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Single‐Atom or Dual‐Atom in TiO<sub>2</sub>Nanosheet: Which is the Better Choice for Electrocatalytic Urea Synthesis?

Lu Pan, Jingnan Wang, Fei Lu, Qiang Liu, Yuhang Gao, Yan Wang, Jingzhe Jiang, Chao Sun, Jian Wang, Xi Wang

2022Angewandte Chemie International Edition166 citationsDOI

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 Pd 1 −TiO 2 and dual‐atom Pd 1 Cu 1 −TiO 2 nanosheets. An ultrahigh urea activity of 166.67 mol urea mol Pd −1 h 1 with the corresponding 22.54 % Faradaic efficiency at −0.5 V vs. reversible hydrogen electrode (RHE) is achieved over Pd 1 Cu 1 −TiO 2 , which is much higher than that of Pd 1 −TiO 2 . Various characterization including an in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and theoretical calculations demonstrate that dual‐atom Pd 1 Cu 1 site in Pd 1 Cu 1 −TiO 2 is more favorable for producing urea, which experiences a C−N coupling pathway with a lower energy barrier compared with Pd 1 in Pd 1 −TiO 2 .

Topics & Concepts

Atom (system on chip)CatalysisNanosheetMaterials scienceUreaDiffuse reflectance infrared fourier transformVacancy defectElectrochemistryElectrodePhotochemistryNanotechnologyChemistryCrystallographyPhysical chemistryPhotocatalysisOrganic chemistryEmbedded systemComputer scienceAmmonia Synthesis and Nitrogen ReductionElectrocatalysts for Energy ConversionAdvanced Photocatalysis Techniques
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