4.8 Article

Understanding the Synergistic Oxidation in Dichalcogenides through Electrochemiluminescence Blinking at Millisecond Resolution

Journal

ADVANCED MATERIALS
Volume 33, Issue 48, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202105039

Keywords

dichalcogenides; electrochemiluminescence blinking; millisecond resolution; sulfur vacancies; synergistic oxidation

Funding

  1. National Natural Science Foundation of China [22025403]
  2. Washington State University Start-up Fund
  3. State Key Laboratory of Pollution Control and Resource Reuse [PCRR-ZZ-202106]

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The synergistic oxidation between edge and basal plane in molybdenum disulfide (MoS2) was observed through electrogenerated chemiluminescence (ECL), revealing the formation of new active sites induced by oxygen doping. The study showed that the formation of sulfur vacancies is more conducive to oxygen doping, leading to the generation of Mo-O-Mo active sites.
The oxidation of transition metal dichalcogenides (TMDCs) has been extensively studied and applied in electronics, optics, and energy sources because of its tunable structure and performance. However, due to the lack of appropriate technology, dynamically observe the oxidation process remains an arduous task. Herein, the synergistic oxidation between edge and basal plane in molybdenum disulfide (MoS2) is observed through electrogenerated chemiluminescence (ECL) blinking with a millisecond resolution. In addition, the ECL method provides a simple, convenient, and quick way to judge structural changes. The transient elevation of the ECL intensity proved the intermittent doping of oxygen at MoS2, which generates O-atom active sites. High ECL intensity enhanced from the produced hydroperoxide intermediates eases the monitoring of MoS2 particles. Further study shows that the formation of sulfur vacancies at MoS2, by the edge activation of hydrogen peroxide and the migration of oxygen to the basal plane, is more conducive to oxygen doping that favors the formation of Mo-O-Mo as new active sites to induce bursts. The revealing of sulfur vacancy-governed blinking from MoS2 indicates a complex interaction between oxygen and MoS2. The same phenomenon is observed on tungsten disulfide (WS2), which provides new information about the oxidation feature of 2D dichalcogenides.

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