueous Zn-ion batteries present a low cost, safe, and high-energy battery technology, but suffer from the lack of suitable cathode materials because of the sluggish intercalation kinetics associated with the large size of hydrated zinc ions. Herein we report an effective and general strategy to transform inactive intercalation hosts into efficient Zn 2+ storage materials through intercaltion energy tuning. Using MoS 2 as a model system, we show both experimentally and theoretically that even hosts with originally poor Zn 2+ diffusivity can allow fast Zn 2+ diffusion. Through simple interlayer spacing and hydrophilicity engineering that can be experimentally achieved by oxygen incorporation, the Zn 2+ diffusivity is boosted by 3 orders of magnitude, effectively enabling the otherwise barely active MoS 2 to achieve a high capacity of 232 mAh g -1 that is 10 times as its pristine form. The strategy developed in our work can be generally applied for enhancing the ion Experimental details and additional supporting data as noted in the main text (PDF).

Supercapacitors (SCs) have experienced a significant increase in research activity and commercialization during the past few decades. As the primary and most important electrode active material for commercial SCs, porous carbon is produced at an industrial‐scale through traditional carbonization‐activation strategies. Nevertheless, commercial porous carbon materials have some disadvantages such as high production cost, corrosion of equipment, and emission of toxic gases and byproduct pollutants during production. In recent years, huge efforts have been made to develop novel synthesis strategies for porous carbon materials. This review focuses on the pore formation mechanisms in traditional carbonization‐activation methods, emerging activation methods, template methods, self‐template methods, and novel emerging methods for the synthesis of porous carbons for SCs. Strategies developed so far for the synthesis of porous carbon materials are summarized. The mechanisms and recent advances for each strategy are reviewed. Furthermore, future directions and synthesis strategies for porous carbons are proposed.

In this work, a simple lignin‐based laser lithography technique is developed and used to fabricate on‐chip microsupercapacitors (MSCs) using 3D graphene electrodes. Specifically, lignin films are transformed directly into 3D laser‐scribed graphene (LSG) electrodes by a simple one‐step CO2 laser irradiation. This step is followed by a water lift‐off process to remove unexposed lignin, resulting in 3D graphene with the designed electrode patterns. The resulting LSG electrodes are hierarchically porous, electrically conductive (conductivity is up to 66.2 S cm−1), and have a high specific surface area (338.3 m2 g−1). These characteristics mean that such electrodes can be used directly as MSC electrodes without the need for binders and current collectors. The MSCs fabricated using lignin laser lithography exhibit good electrochemical performances, namely, high areal capacitance (25.1 mF cm−2), high volumetric energy density (≈1 mWh cm−3), and high volumetric power density (≈2 W cm−3). The versatility of lignin laser lithography opens up the opportunity in applications such as on‐chip microsupercapacitors, sensors, and flexible electronics at large‐scale production.

Aqueous zinc-ion batteries and capacitors are potentially competitive grid-scale energy storage devices because of their great features such as safety, environmental friendliness, and low cost. Herein, a completely new phenanthroline covalent organic framework (PA-COF) was synthesized and introduced in zinc-ion supercapatteries (ZISs) for the first time. Our as-synthesized PA-COF shows a high capacity of 247 mAh g −1 at a current density of 0.1 A g −1 , with only 0.38% capacity decay per cycle during 10 000 cycles at a current density of 1.0 A g −1 . Although covalent organic frameworks (COFs) are attracting great attention in many fields, our PA-COF has been synthesized using a new strategy involving the condensation reaction of hexaketocyclohexanone and 2,3,7,8-phenazinetetramine. Detailed mechanistic investigations, through experimental and theoretical methods, reveal that the phenanthroline functional groups in PA-COF are the active zinc ion storage sites. Furthermore, we provide evidence for the cointercalation of Zn 2+ (60%) and H + (40%) into PA-COF using inductively coupled plasma atomic emission spectroscopy and deuterium solid-state nuclear magnetic resonance (NMR). We believe that this study opens a new avenue for COF material design for zinc-ion storage in aqueous ZISs.

The application of graphite anodes in potassium-ion batteries (KIB) is limited by the large variation in lattice volume and the low diffusion coefficient of potassium ions during (de)potassiation. This study demonstrates nitrogendoped, defect-rich graphitic nanocarbons (GNCs) as high-performance KIB anodes. The GNCs with controllable defect densities are synthesized by annealing an ethylenediaminetetraacetic acid nickel coordination compound. The GNCs show better performance than the previously reported thin-walled graphitic carbonaceous materials such as carbon nanocages and nanotubes. In particular, the GNC prepared at 600 °C shows a stabilized capacity of 280 mAh g −1 at 50 mA g −1 , robust rate capability, and long cycling life due to its high-nitrogen-doping, short-range-ordered, defect-rich graphitic structure. A high capacity of 189 mAh g −1 with a long cycle life over 200 cycles is demonstrated at a current density of 200 mA g −1 . Further, it is confirmed that the potassium ion storage mechanism of GNCs is different from that of graphite using multiple characterization methods. Specifically, the GNCs with numerous defects provide more active sites for the potassiation process, which results in a final discharge product with short-range order. This study opens a new pathway for designing graphitic carbonaceous materials for KIB anodes.

Lignin-derived hierarchical porous carbon (LHPC) was prepared through a facile template-free method. Solidification of the lignin-KOH solution resulted in KOH crystalizing within lignin. The crystalized KOH particles in solid lignin acted both as template and activating agent in the heat-treatment process. The obtained LHPC, exhibiting a 3D network, consisted of macroporous cores, mesoporous channels, and micropores. The LHPC comprised 12.27 at % oxygen-containing groups, which resulted in pseudocapacitance. The LHPC displayed a capacitance of 165.0 F g(-1) in 1 M H2 SO4 at 0.05 A g(-1) , and the capacitance was still 123.5 F g(-1) even at 10 A g(-1) . The LHPC also displayed excellent cycling stability with capacitance retention of 97.3 % after 5000 galvanostatic charge-discharge cycles. On account of the facile preparation of LHPC, this paper offers a facile alternative method for the preparation of hierarchical porous carbon for electrochemical energy storage devices.

High power K + ion capacitors have great potential in various large-scale applications because of the cost advantages and the low redox potential of K/K + . However, the large ionic radius of potassium brings huge challenges for the development of suitable electrode materials.Here we demonstrate a general strategy for preparing porous MXene electrodes that can significantly enhance K + storage performance. Using V2C MXene as a model system, we show that the K + ion storage capacity can be greatly boosted by a simple sequential acid/alkali treatment.The resulting product, K-V2C, not only delivers a capacity of 195 mAh g -1 (in contrast to 98 mAh g -1 of pristine V2C) at 50 mA g -1 , but also good rate performance. The charge storage mechanism was carefully studied and is shown to involve a solvent co-intercalation process. In addition, full cells were fabricated by coupling the K-V2C anode and Prussian blue analogous (KxMnFe(CN)6) cathode, which can work at a high average operating voltage of ~3.3 V within a wide range (0.01 V to 4.6 V). Moreover, the devices can achieve a high energy density of 145 Wh kg −1 at a power density of 112.6 W kg −1 , suggesting that K-V2C, and other porous MXenes prepared by our approach, are promising electrodes in mobile ion capacitors.

Conductive 2D metal–organic frameworks (MOFs) have merits beyond traditional MOFs for electrochemical applications, but reports on using MOFs as electrodes for electrochemical microsupercapacitors (MSCs) are practically non‐existent. In this work, a Ni‐catecholate‐based MOF (Ni‐CAT MOF) having good conductivity and exhibiting redox chemistry in the positive and negative voltage windows is developed. A novel process is developed to selectively grow the conductive Ni‐CAT MOF on 3D laser scribed graphene (LSG). The LSG with its superior wettability serves as a functional matrix‐current collector for the hybridization of conductive Ni‐CAT MOF nanocrystals. Impressively, MSCs fabricated using the hybrid LSG/Ni‐CAT MOF show significant improvement compared with MOF‐free LSG electrodes. Specifically, the LSG/Ni‐CAT MOF electrodes can deliver MSCs with a wide operating voltage (1.4 V), high areal capacitance (15.2 mF cm−2), energy density (4.1 µWh cm−2), power density (7 mW cm−2), good rate performance, and decent cycling stability. This work opens up an avenue for developing electrochemical microsupercapacitors using conductive MOF electrodes.