Single‐Atom or Dual‐Atom in TiO2 Nanosheet: Which is the Better Choice for Electrocatalytic Urea Synthesis?. (13th January 2023)

• Record Type: Journal Article
• Authors: Pan, Lu; Wang, Jingnan; Lu, Fei; Liu, Qiang; Gao, Yuhang; Wang, Yan; Jiang, Jingzhe; Sun, Chao; Wang, Jian; Wang, Xi
• Is Part Of: Angewandte Chemie. Volume 135:Number 8(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2023-01-13
• Subjects: C−N Coupling -- Dual-Atom Catalyst -- Electrocatalytic Urea Synthesis -- Synergistic Effect; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202216835
• Languages: English
• ISSNs: 0044-8249

Abstract

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 .