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[Display omitted] • Mg-Co-Ni LDH were homogenously grown on the surface of reduced graphene (Mg-Co-Ni LDH/rG- x). • The Mg-Co-Ni LDH/rG- x was fabricated by a novel ball milling combined ion-exchange method. • The present ball milling combined ion-exchange method is versatile and does not needs extra alkali sources or auxiliary assembly reagents. • The Mg-Co-Ni LDH/rG- x based asymmetric supercapacitor achieve high energy density and superlong cycling stability. As an electrode for energy storage, the inherently poor conductivity of metal hydroxides (MHs) can be improved by in situ growth of MHs on conductive carbon based substrates so that their performances on energy storage could be enhanced to a high level. However, the incompatibility of hydrophilic component (metal hydroxides) and hydrophobic counterpart (carbon based materials) makes it difficult to be accomplished. Herein, we presented a scalable and easy-operated strategy by ball-milling combined with ion-exchange technique to grow Mg-Co-Ni LDH (layered double hydroxides) on reduced graphene, in which ball-milling was utilized to disperse the staring material of magnesium acetate on graphene oxide (GO) to obtain the composite of Mg(Ac) 2 /GO. The composite can be in situ transformed to MgO/reduced grapheme (rG) by following heat treatment. While, the ion-exchange reaction could enables the in situ growth of Mg-Co-Ni LDHs on the reduced graphene. The derived products (denoted as Mg-Co-Ni LDH/rG- x) owns nanosheet morphology, surface area of 59–115 m2/g, homogenous elements distribution. As electrode for supercapacitor, the maximum capacitance of 1204F/g@1.0 A/g was achieved and the corresponding asymmetric supercapacitor device shows a large energy density of 44.3 Wh/kg@800 W/kg. Particularly, a superlong cycling stability with 90.5% capacitance retention of the first cycle was attained after continuous charge/discharge for 20 000 cycles at current density of 5.0 A/g, promising great potential for practical energy storage application. The present strategy is simple and scalable that can be widely applied to the synthesis of various hydroxides/oxides or multi-component hydroxides/oxides on carbon substrates forming a composite structure, thus offers a great potential for broad application areas including catalysis, adsorption, energy storage, etc. [ABSTRACT FROM AUTHOR]

[Display omitted] • Electrochemically active Oxygen doped carbon (O-PCNs) was fabricated by superbase templated method. • The template basicity on the functionalities and the supercapacitor performances of the derived O-PCNs were disclosed. • The O-PCN-20 is rich in porosity, large in surface area (930 m2/g) and high in active oxygen content (11.4 atom%). • · The O-PCN-20 electrode exhibits large capacitance of 375 F/g@1.0 A/g and energy density of 25.7 Wh/kg@900 W/kg. Templating techniques have been widely adopted for the synthesis of porous carbons, such as oxygen-doped porous carbon nanosheets (O-PCNs), but the effect of the surface characteristics of templates on the surface functionality and performance of a derived carbon has not been well studied. Herein, a series of laboratory-made superbases of K/Mg(OH) 2 with different K/Mg ratios were employed as template to fabricate nanocarbon materials. The aim is to find out how the strength of template basicity could influence the surface functionalities and the supercapacitor performances of the derived O-PCNs. The resulting materials are rich in conjugated hydroxyl and carbonyl groups that are electrochemically active owing to the protection of the conjugated hydroxyl group by KOH and the dehydrogenation step catalyzed by magnesium oxide. Systematic investigations revealed that with the increase of basic strength, the content of the derived electrochemically active oxygen species in the forms of conjugated carbonyl (C O) and hydroxyl (C OH) first increases from 8.4 atom% to 11.4 atom% then decreases to 9.25 atom%. Moreover, the microporosity of the O-PCNs stepwise increases with the rise of KOH loading, ascribable to the effect of KOH etching on the carbon skeleton. The O-PCN-20 templated by 20 % K/Mg(OH) 2 is rich in porosity, large in surface area (930 m2/g) and high in active oxygen content (11.4 atom%). With high active surface area and extra Faradaic capacitance, O-PCN-20 exhibited superior supercapacitor performances including large specific capacitance of 375 F/g@1.0 A/g, high rate capability of 81.1 % (from 1.0 A/g to 20 A/g), energy density of 25.7 Wh/kg@900 W/kg and excellent cycling stability with near 100 % capacitance retentions after 10 000 cycles and more than 86.2 % capacitance retention over 20 000 cycles at large current density of 10 A/g, indicating O-PCN-20 has potential to be used as electrode material for energy storage devices. [ABSTRACT FROM AUTHOR]

[Display omitted] • Solvent-free strategy was developed to synthesize porous carbon (MIC x) doped with rich Faradaic active oxygen (5.8–8.2 atom%). • The resultant MICx owns surface area of 326–427 m2/g and large packing density of 1.12–1.28 g/cm3. • The MICx based electrode achieves superior supercapacitor performances with both high gravimetric and volumetric performances. In the selection of carbon-based electrode materials for supercapacitive energy storage, it is hard to get one that is high in both gravimetric and volumetric performance because there is a trade-off between them. In the presented work, microporous carbon materials denoted herein as MIC x were synthesized through catechol polymerization in the presence of molten FeCl 3. As complexing agent, the iron species coordinate with catechol oligomers, functioning as template as well as catalyst in the synthesis of the microporous carbon. The in situ formation of micropores and carbonaceous skeleton is induced by the carbonyl/hydroxyl redox pairs upon catalytic graphitization during carbonization. The derived nanocarbons have high microporosity (70.6 %–79.2 %) and rich oxygenate functionalities (carbonyl: 3.3–4.0 atom% and hydroxyl: 2.5–4.2 atom%). The FeC x materials are high in faradaic activity. For example, the FeC873-based electrode displays excellent supercapacitor performances: capacitance of 440F/g@1.0 A/g (equivalent to 537F/cm3@1.0 A/g) and 289F/g@20 A/g (equivalent to 353F/cm3@20 A/g), large energy density of 25.5 Wh/kg@900 W/kg (equivalent to 31.1 Wh/L@1098 W/L), and good cycling stability (ca.100 % capacitance retention after 20 000 continual charge/discharge cycles). [ABSTRACT FROM AUTHOR]

[Display omitted] • Expired coffee derived carbons (HCDC) achieves high packing density of 1.81–1.83 cm3/g. • The derived HCDC owns rich nitrogen (4.5 atom%) and oxygenic (12.0 atom%) functionalities. • The HCDC electrode achieves high gravimetric and volumetric capacitance of 312F/g and 567F/cm3. • The HCDC electrode exhibits a high volumetric energy density of 27.8 Wh/L@1820 W/L. Clean production of activated carbon from household expired food provide an alternative way to get value-added product thus benefits waste reutilization and environmental protection. Herein, we fabricated N, O co-doped activated carbons (HCDC) from expired coffee to by a green route of direct water vapor carbonization/activation approach. In our approach, the expired coffee was firstly grinded and then carbonized under water vapor atmosphere. The derived HCDC owns low surface area (172–184 m2/g), large packing density (1.81–1.83 cm3/g), rich redox-active nitrogen (4.5 atom%) and oxygenic (12.0 atom%) functionalities. As electrode for supercapacitor, the HCDC achieves a high gravimetric capacitance of 312F/g at 1.0 A/g (vs 258F/g of commercial AC) and the value can be maintained 223F/g at 20 A/g, showing a high rate capability of 71.5%. Particularly, because of the large packing density, the HCDC exhibits an excellent volumetric supercapacitor performances: ultrahigh volumetric capacitance of 567F/cm3 (vs 165F/cm3 of commercial AC) and large energy density of 27.8 Wh/L@1820 W/L (vs 7.5 Wh/L@576 W/L for commercial AC) and superlong cycling stability with near 100 capacitance retention after continual 30 000 cycles at large current density of 9.0 A/g, suggesting a promising application for practical energy storage devices. [ABSTRACT FROM AUTHOR]

[Display omitted] • An all-solid-state (ASS) strategy without using any solvents and activators was developed. • The ASS strategy derived carbon owns abundant nitrogen species and large packing density. • The resultant product show superior supercapacitor performances with both high gravimetric and volumetric performances. Template synthesis of porous carbon with rich functionalities by a scalable strategy without using any solvents and activators will be a green and promising route. Herein, we reported an all-solid-state synthesis strategy by mixing glucose and graphitic carbon nitride (g -C 3 N 4) by milling and then undergoing a segmented carbonization in which first at low temperature of 573 K to polymerize sucrose onto g -C 3 N 4 , then at high temperature of 973 K to carbonized the composite to obtain a porous carbon (denoted as GNC) with abundant nitrogen species over 20 atom% and large packing density (0.91–1.25 g cm−3). Due to the features of large packing density and rich electrochemically-active N species, as electrode for supercapacitive energy storage, the developed GNC exhibit a comparable energy storage level with both high gravimetric energy density of 26.8 Wh kg−1@1000 W kg−1 and volumetric energy density of 30.8 Wh L−1@1150 W L−1, suggesting a potentiality in energy storage field. Importantly, the present strategy owns characteristics of ease of operation, green and scalable, which would be a promising synthesis route towards the fabrication of functional carbon utilizing in many fields like sorption & separation, catalysis, energy storage and so on. [ABSTRACT FROM AUTHOR]

As an industrial material for supercapacitive energy storage, commercial activated carbons (AC) could achieve a satisfactory gravimetric performances by electric double layered capacitance (EDLC) due to their rich microporosity, but the volumetric performances are usually poor resulted from the low packing density. Herein, we presented a strategy to address this tradeoff relationship and to achieve both high gravimetric and volumetric performance by filling the macro/mesoporosity with extra nitrogen doped carbon. The reconstructed activated carbon could inherit most of microporosity from the parent AC, while the macro/mesoporosity of them was greatly decreased, resulting in increase of packing density and the improvement of surface hydrophilicity. Benefited from the increase of packing density and maintenance of microporosity, the resultant activated carbon achieves greatly enhanced energy storage level including three times higher capacitance of 384 F cm−3@ 1.0 A/g (vs 128 F cm−3@ 1.0 A/g for pristine AC), high rate capability of 73.4% (vs 59.2% for pristine AC), larger energy density of 27.5 Wh L−1@ 900 W L−1 (vs 10.0 Wh L−1@747 W L−1). Importantly, the present strategy provides a facile and unique method to process activated carbon, which offers a possibility improving the energy storage level of the commercial activated carbon. [Display omitted] • Commercial activated carbon (AC) was processed by filling the macro/mesoporosity. • The filled AC owns increased packing density and more nitrogen functionalities. • The filled AC achieves greatly enhanced supercapacitor performances. [ABSTRACT FROM AUTHOR]