Surface lattice oxygen in transition‐metal oxides plays a vital role in catalytic processes. Mastering activation of surface lattice oxygen and identifying the activation mechanism are crucial for the development and design of advanced catalysts. A strategy is now developed to create a spinel Co3O4 /perovskite La0.3Sr0.7CoO3 interface by in situ reconstruction of the surface Sr enrichment region in perovskite LSC to activate surface lattice oxygen. XAS and XPS confirm that the regulated chemical interface optimizes the hybridized orbital between Co 3d and O 2p and triggers more electrons in oxygen site of LSC transferred into lattice of Co3O4 , leading to more inactive O2− transformed into active O2−x. Furthermore, the activated Co3O4/LSC exhibits the best catalytic activities for CO oxidation, oxygen evolution, and oxygen reduction. This work would provide a fundamental understanding to explain the activation mechanism of surface oxygen sites.

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The first observation of surface metallization of TiO 2Àx induced by fluoride ions is presented. The emerging metallic states are contributed by the 3d orbital of surface Ti and the 2p orbital of surface bridging F, which are intrinsically originated from the strong electron repulsion between F À and adjacent Ti 3+ . The metalized TiO 2Àx with reduced work function and downward band bending possesses high electron-donating power to supported Ru species via atomic-scale ohmic contacts, exhibiting unprecedented photocatalytic performances for ammonia synthesis across the entire solar spectrum region (200-1550 nm) at room temperature. Mechanism and kinetic analysis revealed that the loaded Ru could behave as efficient electron sinks to accumulate photogenerated electrons and that the metallic surface markedly enhanced the dissociation of H 2 and N 2 by the hot electrons generated by the visible or even infrared light irradiation.

Surface lattice oxygen in transition‐metal oxides plays a vital role in catalytic processes. Mastering activation of surface lattice oxygen and identifying the activation mechanism are crucial for the development and design of advanced catalysts. A strategy is now developed to create a spinel Co3O4 /perovskite La0.3Sr0.7CoO3 interface by in situ reconstruction of the surface Sr enrichment region in perovskite LSC to activate surface lattice oxygen. XAS and XPS confirm that the regulated chemical interface optimizes the hybridized orbital between Co 3d and O 2p and triggers more electrons in oxygen site of LSC transferred into lattice of Co3O4 , leading to more inactive O2− transformed into active O2−x. Furthermore, the activated Co3O4/LSC exhibits the best catalytic activities for CO oxidation, oxygen evolution, and oxygen reduction. This work would provide a fundamental understanding to explain the activation mechanism of surface oxygen sites.

Achieving efficient photocatalytic ammonia synthesis under mild conditions provides a sustainable approach for producing nitrogen-containing resources. The current challenge is to find ideal photocatalysts with strong N2 activation capacity and superior interfacial charge transfer. Herein, we report that efficient photocatalytic ammonia synthesis can be achieved across the entire visible light region over Ti-doped defective ZnO1–x with Ru cocatalyst loading. Due to the presence of local electrostatic fields and unique surface structures, the Ti atoms doped on the nonpolar (100) facets of ZnO1–x trigger the most strong activation of N2 with excellent electron back-donation power, resulting in an unprecedented elongation of NN bonds, from the original 1.117 to 1.328 Å, as well as one-electron reduction of N2 to N2 –. The supported Ru cocatalyst enables the upward band bending of ZnO and the formation of interfacial Schottky contacts, simultaneously enhancing the reduction potential of photogenerated electrons and minimizing electron–hole recombination, which further promotes the efficiency of ammonia synthesis.

Here, we report that efficient photocatalytic ammonia synthesis was realized across the entire solar spectrum by using Ru modified anatase/TiO2(B) heterostructured nanosheet arrays. The superior NH3 production rates of 2004...

In nature, the biological N2 fixation is accessed by nitrogenase containing FeMo-cofactor under ambient conditions. Unfortunately, due to Brønsted-Evans-Polanyi relations, the strong Mo-N bond restricts the development of efficient Mo-based...

It is highly desirable to develop the low-pressure, low-temperature ammonia synthesis process. Although this process is, in principle, thermodynamically feasible under ambient conditions, it remains a big challenge to find...