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Regulating Water Reduction Kinetics on MoP Electrocatalysts Through Se Doping for Accelerated Alkaline Hydrogen Production.

ABSTRACT: Owing to its low cost, high conductivity, and chemical stability, Molybdenum phosphide (MoP) has great potential for electrochemically catalyzing the hydrogen evolution reaction (HER). Unfortunately, the development of high-activity MoP still remains a grand challenge in alkali-electrolyzers due to its sluggish water reduction kinetics. Here, we demonstrate a novel strategy for regulating the HER kinetics of the MoP nanowire cathode through partially substituting P atoms with Se dopants. In alkaline solutions, the Se-doped MoP (Se-MoP) nanowire cathode exhibits excellent HER performance with a greatly-decreased overpotential of ∼61 mV at 10 mA cm^-2 and a Tafel slope of ∼63 mV dec^-1, outperforming currently reported MoP-based electrocatalysts. Experimental and theoretical investigations reveal that Se doping not only facilitates the water dissociation on MoP, but also optimize the hydrogen adsorption free energy, eventually speeding up the sluggish alkaline HER kinetics. Therefore, this work paves a new path for designing MoP-based electrocatalyst with high HER performance in alkaline electrolyzers.

SUBMITTER: Liu Z

PROVIDER: S-EPMC8517518 | biostudies-literature | 2021

REPOSITORIES: biostudies-literature

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Regulating Water Reduction Kinetics on MoP Electrocatalysts Through Se Doping for Accelerated Alkaline Hydrogen Production.

Liu Zhenpeng Z Bu Jun J Ma Wenxiu W Yang Bin B Zhang Lei L Zhong Hong H Li Shuangming S Zhang Jian J

Frontiers in chemistry 20211001

Owing to its low cost, high conductivity, and chemical stability, Molybdenum phosphide (MoP) has great potential for electrochemically catalyzing the hydrogen evolution reaction (HER). Unfortunately, the development of high-activity MoP still remains a grand challenge in alkali-electrolyzers due to its sluggish water reduction kinetics. Here, we demonstrate a novel strategy for regulating the HER kinetics of the MoP nanowire cathode through partially substituting P atoms with Se dopants. In alka ...[more]

PMID: 34660533

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Project description:Ag-based electrocatalysts are promising candidates to catalyze the sluggish oxygen reduction reaction (ORR) in anion exchange membrane fuel cells (AEMFC) and oxygen evolution reaction (OER) in unitized regenerative fuel cells. However, to be competitive with existing technologies, the AEMFC with Ag electrocatalyst must demonstrate superior performance and long-term durability. The latter implies that the catalyst must be stable, withstanding harsh oxidizing conditions. Moreover, since Ag is typically supported by carbon, the strict stability requirements extend to the whole Ag/C catalyst. In this work, Ag supported on Vulcan carbon (Ag/VC) and mesoporous carbon (Ag/MC) materials is synthesized, and their electrochemical stability is studied using a family of complementary techniques. We first employ an online scanning flow cell combined with inductively coupled plasma mass spectrometry (SFC-ICP-MS) to estimate the kinetic dissolution stability window of Ag. Strong correlations between voltammetric features and the dissolution processes are discovered. Very high silver dissolution during the OER renders this material impractical for regenerative fuel cell applications. To address Ag stability during AEMFC load cycles, accelerated stress tests (ASTs) in O2-saturated solutions are carried out in rotating disk electrode (RDE) and rotating ring-disk electrode (RRDE) setups. Besides tracking the ORR performance evolution, an ex situ long-term Ag dissolution study is performed. Moreover, morphological changes in the catalyst/support are tracked by identical-location transmission electron microscopy (RDE-IL-TEM). Voltammetry analysis before and after AST reveals a smaller change in ORR activity for Ag/MC, confirming its higher stability. RRDE results reveal a higher increase in the H2O2 yield for Ag/VC after the ASTs. The RDE-IL-TEM measurements demonstrate different degradation processes that can explain the changes in the long term performance. The results in this work point out that the stability of carbon-supported Ag catalysts depends strongly on the morphology of the Ag nanoparticles, which, in turn, can be tuned depending on the chosen carbon support and synthesis method.

Dataset Information

Regulating Water Reduction Kinetics on MoP Electrocatalysts Through Se Doping for Accelerated Alkaline Hydrogen Production.

Publications

Regulating Water Reduction Kinetics on MoP Electrocatalysts Through Se Doping for Accelerated Alkaline Hydrogen Production.

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