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The use of molecular modulators to reduce the defect density at the surface and grain boundaries of perovskite materials has been demonstrated to be an effective approach to enhance the photovoltaic performance and device stability of perovskite solar cells. Herein, we employ crown ethers to modulate perovskite films, affording passivation of undercoordinated surface defects. This interaction has been elucidated by solid-state nuclear magnetic resonance and density functional theory calculations. The crown ether hosts induce the formation of host-guest complexes on the surface of the perovskite films, which reduces the concentration of surface electronic defects and suppresses nonradiative recombination by 40%, while minimizing moisture permeation. As a result, we achieved substantially improved photovoltaic performance with power conversion efficiencies exceeding 23%, accompanied by enhanced stability under ambient and operational conditions. This work opens a new avenue to improve the performance and stability of perovskite-based optoelectronic devices through supramolecular chemistry.

The electrochemical CO2 reduction reaction (CO2RR) typically uses transition metals as the catalysts. To improve the efficiency, tremendous efforts have been dedicated to tuning the morphology, size, and structure of metal catalysts and employing electrolytes that enhance the adsorption of CO2. We report here a strategy to enhance CO2RR by constructing the metal–oxide interface. We demonstrate that Au–CeOx shows much higher activity and Faradaic efficiency than Au or CeOx alone for CO2RR. In situ scanning tunneling microscopy and synchrotron-radiation photoemission spectroscopy show that the Au–CeOx interface is dominant in enhancing CO2 adsorption and activation, which can be further promoted by the presence of hydroxyl groups. Density functional theory calculations indicate that the Au–CeOx interface is the active site for CO2 activation and the reduction to CO, where the synergy between Au and CeOx promotes the stability of key carboxyl intermediate (*COOH) and thus facilitates CO2RR. Similar interface...

The electrochemical CO