4.8 Article

Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N-CuO for organic pollutants degradation

Journal

NATURE COMMUNICATIONS
Volume 13, Issue 1, Pages -

Publisher

NATURE PORTFOLIO
DOI: 10.1038/s41467-022-33149-4

Keywords

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Funding

  1. Natural Science Foundation of China [22225604, 22076082, 21874099, 22176140, 22006029]
  2. Tianjin Commission of Science and Technology as key technologies RD projects [19YFZCSF00740, 20YFZCSN01070, 21YFSNSN00250]
  3. Frontiers Science Center for New Organic Matter [63181206]

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The authors propose a nitrogen doping strategy for selective electrocatalytic singlet oxygen production. By using this strategy, the selectivity and activity of O-1(2) production can be significantly improved.
Side-on configuration of O-2 on the catalysts conventionally leads to reduction of O-2 to water. Here, the authors propose a nitrogen doping strategy with Pauling-type adsorption of O-2 for selective electrocatalytic singlet oxygen production. Due to environmentally friendly operation and on-site productivity, electrocatalytic singlet oxygen (O-1(2)) production via O-2 gas is of immense interest in environment purification. However, the side-on configuration of O-2 on the catalysts surface will lead to the formation of H2O, which seriously limits the selectivity and activity of O-1(2) production. Herein, we show a robust N-doped CuO (N-CuO) with Pauling-type (end-on) adsorption of O-2 at the N-Cu-O-3 sites for the selective generation of O-1(2) under direct-current electric field. We propose that Pauling-type configuration of O-2 not only lowers the overall activation energy barrier, but also alters the reaction pathway to form O-1(2) instead of H2O, which is the key feature determining selectivity for the dissociation of Cu-O bonds rather than the O-O bonds. The proposed N dopant strategy is applicable to a series of transition metal oxides, providing a universal electrocatalysts design scheme for existing high-performance electrocatalytic O-1(2) production.

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