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Transition metal single atoms anchored on nitrogen‐doped carbon (M‐N‐C) matrix with M‐N‐C active sites have shown to be promising catalysts for both hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). Herein, a hybrid catalyst with low‐level loading of atomic Pt and Co species encapsulated in nitrogen‐doped graphene (Pt@CoN4‐G) is developed. The Pt@CoN4‐G shows low overpotential for HER in wide‐pH electrolyte and manifests improved mass activity with almost eight times greater than that of Pt/C at an overpotential of 50 mV. The Pt@CoN4‐G also exhibits a top‐level ORR activity (half‐wave potential, E1/2 = 0.893 V) and robust stability (>200 h) in alkaline medium. Using theoretical calculations and comprehensive characterizations , the strong metal–support interactions between Pt species and CoN4‐G support and synergistical cooperation of multiple active sites are clarified. A flow alkali‐Al/acid hybrid fuel cell using Pt@CoN4‐G as cathode catalyst delivers a large power density of 222 mW cm−2 with excellent stability to achieve simultaneously hydrogen evolution and electricity generation. In addition, Pt@CoN4‐G endows a flow Zn‐air battery with high power density (316 mW cm−2), good stability under large current density (>100 h at 100 mA cm−2), and long cycle life (over 600 h at 5 mA cm−2). [ABSTRACT FROM AUTHOR]

The development of precious‐metal alternative electrocatalysts for oxygen reduction reaction (ORR) is highly desired for a variety of fuel cells, and single atom catalysts (SACs) have been envisaged to be the promising choice. However, there remains challenges in the synthesis of high metal loading SACs (>5 wt.%), thus limiting their electrocatalytic performance. Herein, a facile self‐sacrificing template strategy is developed for fabricating Co single atoms along with Co atomic clusters co‐anchored on porous‐rich nitrogen‐doped graphene (Co SAs/AC@NG), which is implemented by the pyrolysis of dicyandiamide with the formation of layered g‐C3N4 as sacrificed templates, providing rich anchoring sites to achieve high Co loading up to 14.0 wt.% in Co SAs/AC@NG. Experiments combined with density functional theory calculations reveal that the co‐existence of Co single atoms and clusters with underlying nitrogen doped carbon in the optimized Co40SAs/AC@NG synergistically contributes to the enhanced electrocatalysis for ORR, which outperforms the state‐of‐the‐art Pt/C catalysts with presenting a high half‐wave potential (E1/2 = 0.890 V) and robust long‐term stability. Moreover, the Co40SAs/AC@NG presents excellent performance in Zn–air battery with a high‐peak power density (221 mW cm−2) and strong cycling stability, demonstrating great potential for energy storage applications. [ABSTRACT FROM AUTHOR]

Developing high-active, good-stable, and cost-effective electrocatalyst for oxygen reduction reaction (ORR) in all-pH medium is highly desired for the application of various fuel cell systems. Here, a network architecture hybrid with porous nitrogen-doped graphene encapsulated β-FeOOH nanoparticals (β-FeOOH/PNGNs) as ORR electrocatalyst, which exhibits remarkable enhancement ORR performance in terms of activity and stability in pHuniversal medium is reported. Systematic characterization combining with X-ray absorption fine structure analysis and the first principles simulations reveal that the as-formed surface FeO6 active sites that induced by a mass of Fe vacancies in β-FeOOH/PNGNs can significantly lower the thermodynamic barrier of the total reaction, and hence contribute to a remarkable enhancement in ORR activity. [ABSTRACT FROM AUTHOR]

It is of increasing importance to explore new low-cost and high-activity electrocatalysts for oxygen reduction reaction (ORR), which have had a substantial impact across a diverse range of energy conversion system, including various fuel cell and metal-air batteries. Although engineering carbon nanostructures have been widely explored as a candidate class of Pt-based ORR electrocatalysts owing to their proved high activity, outstanding stability, and ease of use, there still remains a daunting challenge to develop high activity metal-free electrocatalysts in pH-universal electrolyte system. Here, a reliable and controllable route amenable to prepare nitrogen-doped porous carbon (NPC) with high yields and exceptional quality is described. The as-prepared NPC shows advantages of high activity, high durability, and methanol-tolerant as an efficient pH-universal electrocatalyst for ORR, showing comparable or even better activity as compared with the commercial Pt/C catalysts not only in alkaline media but also in acidic and neutral electrolyte. Systematic electrochemical studies, combining with density functional theory calculation, demonstrate the unique nitrogen-doping species and favorable pores in the as-designed NPC synergistically contribute to the significantly improved catalytic activity in pH-universal medium. The present work potentially presents an important breakthrough in developing ORR electrocatalysts for various fuel cells. [ABSTRACT FROM AUTHOR]

A novel hybrid electrocatalyst consisting of nitrogen-doped graphene/cobalt-embedded porous carbon polyhedron (N/Co-doped PCP//NRGO) is prepared through simple pyrolysis of graphene oxide-supported cobalt-based zeolitic imidazolate-frameworks. Remarkable features of the porous carbon structure, N/Co-doping effect, introduction of NRGO, and good contact between N/Co-doped PCP and NRGO result in a high catalytic efficiency. The hybrid shows excellent electrocatalytic activities and kinetics for oxygen reduction reaction in basic media, which compares favorably with those of the Pt/C catalyst, together with superior durability, a four-electron pathway, and excellent methanol tolerance. The hybrid also exhibits superior performance for hydrogen evolution reaction, offering a low onset overpotential of 58 mV and a stable current density of 10 mA cm−2 at 229 mV in acid media, as well as good catalytic performance for oxygen evolution reaction (a small overpotential of 1.66 V for 10 mA cm−2 current density). The dual-active-site mechanism originating from synergic effects between N/Co-doped PCP and NRGO is responsible for the excellent performance of the hybrid. This development offers an attractive catalyst material for large-scale fuel cells and water splitting technologies. [ABSTRACT FROM AUTHOR]

On page 872 novel nitrogen‐doped graphene/cobalt‐embedded porous carbon polyhedron hybrid electrocatalyst is obtained by Z. H. Wen, J. H. Chen, and co‐workers through a simple strategy. Benefitting from well defined structural features including excellent porous carbon structure, N/Co‐doping effect, introduction of NRGO, and good contact between N/Co‐doped PCP and NRGO sheets, the hybrid exhibits excellent tri‐functional catalytic activities for ORR, HER, and OER with long‐term stability in both acid and basic media. [ABSTRACT FROM AUTHOR]