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The development of efficient electrocatalysts for the CO2 reduction reaction (CO2RR) remains a challenge. Demonstrated here is a NiSn atomic‐pair electrocatalyst (NiSn‐APC) on a hierarchical integrated electrode, which exhibits a synergistic effect in simultaneously promoting the activity and selectivity of the CO2RR to formate. The NiSn atomic pair consists of adjacent Ni and Sn, each coordinated with four nitrogen atoms (N4‐Ni‐Sn‐N4). The as‐prepared NiSn‐APC displays exceptional activity for the CO2RR to formate with a turnover frequency of 4752 h−1, a formate productivity of 36.7 mol h−1 gSn−1 and an utilization degree of active sites (57.9 %), which are superior to previously reported single‐atomic catalysts. Both experimental data and density‐functional theory calculations verify the electron redistribution of Sn imposed by adjacent Ni, which reduces the energy barrier of the *OCHO intermediate and makes this potential‐determining step thermodynamically spontaneous. This synergistic catalysis provides a successful paradigm for rational design and preparation of atomic‐pair electrocatalysts with enhanced performance. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) materials have attracted increasing interest in electrochemical energy storage and conversion. As typical 2D materials, layered double hydroxides (LDHs) display large potential in this area due to the facile tunability of their composition, structure and morphology. Various preparation strategies, including in situ growth, electrodeposition and layer-by-layer (LBL) assembly, have been developed to directly modify electrodes by using LDH materials. Moreover, several composite materials based on LDHs and conductive matrices have also been rationally designed and employed in supercapacitors, batteries and electrocatalysis with largely enhanced performances. This feature article summarizes the latest developments in the design, preparation and evaluation of LDH materials toward electrochemical energy storage and conversion. [ABSTRACT FROM AUTHOR]

Magnetic films based on CoFe LDH nanoplatelets and porphyrin anions were fabricated by the layer-by-layer assembly technique with an assistance of an external magnetic field, which show enhanced electrochemical behavior and magnetic anisotropy. [ABSTRACT FROM AUTHOR]

Review: 149 refs. [ABSTRACT FROM AUTHOR]

Graphical abstract The (Ni, Fe)S 2 @MoS 2 heterostructures are directly prepared, which exhibits remarkable electrochemical performance towards overall water splitting. The interface engineering of obtained sulfides facilitie formation of S-H ads , which synergistically lower the chemisorption energy of the intermediates of HER and OER, thereby facilitating the electrocatalytic overall water splitting. Highlights • A synergetic electrocatalyst is achieved for water splitting based on (Ni, Fe)S 2 @MoS 2 heterostructrues. • The interface engineering of sulfide heterostructures facilitates the formation of S-H ads. • The stability can be further enhanced by optimizing the interface of electrode/electrolyte. Abstract Water splitting to generate hydrogen is a promising and sustainable process, whereas is limited by the large overpotential of electrode materials for cathode hydrogen evolution reaction (HER) and anode oxygen evolution reaction (OER). Here we present an interface engineering strategy to construct efficient bifunctional electrocatalyst based on (Ni, Fe)S 2 @MoS 2 heterostructrues for water-splitting process. The as-prepared (Ni, Fe)S 2 @MoS 2 catalyst gives remarkable electrochemical activity and durability under alkaline environments, with a low overpotential of 130 mV for HER and 270 mV for OER to deliver the current density of 10 mA cm−2, respectively. In combination with in-situ Raman spectra, we demonstrate that the constructed interfacial active sites are favorable to the formation of S-H ads , which synergistically lower the chemisorption energy of the intermediates of HER and OER, thereby facilitating the electrocatalytic overall water splitting. Furthermore, we regulate the interface of (Ni, Fe)S 2 @MoS 2 and electrolyte through changing the composition of electrolyte to achieve much longer electrochemical stability of this hybrid sulfide electrocatalyst. [ABSTRACT FROM AUTHOR]