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Developing efficient bifunctional electrocatalysts toward oxygen/hydrogen evolution reactions is crucial for electrochemical water splitting toward hydrogen production. The high‐performance electrocatalysts depend on the catalytically active and highly accessible reaction sites and their structural robustness, while the rational design of such electrocatalysts with desired features avoiding tedious manufacture is still challenging. Here, a facile method is reported to synthesize mesoporous and heterostructured transition metal oxides strongly anchored on a nickel skeleton (MH‐TMO) containing identified Fe–Cu oxide interfaces with high intrinsic activity, easy accessibility for reaction intermediates, and long‐term stability for alkaline oxygen/hydrogen evolution reactions. The MH‐TMO with the electrocatalytically active Fe–O–Cu bridge has an optimal oxygen binding energy to facilitate adsorption/desorption of oxygen intermediates for oxygen molecules. Associated with the high mass transport through the nanoporous structure, MH‐TMO exhibits impressive oxygen evolution reaction catalysis, with an extremely low overpotential of around 0.22 V at 10 mA cm−2 and low Tafel slope (44.5 mV dec−1) in 1.0 M KOH, realizing a current density of 100 mA cm−2 with an overpotential as low as 0.26 V. As a result, the alkaline electrolyzer assembled by the bifunctional MH‐TMO catalysts operates with an outstanding overall water‐splitting output (1.49 V@10 mA cm−2), outperforming one assembled with noble‐metal‐based catalysts. [ABSTRACT FROM AUTHOR]

In high demand is developing trifunctional electrocatalysts to simultaneously drive hydrogen evolution reaction (HER) and oxygen evolution/reduction reaction (OER/ORR) for metal-air batteries and water splitting. Here we develop the carbon nanotubes (CNTs)-grafted FeC/MnO 2 nanocomposite catalyst by carbonizing FeMn metal-organic frameworks. The synergistic effect between FeC and MnO 2 dominantly contributes the ORR, OER, and HER. The transition metal-mediated growth of CNTs by an in-situ catalysis mechanism enables high electrical conductivity, abundant active sites, as well as efficient reaction pathways. The optimized chemical composite and unique hierarchical structure endow the FeC/MnO 2 with low overpotentials for multiply electrochemical reactions. Consequently, the composite catalyst successfully serves as the bifunctional electrode for water splitting with a voltage of 1.66 V at 10 mA cm−2 as well as the cathode for all-solid-state metal-air battery with Pt/C-comparable performance. The advanced transition metal composite presented in this work provides the guidance for rationally developing trifunctional electrocatalysts for efficient integrated energy conversion systems. FeC/MnO 2 , as an advanced trifunctional catalyst that can be used for water splitting and metal-air batteries, benefits from strong synergy, abundant active sites and efficient electron transfer rate. [Display omitted] • FeC/MnO 2 is electrocatalytically active and stable for OER, ORR and HER. • The porous structure provides abundant active sites and proton transfer channels. • The combination of CNTs and FeC/MnO 2 increases the electron transfer rate. • The internal synergy of FeC/MnO 2 plays a major role in electrocatalytic activity. [ABSTRACT FROM AUTHOR]

Synthesis of highly efficient, non-noble and bi-functional electrocatalysts is exceedingly challenging and necessary for water splitting devices. In this work, three-dimensional spherical Ni(OH) 2 /NiCo 2 O 4 heterojunctions are prepared by a one-step hydrothermal method and the hybrids are explored as efficient electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in an alkaline electrolyte via tuning different Ni/Co atomic ratios of heterojunctions. The optimized Ni(OH) 2 /NiCo 2 O 4 (S (1:1)) exhibits high electrocatalytic activity with an ultralow over-potential of 189 mV at 10 mA cm−2 for the HER. With regard to the OER, the over-potential of the as-synthesized S (1:1) heterojunction is only 224 mV at the current density of 10 mA cm−2. The improved catalytic performance of the Ni(OH) 2 /NiCo 2 O 4 heterojunctions is attributed to the chemical synergic combining of Ni(OH) 2 and NiCo 2 O 4 , large specific surface area for exposing more accessible active sites, and heterointerface for activating the intermediates that facilitates electron/electrolyte transport. The prepared catalyst exhibits good durability and stability in HER and OER catalyzing conditions. This study provides a feasible approach for the building of highly efficient bifunctional water splitting electrocatalysts and stimulates the development of renewable energy conversion and storage devices. • The three-dimensional spherical Ni(OH) 2 /NiCo 2 O 4 heterojunctions were constructed. • The heterostructure would improve electrocatalytic performance. • The optimized catalyst exhibits remarkable catalytic activity for water splitting. • The S (1:1) heterojunction exhibits an overpotential of 224 mV for OER and 189 mV for HER. [ABSTRACT FROM AUTHOR]

Developing of inexpensive, high-efficient, and earth-abundant bifunctional catalysts for water splitting is of great significance for green and sustainable energy development. Herein, a bifunctional hybrid electrocatalyst of Ni 3 ZnC 0.7 nanodots in-situ grown on nitrogen-doped carbon nanotube (Ni 3 ZnC 0.7 /NCNT) arrays is synthesized by a one-step template strategy with 1, 3, 5-triamino-2, 4, 6-trinitrobenzene serving as carbon/nitrogen sources, ZnO nanorods as template and zinc source, and nickel foam as substrate and nickel source. Benefiting from the introduction of Ni 3 ZnC 0.7 nanodots and nitrogen doping to the carbon nanotubes, the Ni 3 ZnC 0.7 /NCNT-700 arrays exhibit superior hydrogen evolution reaction and oxygen evolution reaction catalytic activity in terms of low overpotential (203 mV and 380 mV vs RHE at 10 mA cm−2 for hydrogen evolution reaction and oxygen evolution reaction, respectively). When the Ni 3 ZnC 0.7 /NCNT-700 is served as both anode and cathode catalysts for overall water splitting, a potential of 1.66 V is needed to deliver a current density of 10 mA cm−2, and it also displays negligible degradation after 24 h of operation in alkaline solution. The present work not only provides an efficient bifunctional electrocatalyst for overall water splitting, but also offers a new strategy to design and synthetize the bimetallic carbide. Image 1 [ABSTRACT FROM AUTHOR]