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Highly effective catalysts are of great importance for artificial nitrogen fixation. Inspired by the natural nitrogenase, we biomimetically designed an inorganic catalyst, Mo(IV)-doped FeS2, for el...

Hydrogen evolution reaction (HER) is an essential step in converting renewable energy to clean hydrogen fuel. Exploring highly efficient, stable and cost-effective electrocatalysts is of crucial significance for sustainable HER. Here, we report the design of a coupled ruthenium/cobalt oxide (Ru/CoO) hybrid electrocatalyst for alkaline HER. In this hybrid metal/oxide system, the complicated alkaline HER pathways are overall facilitated; oxygen (O)-vacancy-abundant oxide enhances water splitting and Ru promotes successive hydrogen intermediates to generate hydrogen. The resulting Ru/CoO hybrid electrocatalyst exhibits significantly promoted catalytic activity compared with benchmark Ru catalyst, displaying an overpotential of 55 mV to generate a HER current density of 10 mA cm−2, comparable with the state-of-the-art Pt/C catalyst and the most efficient alkaline HER electrocatalysts. Furthermore, the strong interaction of Ru nanoparticles with oxide support and the in-situ growth of oxide support on conductive substrate guarantee the long-term stability of as-fabricated Ru/CoO hybrid electrocatalyst. This newly designed hybrid catalyst with abundant metal/oxide interfaces may pave a new pathway for exploring efficient and stable HER electrocatalysts.

Driven by the intensified demand for energy storage systems with high-energy density and safety, all-solid-state zinc (Zn) air batteries have drawn extensive attentions. However, the development of non-precious metals with high catalytic activity as the air electrode is still a big challenge. In this work, we realize the large-scale fabrication of single-crystal CoO nanorods with high active facets and abundant oxygen vacancies in-situ on conductive substrate, which exhibits superior electrocatalytic activity in both oxygen reduction reaction and oxygen evolution reaction. The all-solid-state Zn-air batteries assembled with such free-standing CoO NRs show low charge/discharge overpotentials, a high energy density and a high cyclic stability. Our work indicates that the rational structure design of catalysts can pave a new route to next generation efficient and durable electrochemical devices.

Cost-effective carbon-based catalysts are promising for catalyzing the electrochemical N2 reduction reaction (NRR). However, the activity origin of carbon-based catalysts towards NRR remains unclear, and regularities and rules for the rational design of carbon-based NRR electrocatalysts are still lacking. Based on a combination of theoretical calculations and experimental observations, chalcogen/oxygen group element (O, S, Se, Te) doped carbon materials were systematically evaluated as potential NRR catalysts. Heteroatom-doping-induced charge accumulation facilitates N2 adsorption on carbon atoms and spin polarization boosts the potential-determining step of the first protonation to form *NNH. Te-doped and Se-doped C catalysts exhibited high intrinsic NRR activity that is superior to most metal-based catalysts. Establishing the correlation between the electronic structure and NRR performance for carbon-based materials paves the pathway for their NRR application.

Zinc-air batteries offer a possible solution for large-scale energy storage due to their superhigh theoretical energy density, reliable safety, low cost, and long durability. However, their widespread application is hindered by low power density. Herein, a multiscale structural engineering of Ni-doped CoO nanosheets (NSs) for zinc-air batteries with superior high power density/energy density and durability is reported for the first time. In micro- and nanoscale, robust 2D architecture together with numerous nanopores inside the nanosheets provides an advantageous micro/nanostructured surface for O2 diffusion and a high electrocatalytic active surface area. In atomic scale, Ni doping significantly enhances the intrinsic oxygen reduction reaction activity per active site. As a result of controlled multiscale structure, the primary zinc-air battery with engineered Ni-doped CoO NSs electrode shows excellent performance with a record-high discharge peak power density of 377 mW cm-2 , and works stable for >400 h at 5 mA cm-2 . Rechargeable zinc-air battery based on Ni-doped CoO NSs affords an unprecedented small charge-discharge voltage of 0.63 V, outperforming state-of-the-art Pt/C catalyst-based device. Moreover, it is shown that Ni-doped CoO NSs assembled into all-solid-state coin cells can power 17 light-emitting diodes and charge an iPhone 7 mobile phone.