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Electrosynthesis of H2O2 has great potential for directly converting O2 into disinfectant, yet it is still a big challenge to develop effective electrocatalysts for medical‐level H2O2 production. Herein, we report the design and fabrication of electrocatalysts with biomimetic active centers, consisting of single atomic iron asymmetrically coordinated with both nitrogen and sulfur, dispersed on hierarchically porous carbon (FeSA‐NS/C). The newly‐developed FeSA‐NS/C catalyst exhibited a high catalytic activity and selectivity for oxygen reduction to produce H2O2 at a high current of 100 mA cm−2 with a record high H2O2 selectivity of 90 %. An accumulated H2O2 concentration of 5.8 wt.% is obtained for the electrocatalysis process, which is sufficient for medical disinfection. Combined theoretical calculations and experimental characterizations verified the rationally‐designed catalytic active center with the atomic Fe site stabilized by three‐coordinated nitrogen atoms and one‐sulfur atom (Fe‐N3S‐C). It was further found that the replacement of one N atom with S atom in the classical Fe‐N4‐C active center could induce an asymmetric charge distribution over N atoms surrounding the Fe reactive center to accelerate proton spillover for a rapid formation of the OOH* intermediate, thus speeding up the whole reaction kinetics of oxygen reduction for H2O2 electrosynthesis. [ABSTRACT FROM AUTHOR]

Optimized electrocatalyst that hybrids with carbon coating FeCoP x nanoparticles possesses catalytic activity toward ORR, OER and HER. Furthermore, through the design of alkali-acid electrolyzer and device integration, for the very first time, a single Zinc-air battery enable to drive an alkali-acid electrolyzer for producing hydrogen and oxygen. [Display omitted] • A one-pot scalable pyrolysis strategy to fabricate a tri-functional electrocatalyst. • High catalytic activity toward ORR&OER in alkaline and HER in acidic media. • The Zn-air battery can run stably for 1500 cycles. • An alkali-acid electrolyzer only requires 0.99 V to release an electrolysis current density of 10 mA cm−2. • A single self-made Zinc-air battery can drive an alkali-acid electrolyzer to produce hydrogen. Developing handy synthesis routes to fabricate low-cost, high-activity, and multifunctional electrocatalysts for a variety of electrochemical reactions is highly desirable so as to achieve the goal that one catalyst can be used for integrated electrolysis devices, thus greatly simplifying the electrocatalyst system processing. Here, we report a one-pot scalable pyrolysis strategy to fabricate a tri-functional electrocatalyst, i.e. , hybrids with carbon coating FeCoP x nanoparticles, which shows favorable electrocatalytic properties toward oxygen reduction reaction, oxygen evolution reaction in alkaline solution, and hydrogen evolution reaction in acidic condition. The new synthesis routes enable us to readily develop an integrated device with a Zn-air battery driving an alkali-acid electrolyzer by just using one catalyst. The present work may shed light on the practical viability of the development of multifunctional electrocatalysts for integrated devices applications. [ABSTRACT FROM AUTHOR]

Highly electrocatalytic activity and strong stability towards both oxygen evolution (OER) and oxygen reduction reaction (ORR) have been regarded as the critical factors in widespread application for the renewable energy technologies. It still remains a huge challenge for developing bifunctional catalysts with low cost, efficiently electrocatalytic activity and strong stability. In this paper, FeCo alloy nanoparticles embedded in nitrogen-doped carbon are synthesized through a simple thermal decomposition of Co-Fe Prussian Blue Analogue (Co-Fe PBA) in Ar atmosphere, during which the organic ligand of CN − in Co-Fe PBA provides both carbon and nitrogen sources for forming nitrogen-doped carbon and FeCo alloy nanoparticles were formed, and thus producing a core-shell structure (FeCo@NC). According to a set of electrochemical tests, the obtained FeCo@NC can function as a Janus to drive OER and ORR with desirable activities and stabilities in alkaline media. Specifically, the FeCo@NC presents an onset-potential of 1.45 V, a potential of 1.49 V at 10 mA cm −2 , a Tafel slope of 62 mV dec −1 as OER catalyst, and an onset potential of 0.94 V, a half-wave potential of 0.8 V as ORR catalyst. The performance is comparable to those of precious metal based electrocatalysts, making it possible for potential application in the renewable energy devices, especially Zn-air battery. [ABSTRACT FROM AUTHOR]

It presents the scalable salt-templated synthesis of two-dimensional porous fluorine-doped carbon (FC) nanosheets with the high active sites and larger special surface area, which shows impressive oxygen reduction reaction (ORR) activities. The synergistic effect of fluoride doping and defects provided more density of active sites in carbon material. It may open up a promising avenue for developing electrocatalysts with high catalytic activity and high stability for electrolyzed application. • Two-dimensional porous fluorine-doped carbon (FC) nanosheets. • Long-term durability and the large active surface area. • Remarkably enhanced oxygen electrocatalytic performance. We present the scalable salt-templated synthesis of two-dimensional porous fluorine-doped carbon (FC) nanosheets. Due to the larger special surface area (1031 m2 g−1) and high active sites, FC-900 (pyrolyzed at 900 °C) shows impressive oxygen reduction reaction (ORR). The synergistic effect of fluoride doping and defects provides richer density of active sites in these nanosheets. When the samples are further calcined at 900 °C for different hours, the ORR activity of the resulting samples shows a little improvement, indicating the influence of the defects on the ORR performance is much inferior to the doped fluorine. The formation of FC structures is beneficial to the ORR activity, and supported by First-principles density functional theory. The results reveal F dopants and defects important role in efficient ORR electrocatalysis owing to the synergistic effect, which is important for comprehending the origin of ORR, and it is also strong evidence to search advanced carbon-based catalysts. [ABSTRACT FROM AUTHOR]