Solar-driven reduction of dinitrogen (N ) to ammonia (NH ) is severely hampered by the kinetically complex and energetically challenging multielectron reaction. Oxygen vacancies (OVs) with abundant localized electrons on the surface of bismuth oxybromide-based semiconductors are demonstrated to have the ability to capture and activate N , providing an alternative pathway to overcome such limitations. However, bismuth oxybromide materials are susceptible to photocorrosion, and the surface OVs are easily oxidized and therefore lose their activities. For realistic photocatalytic N fixation, fabricating and enhancing the stability of sustainable OVs on semiconductors is indispensable. This study shows the first synthesis of self-assembled 5 nm diameter Bi O Br nanotubes with strong nanotube structure, suitable absorption edge, and many exposed surface sites, which are favorable for furnishing sufficient visible light-induced OVs to realize excellent and stable photoreduction of atmospheric N into NH in pure water. The NH generation rate is as high as 1.38 mmol h g , accompanied by an apparent quantum efficiency over 2.3% at 420 nm. The results presented herein provide new insights into rational design and engineering for the creation of highly active catalysts with light-switchable OVs toward efficient, stable, and sustainable visible light N fixation in mild conditions.
Through a facile and effective strategy by employing lithium molten salts the controlled synthesis of 2H- and 1T-MoS monolayers with high-yield production is achieved. Both phases of MoS monolayers exhibit high stabilities. When used as a catalyst for hydrogen evolution, these phased MoS monolayers deliver respective advantages in the field of electro- and photo-catalytic hydrogen evolution.
Electrochemical conversion of CO2 into valued products is one of the most important issues but remains a great challenge in chemistry. Herein, we report a novel synthetic approach involving prolonged thermal pyrolysis of hemin and melamine molecules on graphene for the fabrication of a robust and efficient single‐iron‐atom electrocatalyst for electrochemical CO2 reduction. The single‐atom catalyst exhibits high Faradaic efficiency (ca. 97.0 %) for CO production at a low overpotential of 0.35 V, outperforming all Fe‐N‐C‐based catalysts. The remarkable performance for CO2‐to‐CO conversion can be attributed to the presence of highly efficient singly dispersed FeN5 active sites supported on N‐doped graphene with an additional axial ligand coordinated to FeN4. DFT calculations revealed that the axial pyrrolic nitrogen ligand of the FeN5 site further depletes the electron density of Fe 3d orbitals and thus reduces the Fe–CO π back‐donation, thus enabling the rapid desorption of CO and high selectivity for CO production.
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