The development of efficient catalysts is of great importance for hydrogen evolution reaction (HER) of water splitting via electrocatalytic/photocatalytic processes to remediate the current severe environmental and energy problems. By aid of the stabilization effects of uncoordinated groups and inherent pore‐confinement of amine‐functionalized metal–organic frameworks (NH2‐MIL‐125), two forms of Ru species including nanoparticles (NPs) and/or single atoms (SAs) can be firmly embedded in NH2‐MIL‐125 derived N‐doped TiO2/C support (N‐TC), and thus obtain two kinds of samples named Ru‐NPs/SAs@N‐TC and Ru‐SAs@N‐TC, respectively. In the synthetic process, the initial feeding amount of Ru3+ ions not only strongly determines the final size and dispersion states of Ru species but also the morphology and defective structures of N‐TC support. Impressively, Ru‐NPs/SAs@N‐TC exhibit superior catalytic activities to Ru‐SAs@N‐TC for either electrocatalytic or photocatalytic HER. This should be attributed to its larger specific surface area and benefiting from synergistic coupling of Ru NPs and Ru SAs. It is envisioned that the present work can provide a new avenue for development of high‐efficiency and multifunctional hybrid catalysts in sustainable energy conversion.

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The flexible Li‐O2 battery is suitable to satisfy the requirements of a self‐powered energy system, thanks to environmental friendliness, low cost, and high theoretical energy density. Herein, a flexible porous bifunctional electrode with both electrocatalytic and photocatalytic activity was synthesized and introduced as a cathode to assemble a high‐performance Li‐O2 battery that achieved an overpotential of 0.19 V by charging with the aid of solar energy. As a proof‐of‐concept application, a flexible Li‐O2 battery was constructed and integrated with a solar cell via a scalable encapsulate method to fabricate a flexible self‐powered energy system with excellent flexibility and mechanical stability. Moreover, by exploring the evolution of the electrode morphology and discharge products (Li2O2), the charging process of the Li‐O2 battery powered by solar energy and solar cell was demonstrated.

In this work, we have successfully triggered the aqueous auto‐redox reactions between reductive Ce(OH)3 and oxidative MnO4−/Pd2+ ions to form PdO/Mn3O4/CeO2 (PMC) nanocomposites. PMC could spontaneously self‐assemble into compact encapsulation on the surface of halloysite nanotubes (HNTs) to form the final one dimensional HNTs supported PMCs (HPMC). It is identified that there exists strong synergistic effects among the components of PdO, Mn3O4, and CeO2, and hence HPMC could show excellent performance on photoassisted thermal catalytic CH4 combustion that its light‐off temperature was sharply reduced to be 180 °C under visible light irradiation. Based on detailed studies, it is found that the catalytic reaction process well follows the classic MVK mechanism, and adsorption/activation of O2 into active oxygen species (O*) should be the rate‐determining step for CH4 conversion.