Ultrathin In‐Plane Heterostructures for Efficient CO2 Chemical Fixation

Abstract Chemical fixation of carbon dioxide (CO 2 ) into value‐added organics is regarded as a competitive and viable method in large scale industrial production, during which the catalysts with promoting CO 2 activation ability are needed. Herein, we proposed an in‐plane heterostructure strategy to construct Lewis acid–base sites for efficient CO 2 activation. By taking ultrathin in‐plane Cu 2 O/Cu heterostructures as a prototype, we show that Lewis acid‐base sites on heterointerface can facilitate a mixed C and O dual coordination on surface, which not only strengthen CO 2 adsorption, but also effectively activate the inert molecules. As revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and quasi in situ X‐ray photoelectron spectroscopy (XPS), Lewis acid‐base sites could readily activate CO 2 to . CO 2 − species, which is the key intermediate radical for CO 2 fixation. As a result, abundant Lewis acid–base sites endow Cu 2 O/Cu nanosheets with excellent performances for dimethyl carbonate generation, a high conversion yield of 28 % with nearly 100 % selectivity under mild conditions. This study provides a model structure for CO 2 fixation reactions.