Tuning the coordination environment is the research axis of single atom catalysts (SACs). SACs are commonly stabilized by various defects from support. Here, we report a lattice confined Pd SAC using MnO_(2) as suppor...Tuning the coordination environment is the research axis of single atom catalysts (SACs). SACs are commonly stabilized by various defects from support. Here, we report a lattice confined Pd SAC using MnO_(2) as support. Compared with the Pd clusters anchored on the surface, the lattice confined Pd single atoms allows spontaneous exaction of surrounding lattice oxygen at room temperature when employed in CO oxidation. The MnO_(2) supported Pd SAC exhibited a high turnover frequency of 0.203 s^(−1) at low reaction temperature, which is higher than that of recently reported Pd SACs. Theoretical calculations also confirmed the confined monatomic Pd activate lattice oxygen with an ultralow energy barrier. Our results illustrate that the unique coordination environment of single atom provided by lattice confinement is promising to boost the activity of SACs.展开更多
基金X.Liao gratefully thanks the support from the National Natural Science Foundation of China(No.21706216)the Sichuan Science and Technology Program(2020YFG0162)+3 种基金the Young Scholar Project in Xihua University.X.Li acknowledges the support from the National Natural Science Foundation of China(No.21972163)the Fundamental Research Funds for the Central Universities and DHU Distinguished Young Professor Program,and the Development Fund for Shanghai Talents.Z.Jiang acknowledges financial support from the Joint Fund U1732267.M.Y.thanks the JSPS KAKENHI(No.JP 18H05517)JST-CREST for financial supports,and Riken SPring-8 for the approval of the SRXRD measurement(20190028)EXAFS studies were carried out at the BL14W1 beamline in the Shanghai Synchrotron Radiation Facility[63],Shanghai Institute of Applied Physics,China(16ssr-f00787).X.Liao gratefully thanks the useful discussion with Ya Wang and Yanmin Liu.
文摘Tuning the coordination environment is the research axis of single atom catalysts (SACs). SACs are commonly stabilized by various defects from support. Here, we report a lattice confined Pd SAC using MnO_(2) as support. Compared with the Pd clusters anchored on the surface, the lattice confined Pd single atoms allows spontaneous exaction of surrounding lattice oxygen at room temperature when employed in CO oxidation. The MnO_(2) supported Pd SAC exhibited a high turnover frequency of 0.203 s^(−1) at low reaction temperature, which is higher than that of recently reported Pd SACs. Theoretical calculations also confirmed the confined monatomic Pd activate lattice oxygen with an ultralow energy barrier. Our results illustrate that the unique coordination environment of single atom provided by lattice confinement is promising to boost the activity of SACs.
