Single‐Atom or Dual‐Atom in TiO2 Nanosheet: Which is the Better Choice for Electrocatalytic Urea Synthesis?. (13th January 2023) - Pan, Lu
Abstract: As rising star materials, single‐atom and dual‐atom catalysts have been widely reported in the electro‐catalysis area. To answer the key question: single‐atom and dual‐atom catalysts, which is better for electrocatalytic urea synthesis? we design two types of catalysts via a vacancy‐anchorage strategy: single‐atom Pd1 −TiO2 and dual‐atom Pd1 Cu1 −TiO2 nanosheets. An ultrahigh urea activity of 166.67 molurea molPd −1 h 1 with the corresponding 22.54 % Faradaic efficiency at −0.5 V vs. reversible hydrogen electrode (RHE) is achieved over Pd1 Cu1 −TiO2, which is much higher than that of Pd1 −TiO2 . Various characterization including an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and theoretical calculations demonstrate that dual‐atom Pd1 Cu1 site in Pd1 Cu1 −TiO2 is more favorable for producing urea, which experiences a C−N coupling pathway with a lower energy barrier compared with Pd1 in Pd1 −TiO2 . Abstract : Dual‐atom Pd1 Cu1 active center in Pd1 Cu1 −TiO2 is more favourable for producing urea, and experiences a C−N coupling pathway with a lower energy barrier as compared with single‐atom Pd1 in Pd1 −TiO2 .