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Ion regulation strategy is regarded as a promising pathway for designing transition metal oxide‐based electrocatalysts for oxygen evolution reaction (OER) with improved activity and stability. Precise anion conditioning can accurately change the anionic environment so that the acid radical ions (SO42−, PO32−, SeO42−, etc.), regardless of their state (inside the catalyst, on the catalyst surface, or in the electrolyte), can optimize the electronic structure of the cationic active site and further increase the catalytic activity. Herein, we report a new approach to encapsulate S atoms at the tetrahedral sites of the NaCl‐type oxide NiO to form a tetraoxo‐tetrahedral coordination structure (S‐O4) inside the NiO (S‐NiO ‐I). Density functional theory (DFT) calculations and operando vibrational spectroscopy proves that this kind of unique structure could achieve the S‐O4 and Ni‐S stable structure in S‐NiO‐I. Combining mass spectroscopy characterization, it could be confirmed that the S‐O4 structure is the key factor for triggering the lattice oxygen exchange to participate in the OER process. This work demonstrates that the formation of tetraoxygen tetrahedral structure is a generalized key for boosting the OER performances of transition metal oxides. [ABSTRACT FROM AUTHOR]

Designing polymeric photocatalysts at the molecular level to modulate the photogenerated charge behavior is a promising and challenging strategy for efficient hydrogen peroxide (H2O2) photosynthesis. Here, we introduce electron‐deficient 1,4‐dihydroxyanthraquinone (DHAQ) into the framework of resorcinol‐formaldehyde (RF) resin, which modulates the donor/acceptor ratio from the perspective of molecular design for promoting the charge separation. Interestingly, H2O2 can be produced via oxygen reduction and water oxidation pathways, verified by isotopic labeling and in situ characterization techniques. Density functional theory (DFT) calculations elucidate that DHAQ can reduce the energy barrier for H2O2 production. RF‐DHAQ exhibits excellent overall photosynthesis of H2O2 with a solar‐to‐chemical conversion (SCC) efficiency exceeding 1.2 %. This work opens a new avenue to design polymeric photocatalysts at the molecular level for high‐efficiency artificial photosynthesis. [ABSTRACT FROM AUTHOR]

Keywords: Hollow Structure; Hydrogenation; Nanoreactor; Polymer; Supported Catalyst EN Hollow Structure Hydrogenation Nanoreactor Polymer Supported Catalyst 1 1 1 10/18/23 20231023 NES 231023 B Hollow nanoreactors b with a hollow multishelled structure and spatially loaded metal nanoparticles are reported by Jian Liu et al. in their Research Article (e202307096). Hollow Structure, Hydrogenation, Nanoreactor, Polymer, Supported Catalyst Calculations provide insights into the nanoreactors with distinct behaviors due to the differences in the energy barrier of substrate adsorption and steric hindrance. [Extracted from the article]