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Cu-catalyzed CO2 electroreduction can produce various hydrocarbons and oxygenates. However, it suffers from low activity and poor selectivity. Herein, Cu-decorated CeO2 composites (Cu y /CeO2) with distinct interfacial characteristics were fabricated through a highly controllable synthesis, based on chemical prelithiation of CeO2 and then galvanic displacement with Cu. The Cu decoration induced a strong-binding site for CO2 adsorption at the Cu and CeO2 interface, facilitating the CO2 activation and conversion to the *CO intermediate on the nearby Cu surface. Selective CO2 conversion to C1 or C2+ products was customized by adjusting the Cu decoration amount. With the increase in the Cu loading, the C1 and C2+ products exhibited a declining and volcano-shaped trend, showing a maximum faradaic efficiency of 70 and 63%, respectively. In situ infrared and Raman spectroscopy revealed that the reduction pathway depended on the relative ratio of the low-frequency band *COLFB to the high-frequency band *COHFB. Our findings may contribute to the rational design of heterostructured catalysts toward CO2 electroreduction.

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mechanical properties, good processing properties, ease of chemical modification, and easy preparation processes. [6][7][8][9] It is clear from the Jablonski diagram that to achieve phosphorescence emission, we can follow two approaches. One is to promote the S 1 → T n intersystem crossing. [10] The second is to suppress the nonradiative relaxation processes. Traditionally, organic molecules cannot emit phosphorescence at room temperature due to their inherently weak spin-orbit coupling, which means that excitons cannot efficiently span single and triplet states. [11] Therefore, it is often necessary to create strong intermolecular interactions to build a rigid network structure to enable phosphorescence generation and enhancement at room temperature. It is still a difficult task to build a non-toxic, non-hazardous, environmentally friendly, room-temperature phosphorescent material that can achieve colorful and long lifetimes. Most natural polymers are biocompatible, environmentally friendly, and non-toxic. Therefore, it is essential to explore more natural polymers with RTP properties that can be used to construct RTP emitting materials with long lifetimes. Usually, in order to obtain longer-lived and more-efficient phosphorescence emissions, researchers increase the inter-system scattering rate by introducing heavy atoms to increase the spin-orbit coupling between single and triplet states [12] or by cross-linking and polymerizing to produce a rigid environment to suppress non-radiative transitions. [13] Actually, several macrocycles, such as cyclodextrin and cucurbituril, have been used to tune phosphorescent characteristics. [14] Most of these only show adjustability in solution, reports on tunable RTP in the solid state are scarce.There is an increasing interest in stimulus-responsive luminescent materials that can undergo physical or chemical changes in response to external stimuli, such as mechanical forces, light, PH, and heat, due to the possible applications of such materials in the fields of lighting and display, optoelectronic devices, data storage, anti-counterfeiting, bio-imaging, and sensing. [15][16][17][18][19][20][21] To date, most of the stimulus-responsive luminescent materials have been based on fluorescence. [22][23][24] Compared with fluorescence emission, phosphorescence emission

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