Hierarchical porous Fe/N/S-doped carbon with a high content of graphitic nitrogen (FeNS/HPC) has been successfully synthesized by a facile dual-template method. FeNS/HPC shows not only macropores resulting from the dissolution of the SiO template, but abundant mesopores were also obtained after removing the in situ generated FeO nanoparticles on the ultrathin (∼4 nm) carbon shell of the macropores. Moreover, micropores are produced during the thermal pyrolysis of the carbon precursors. With respect to the electrochemical performance in the oxygen reduction reaction (ORR), FeNS/HPC not only exceeds other prepared porous carbon materials completely but also shows higher onset potential (0.97 vs 0.93 V), half-wave potentials (0.87 vs 0.83 V), and diffusion current density (5.5 vs 5.3 mA cm) than those of Pt/C. Furthermore, FeNS/HPC also exhibits outstanding stability and methanol tolerance, making it a competent candidate for ORR. The following aspects contribute to its excellent ORR performance. (1) High content of graphitic N (5.1%) and codoping of pyridinic N species, thiophene-S, FeN, and graphitic carbon-encapsulated iron nanoparticles, providing highly active sites. (2) The hierarchical porous mesh structure with micro-, meso-, and macroporosity, accelerating the mass transfer and facilitating full utilization of the active sites. (3) The high specific surface area (1148 m g) of the graphitic carbon shell, assuring a large interface and rapid electron conduction for ORR.

3D self-supported hierarchical Ni@NCNT/NiMoN shows remarkable activity, durability and anti-oxidation ability as the promising HER&OER electrode for storing electricity.

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Sodium borohydride is a promising candidate as hydrogen storage material. The direct borohydride fuel cell (DBFC) as an energy conversation device has attracted intensive attention owing to the low theoretical potential of borohydride oxidation reaction (BOR, −1.24 V vs SHE) on the anode. In this paper, the hierarchical sea urchin-like NiMoN@NC coated by thin carbon layer with optimal BH 4 − adsorption characteristic was synthesized as a superior electrocatalyst toward BOR. In 1 M NaOH-0.05 M NaBH 4 , the BOR working potentials are only −55 and 44 mV at the current densities of 10 and 200 mA cm −2 on NiMoN@NC, respectively. Furthermore, the membrane-free DBFC using NiMoN@NC as anodic electrocatalyst shows a maximum power density of 67 mW cm −2 at room temperature with appreciative stability. This well-designed carbon coated and nitrogen doped transitionmetal material with hierarchical nano/microstructure as a highly efficient electrocatalyst shows promising potential and bright prospects in electrocatalysis research and practical application for energy conversion systems of DBFC.

The pedestal of the rechargeable zinc–air battery (ZAB) is based on high‐performance bifunctional oxygen reduction/evolution reactions (ORR/OER) electrocatalysts. Herein, without any template or surfactant, in situ grown nitrogen‐doped carbon‐nanotube (NCNT)‐embedded with two phases of bimetal CoFe alloys and CoFe2O4 spinel oxide are constructed, using inexpensive materials of glucose, urea, and cobalt/iron acetates by programing the pyrolysis temperature. The obtained catalyst with optimal cobalt/iron acetates mass ratio (1:1) denoted as CoFe–CoFe2O4–NCNT not only exceeds Pt–Ru/C in terms of ORR half‐wave potentials [(0.88 vs 0.84 V versus reversible hydrogen electrode (RHE)] and limiting current densities (6.40 vs 5.40 mA cm−2), but also manifests superior OER activity with the potentials of (1.58 vs 1.67 V versus RHE) at 10 mA cm−2. Therefore, CoFe–CoFe2O4–NCNT exhibits a smaller ΔE value of (0.70 V versus RHE), surpassing that of Pt–Ru/C (0.85 V versus RHE) and shows excellent stability as well as outstanding methanol tolerance compared with the Pt–Ru/C commercial catalyst. In addition, CoFe–CoFe2O4–NCNT applied as a bifunctional air electrode in rechargeable ZAB displays a promising rechargeability performance with high‐discharge and low‐charge potentials and a relatively stable potential gap under 550 cycles, outperforming those of Pt–Ru/C.

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