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Abstract: Electrochemical carbon dioxide (CO2) reduction can produce valuable carbonaceous compounds that are in significant demand, due to its ability to decrease the accumulated atmospheric CO2 and improve the intermittent nature of renewable energy sources. Considering the sluggish kinetics of CO2 reduction reaction, the multielectron–proton transfer process, and the inevitable mixed reduction products, designing efficient and robust electrocatalysts that benefit from the structure–activity relationship is the focus to promote CO2 conversion. In this review, various metal‐based materials are first classified and discussed in terms of their structural and elemental compositions for catalytic behaviors. Afterward, the most intrinsic microstructural/electronic effects as well as the influence of compositional alteration on the catalyst activity, selectivity, and stability are summarized. Additionally, recent attempts to develop the assigned electrochemical cells are surveyed and described from a technological point of view. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

A class of ruthenium-nickel alloy catalysts featured with nanoporous nanowires (NPNWs) were synthesized by a strategy combining rapid solidification with two-step dealloying. RuNi NPNWs exhibit excellent electrocatalytic activity and stability for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in which the RuNi-2500 NPNWs catalyst shows an OER overpotential of 327 mV to deliver a current density of 10 mA cm−2 and the RuNi-0 NPNWs catalyst requires the overpotential of 69 mV at 10 mA cm−2 showing the best HER activity in alkaline media. Moreover, the RuNi-1500 NPNWs catalyst was used as the bifunctional electrocatalyst in a two-electrode alkaline electrolyzer for water splitting, which exhibits a low cell voltage of 1.553 V and a long-term stability of 24 h at 10 mA cm−2, demonstrating that the RuNi NPNWs catalysts can be considered as promising bifunctional alkaline electrocatalysts. A class of ruthenium-nickel alloy catalysts featured with nanoporous nanowires (NPNWs) was synthesized by a strategy combined rapid solidification with two-step dealloying, in which the total cell voltage of RuNi-1500 NPNWs electrolyzer for water splitting is 1.553 V to deliver a current density of 10 mA cm−2. [Display omitted] • A two-step dealloying strategy was used to prepare RuNi catalysts. • RuNi catalysts exhibit a unique nanoporous nanowires (NPNWs) morphology. • RuNi NPNWs catalysts show excellent electrocatalytic performance for OER and HER. • RuNi NPNWs catalysts can be used as bifunctional catalysts for water splitting. [ABSTRACT FROM AUTHOR]

The synthesis of cost-effective and high-performance electrocatalysts for water splitting is the main challenge in electrochemical hydrogen production. In this study, we adopted a high throughput method to prepare bi-metallic catalysts for oxygen/hydrogen evolution reactions (OER/HER). A series of Ni–Mo alloy electrocatalysts with tunable compositions were prepared by a simple co-sputtering method. Due to the synergistic effect between Ni and Mo, the intrinsic electrocatalytic activity of the Ni–Mo alloy electrocatalysts is improved, resulting in excellent HER and OER performances. The Ni 90 Mo 10 electrocatalyst shows the best HER performance, with an extremely low overpotential of 58 mV at 10 mA cm−2, while the Ni 40 Mo 60 electrocatalyst shows an overpotential of 258 mV at 10 mA cm−2 in OER. More significantly, the assembled Ni 40 Mo 60 //Ni 90 Mo 10 electrolyzer only needs a cell voltage of 1.57 V to reach 10 mA cm−2 for overall water splitting. [Display omitted] • A high throughput method was used to prepare Ni–Mo alloy catalysts. • Ni–Mo alloy catalysts exhibit remarkable activity and stability for HER and OER. • The Ni–Mo alloy acts as a bifunctional catalyst for overall water splitting. • The synergistic effect between Ni and Mo leads to the excellent performances. [ABSTRACT FROM AUTHOR]