Illustration for the selective conversion of carbon dioxide based on the lattice engineering of catalytic sites in photocatalysts (Courtesy of XIONG Yujie and Journal of the American Chemical Society)
To address this grand challenge, Xiong research group has incorporated single-atom copper sites into palladium lattice, which can largely prevent the oxidation of copper sites. Meanwhile, the strong binding of hydrogen to palladium can suppress hydrogen evolution and other side reactions in photocatalytic carbon dioxide conversion. Based on the bimetallic palladium-copper structures, the researchers have further combined synchrotron radiation-based X-ray absorption fine structure spectroscopy characterization, in-situ infrared spectroscopy detection and theoretical simulations to establish the structure-property relationship between catalytic sites and carbon dioxide conversion performance. Taking titania photocatalyst as an example, the conversion selectivity carbon dioxide to methane in photocatalysis achieves 96% by Pd7Cu1-TiO2. This design is also applicable to visible-responsive photocatalysts, which can be implemented in photocatalytic carbon dioxide conversion under visible illumination. This work provides fresh insights into the catalytic site design for selective photocatalytic carbon dioxide conversion, and highlights the importance of catalyst lattice engineering at atomic precision to catalytic performance.
Profs. Li Song, Junfa Zhu, Zeming Qi and Jun Jiang made important contributions to the synchrotron radiation-based X-ray absorption fine structure spectroscopy, photoelectron spectroscopy, in-situ diffuse reflectance infrared Fourier-transform spectroscopy characterizations and theoretical simulations in this work. This work was financially supported by the 973 Program, NSFC and CAS Key Research Program of Frontier Sciences.