Design of Efficient Catalysts with Double Transition Metal Atoms on C2N Layer.
Heterogeneous catalysis often involves molecular adsorptions to charged catalyst site and reactions triggered by catalyst charges. Here we use first-principles simulations to design oxygen reduction reaction (ORR) catalyst based on double transition metal (TM) atoms stably supported by 2D crystal C2N. It not only holds characters of low cost and high durability but also effectively accumulates surface polarization charges on TMs and later deliveries to adsorbed O2 molecule. The Co-Co, Ni-Ni, and Cu-Cu catalysts exhibit high adsorption energies and extremely low dissociation barriers for O2, as compared with their single-atom counterparts. Co-Co on C2N presents less than half the value of the reaction barrier of bulk Pt catalysts in the ORR rate-determining steps. These catalytic improvements are well explained by the dependences of charge polarization on various systems, which opens up a new strategy for optimizing TM catalytic performance with the least metal atoms on porous low-dimensional materials.
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Hefei Science Center of CAS, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Xiyu
X
Li
Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Institute of Applied Physics, Guizhou Synergetic Innovation Cen-ter of Scientific Big Data for Advanced Manufacturing Technology, Guizhou Normal College , Gaoxin Road 115, Guiyang, Guizhou 550018, P. R. China.
Wenhui
W
Zhong
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Hefei Science Center of CAS, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Peng
P
Cui
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Hefei Science Center of CAS, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Jun
J
Li
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, Hefei Science Center of CAS, School of Chemistry and Materials Science, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Jun
J
Jiang