Formate production from direct CO2 electrolysis is economically appealing yet challenging in activity, selectivity, and stability. Herein, sulfur and silver dual‐decorated indium quasi‐core–shell structures with compressive or tensile strain are rationally designed for efficiently electrocatalyzing CO2 to formate. The introduction of Ag and S increases the current density, Faradaic efficiency, and operational stability of formate both in H‐cell and flow cell systems. As a result, the optimized Ag‐In‐S bimetallic catalysts exhibit the FEHCOO− of ≈94.0% with a JHCOO− of more than −560.0 mA cm−2 at ≈−0.951 VRHE in the flow cell system, which far surpasses the undecorated In catalyst. The experimental and theoretical calculations provide a deeper understanding of the role of the interfacial strain between In or In4Ag9 shell and AgIn2 core in boosting the electrocatalytic CO2 reduction efficiency, in which the formation energy of *OCHO intermediate decreases and the charge transfer rate is accelerated by interface strain.
During partial oxidation of methane (POM), the greatest challenge is to maintain the thermal stability of the catalyst at high temperatures. One of the most effective ways to improve thermal stability is to construct core-shell structure. Herein, using a microemulsion method, we synthesized a core-shell Ni/nanorod-CeO2@SiO2 catalyst, in which the Ni nanoparticles were supported on the CeO2 nanorods and encapsulated by SiO2 shells. Based on a series of characterizations, we found that the Ni particles are of nanosize (2.2 nm) and the thickness of the SiO2 shell is about 8 nm in the core-shell catalyst. Moreover, the Ni/nanorod-CeO2@SiO2 catalyst can perfectly maintain rod-like structures of the CeO2 support and enhance interaction between the metal Ni and CeO2, significantly reducing the sintering of metal Ni particles at high temperatures. Therefore, the as-prepared Ni/nanorod-CeO2@SiO2 catalyst shows high catalytic activity and good thermal stability during the POM reaction.
Electrochemically reducing carbon dioxide (CO2RR) to ethylene is one of the most promising strategies to reduce carbon dioxide emissions and simultaneously produce high value‐added chemicals. However, the lack of catalysts with excellent activity and stability limits the large‐scale application of this technology. In this work, a graphitic carbon nitride (g‐C3N4)‐supported Cu2O composite was fabricated, which exhibited a 32.2 % faradaic efficiency of C2H4 with a partial current density of −4.3 mA cm−2 at −1.1 V vs. reversible hydrogen electrode in 0.1 m KHCO3 electrolyte. The introduction of g‐C3N4 support not only enhanced the uniform dispersion of Cu2O nanocubes, but also stabilized the important *CO intermediates. Moreover, the g‐C3N4 itself had a good activity of reducing CO2 to form *CO, which enriched the key intermediates of C−C coupling around cuprous oxide. The findings highlight the importance of the g‐C3N4 support, a unique two‐dimensional material, including not only the strong CO2 adsorption and activation capacity but also its synergistic effect with the cuprous oxide in CO2RR selectivity.
A gradual sulfur doping strategy was first proposed here to expand the optical absorption range, improve the separation efficiency of photogenerated electron–hole pairs, and finally enhance the photocatalytic activity.
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