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The development of an efficient catalytic electrode toward both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of great significance for overall water splitting associated with the conversion and storage of clean and renewable energy. In this study, carbon paper/carbon tubes/cobalt-sulfide is introduced as an integrated three-dimensional (3D) array electrode for cost-effective and energy-efficient HER and OER in alkaline medium. Impressively, this electrode displays superior performance compared to non-noble metal catalysts reported previously, benefiting from the unique 3D array architecture with increased exposure and accessibility of active sites, improved vectorial electron transport capability, and enhanced release of gaseous products. Such an integrated and versatile electrode makes the overall water splitting proceed in a more direct and smooth manner, reducing the production cost of practical technological devices.

In the development of energy-storage devices, simultaneously achieving high power and large energy capacity at fast rate is still a great challenge. In this paper, the synergistic effect of structure and doping in the graphene is demonstrated for high-performance lithium storage with ulftrafast and long-cycling capabilities. By an in situ constructing strategy, hierarchically porous structure, highly conductive network, and heteroatom doping are ideally combined in one graphene electrode. Compared to pristine graphene, it is found that the degree of improvement with both structure and doping effects is much larger than the sum of that with only structure effect or doping effect. Benefitting from the synergistic effect of structure and doping, the novel electrodes can deliver a high-power density of 116 kW kg(-1) while the energy density remains as high as 322 Wh kg(-1) at 80 A g(-1) (only 10 s to full charge), which provides an electrochemical storage level with the power density of a supercapacitor and the energy density of a battery, bridging the gap between them. Furthermore, the optimized electrodes exhibit long-cycling capability with nearly no capacity loss for 3000 cycles and wide temperature features with high capacities ranging from -20 to 55 °C.

Development of an efficient hydrogen evolution reaction (HER) catalyst composed of earth-abundant elements is scientifically and technologically important for the water splitting associated with the conversion and storage of renewable energy. Herein we report a new class of Co-C-N complex bonded carbon (only 0.22 at% Co) for HER with a self-supported and three-dimensional porous structure that shows an unexpected catalytic activity with low overpotential (212 mV at 100 mA cm(-2)) and long-term stability, better than that of most traditional-metal catalysts. Experimental observations in combination with density functional theory calculations reveal that C and N hybrid coordination optimizes the charge distribution and enhances the electron transfer, which synergistically promotes the proton adsorption and reduction kinetics.

A novel in situ replication and polymerization strategy is developed for the synthesis of Fe-N-doped mesoporous carbon microspheres (Fe-NMCSs). This material benefits from the synergy between the high catalytic activity of Fe-N-C and the fast mass transport of the mesoporous microsphere structure. Compared to commercial Pt/C catalysts, the Fe-NMCSs show a much better electrocatalytic performance in terms of higher catalytic activity, selectivity, and durability for the oxygen reduction reaction.

Ultralong cycle life, high energy, and power density rechargeable lithium‐ion batteries are crucial to the ever‐increasing large‐scale electric energy storage for renewable energy and sustainable road transport. However, the commercial graphite anode cannot perform this challenging task due to its low theoretical capacity and poor rate‐capability performance. Metal oxides hold much higher capacity but still are plagued by low rate capability and serious capacity degradation. Here, a novel strategy is developed to prepare binder‐free and mechanically robust CoO/graphene electrodes, wherein homogenous and full coating of β‐Co(OH)2 nanosheets on graphene, through a novel electrostatic induced spread growth method, plays a key role. The combined advantages of large 2D surface and moderate inflexibility of the as‐obtained β‐Co(OH)2/graphene hybrid enables its easy coating on Cu foil by a simple layer‐by‐layer stacking process. Devices made with these electrodes exhibit high rate capability over a temperature range from 0 to 55 °C and, most importantly, maintain excellent cycle stability up to 5000 cycles even at a high current density.

Triblock copolymer micelles coated with melamine-formaldehyde resin were self-assembled into closely packed two-dimensional (2D) arrangements on the surface of graphene oxide sheets. Carbonizing these structures created a 2D architecture composed of reduced graphene oxide (rGO) sandwiched between two monolayers of sub-40 nm diameter hollow nitrogen-doped carbon nanospheres (N-HCNS). Electrochemical tests showed that these hybrid structures had better performance for oxygen reduction compared to physically mixed rGO and N-HCNS that were not chemically bonded together. Further impregnation of the sandwich structures with iron (Fe) species followed by carbonization yielded Fe-N-HCNS/rGO-900 with a high specific surface area (968.3 m g), a high nitrogen doping (6.5 at%), and uniformly distributed Fe dopant (1.6 wt %). X-ray absorption fine structure analyses showed that most of the Fe in the nitrogen-doped carbon framework is composed of single Fe atoms each coordinated to four N atoms. The best Fe-N-HCNS/rGO-900 catalyst performed better in electrocatalytic oxygen reduction than 20 wt % Pt/C catalyst in alkaline medium, with a more positive half-wave potential of 0.872 V and the same limiting current density. Bottom-up soft-patterning of regular carbon arrays on free-standing 2D surfaces should enable conductive carbon supports that boost the performance of electrocatalytic active sites.

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