Large-scale industrial application of electrolytic splitting of water has called for the development of oxygen evolution electrodes that are inexpensive, robust and can deliver large current density (>500 mA cm−2) at low applied potentials. Here we show that an efficient oxygen electrode can be developed by electrodepositing amorphous mesoporous nickel–iron composite nanosheets directly onto macroporous nickel foam substrates. The as-prepared oxygen electrode exhibits high catalytic activity towards water oxidation in alkaline solutions, which only requires an overpotential of 200 mV to initiate the reaction, and is capable of delivering current densities of 500 and 1,000 mA cm−2 at overpotentials of 240 and 270 mV, respectively. The electrode also shows prolonged stability against bulk water electrolysis at large current. Collectively, the as-prepared three-dimensional structured electrode is the most efficient oxygen evolution electrode in alkaline electrolytes reported to the best of our knowledge, and can potentially be applied for industrial scale water electrolysis.

Two-dimensional metal-organic frameworks represent a family of materials with attractive chemical and structural properties, which are usually prepared in the form of bulk powders. Here we show a generic approach to fabricate ultrathin nanosheet array of metal-organic frameworks on different substrates through a dissolution–crystallization mechanism. These materials exhibit intriguing properties for electrocatalysis including highly exposed active molecular metal sites owning to ultra-small thickness of nanosheets, improved electrical conductivity and a combination of hierarchical porosity. We fabricate a nickel-iron-based metal-organic framework array, which demonstrates superior electrocatalytic performance towards oxygen evolution reaction with a small overpotential of 240 mV at 10 mA cm−2, and robust operation for 20,000 s with no detectable activity decay. Remarkably, the turnover frequency of the electrode is 3.8 s−1 at an overpotential of 400 mV. We further demonstrate the promise of these electrodes for other important catalytic reactions including hydrogen evolution reaction and overall water splitting.

Polynary single‐atom structures can combine the advantages of homogeneous and heterogeneous catalysts while providing synergistic functions based on different molecules and their interfaces. However, the fabrication and identification of such an active‐site prototype remain elusive. Here we report isolated diatomic Ni‐Fe sites anchored on nitrogenated carbon as an efficient electrocatalyst for CO2 reduction. The catalyst exhibits high selectivity with CO Faradaic efficiency above 90 % over a wide potential range from −0.5 to −0.9 V (98 % at −0.7 V), and robust durability, retaining 99 % of its initial selectivity after 30 hours of electrolysis. Density functional theory studies reveal that the neighboring Ni‐Fe centers not only function in synergy to decrease the reaction barrier for the formation of COOH* and desorption of CO, but also undergo distinct structural evolution into a CO‐adsorbed moiety upon CO2 uptake.

Large-scale storage of renewable energy in the form of hydrogen (H2) fuel via electrolytic water splitting requires the development of water oxidation catalysts that are efficient and abundant. Carbon-based nanomaterials such as carbon nanotubes have attracted significant applications for use as substrates for anchoring metal-based nanoparticles. We show that, upon mild surface oxidation, hydrothermal annealing and electrochemical activation, multiwall carbon nanotubes (MWCNTs) themselves are effective water oxidation catalysts, which can initiate the oxygen evolution reaction (OER) at overpotentials of 0.3 V in alkaline media. Oxygen-containing functional groups such as ketonic C═O generated on the outer wall of MWCNTs are found to play crucial roles in catalyzing OER by altering the electronic structures of the adjacent carbon atoms and facilitates the adsorption of OER intermediates. The well-preserved microscopic structures and highly conductive inner walls of MWCNTs enable efficient transport of the electrons generated during OER.

Exploiting the valley degree of freedom to store and manipulate information provides a novel paradigm for future electronics. A monolayer transition-metal dichalcogenide (TMDC) with a broken inversion symmetry possesses two degenerate yet inequivalent valleys, which offers unique opportunities for valley control through the helicity of light. Lifting the valley degeneracy by Zeeman splitting has been demonstrated recently, which may enable valley control by a magnetic field. However, the realized valley splitting is modest (∼0.2 meV T). Here we show greatly enhanced valley spitting in monolayer WSe, utilizing the interfacial magnetic exchange field (MEF) from a ferromagnetic EuS substrate. A valley splitting of 2.5 meV is demonstrated at 1 T by magnetoreflectance measurements and corresponds to an effective exchange field of ∼12 T. Moreover, the splitting follows the magnetization of EuS, a hallmark of the MEF. Utilizing the MEF of a magnetic insulator can induce magnetic order and valley and spin polarization in TMDCs, which may enable valleytronic and quantum-computing applications.