期刊
ACS NANO
卷 15, 期 8, 页码 13504-13515出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c04126
关键词
electrocatalysis; alkaline water splitting; nickel molybdate; molybdenum leaching; in situ catalyst formation; nanostructures; time-resolved operando Raman spectroscopy
类别
资金
- eSCALED project
- European Union's Horizon 2020 Research and Innovation Programme under the Marie Sklodowska-Curie Grant [765376]
- Swedish Research Council (VR) [2015-03814]
- Myfab
- Swedish Research Council [2015-03814] Funding Source: Swedish Research Council
This study investigates NiMoO4 as a catalyst for the oxygen evolution reaction, showing its phase transformation under applied bias and the leaching of molybdenum from the catalyst. Molybdenum leaching increases the number of active sites on the catalyst, leading to higher current densities. Different NiMoO4 nanostructures influence the stability of the catalyst in alkaline media.
Water electrolysis powered by renewable energies is a promising technology to produce sustainable fossil free fuels. The development and evaluation of effective catalysts are here imperative; however, due to the inclusion of elements with different redox properties and reactivity, these materials undergo dynamical changes and phase transformations during the reaction conditions. NiMoO4 is currently investigated among other metal oxides as a promising noble metal free catalyst for the oxygen evolution reaction. Here we show that at applied bias, NiMoO4 center dot H2O transforms into gamma-NiOOH. Time resolved operando Raman spectroscopy is utilized to follow the potential dependent phase transformation and is collaborated with elemental analysis of the electrolyte, confirming that molybdenum leaches out from the as-synthesized NiMoO4 center dot H2O. Molybdenum leaching increases the surface coverage of exposed nickel sites, and this in combination with the formation of gamma-NiOOH enlarges the amount of active sites of the catalyst, leading to high current densities. Additionally, we discovered different NiMoO4 nanostructures, nanoflowers, and nanorods, for which the relative ratio can be influenced by the heating ramp during the synthesis. With selective molybdenum etching we were able to assign the varying X-ray diffraction (XRD) pattern as well as Raman vibrations unambiguously to the two nanostructures, which were revealed to exhibit different stabilities in alkaline media by time-resolved in situ and operando Raman spectroscopy. We advocate that a similar approach can beneficially be applied to many other catalysts, unveiling their structural integrity, characterize the dynamic surface reformulation, and resolve any ambiguities in interpretations of the active catalyst phase.
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