Simultaneous interfacial chemistry and inner Helmholtz plane regulation for superior alkaline hydrogen evolution

Bao, Zhenan; Zhang, Lishang; Tan, Qiuyang; Wang, Jinsong; Liu, Jia; Wan, Houzhao; Miao, Ling; Jian-jun, Jiang

doi:10.1039/d0ee02020f

Cited by 96 publications

(78 citation statements)

References 45 publications

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“…38 and 39 ). Thus, the electron mobility of the 1T phase -MoS 2 @NiS 2 catalysts was more favorable for the efficient charge transfer, which agrees consistent with the EIS test results 58 . Moreover, the PDOS results imply that the NiS 2 interface hybrid generates some new interface electronic states in 1T phase -MoS 2 (Supplementary Fig.…”

Section: Resultssupporting

confidence: 88%

Interfacial electronic structure engineering on molybdenum sulfide for robust dual-pH hydrogen evolution

et al. 2021

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Molybdenum disulfide, as an electronic highly-adjustable catalysts material, tuning its electronic structure is crucial to enhance its intrinsic hydrogen evolution reaction (HER) activity. Nevertheless, there are yet huge challenges to the understanding and regulation of the surface electronic structure of molybdenum disulfide-based catalysts. Here we address these challenges by tuning its electronic structure of phase modulation synergistic with interfacial chemistry and defects from phosphorus or sulfur implantation, and we then successfully design and synthesize electrocatalysts with the multi-heterojunction interfaces (e.g., 1T0.81-MoS2@Ni2P), demonstrating superior HER activities and good stabilities with a small overpotentials of 38.9 and 95 mV at 10 mA/cm2, a low Tafel slopes of 41 and 42 mV/dec in acidic as well as alkaline surroundings, outperforming commercial Pt/C catalyst and other reported Mo-based catalysts. Theoretical calculation verified that the incorporation of metallic-phase and intrinsic HER-active Ni-based materials into molybdenum disulfide could effectively regulate its electronic structure for making the bandgap narrower. Additionally, X-ray absorption spectroscopy indicate that reduced nickel possesses empty orbitals, which is helpful for additional H binding ability. All these factors can decrease Mo-H bond strength, greatly improving the HER catalytic activity of these materials.

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Section: Resultssupporting

confidence: 88%

Interfacial electronic structure engineering on molybdenum sulfide for robust dual-pH hydrogen evolution

et al. 2021

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“…For Ni3N, it requires a high energy barrier of 0.33 eV for water dissociation, leading to a sluggish kinetics for the Volmer step which provides H* intermediate. It has been reported that metallic Ni possesses active sites for hydroxyl adsorption and serves as the promoter for water dissociation[64]. Our calculations have confirmed the enhanced water adsorption on Ni3N/Ni.…”

supporting

confidence: 82%

“…As a result, the V-Ni3N/Ni shows an appropriated energy of 0.14 eV for water dissociation. The adsorption energy of hydrogen (GH*) has been widely employed as a descriptor for predicting the activity of HER electrocatalysts[14,28,43,64]. Upon comparison, Ni3N and V-Ni3N exhibit a negative GH* of −0.33 and −0.24 eV, indicating the strong adsorption for H* that hinders the desorption of H2 product.…”

mentioning

confidence: 99%

V-doped Ni3N/Ni heterostructure with engineered interfaces as a bifunctional hydrogen electrocatalyst in alkaline solution: Simultaneously improving water dissociation and hydrogen adsorption

et al. 2021

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Alkali-water electrolyzers and hydroxide exchange membrane fuel cells are emerging as promising technologies to realize hydrogen economy. Developing cost-effective electrode materials with high activities towards corresponding hydrogen evolution (HER) and oxidation (HOR) reactions plays a crucial role in commercial hydrogen production and utilization. Herein, we fabricated a V-doped Ni 3 N/Ni heterostructure (V-Ni 3 N/Ni) through a controlled nitridation treatment on a V-incorporated nickel hydroxide precursor. The resultant catalyst exhibits comparable catalytic activity and durability to commercial Pt/C in terms of both HER (a low overpotential of 44 mV at the current density of 10 mA•cm −2 ) and HOR (a high current density of 1.54 mA•cm −2 at 0.1 V versus reversible hydrogen electrode) under alkaline conditions. The superior activity of V-Ni 3 N/Ni grown on different substrates further implies its intrinsic performance. Density functional theory (DFT) calculations reveal that the coupled metallic Ni and doped V can promote the water adsorption, accelerate the Volmer step of alkaline HER, as well as optimize the adsorption and desorption of hydrogen intermediate (H * ) to reach a balanced ∆G H* value.

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“…Thus, the electron mobility of the 1T phase -MoS 2 @NiS 2 catalysts was more favorable for the e cient charge transfer, which agrees consistent with the EIS test results. 45 Moreover, the PDOS results imply that the NiS 2 interface hybrid generates some new interface electronic states in 1T phase -MoS 2 (Supplementary Fig. 15c However, H* can be absorbed not only by the 1T phase -MoS 2 @NiS 2 surface.…”

Section: Introductionmentioning

confidence: 95%

Interfacial Electronic Structure Engineering on Molybdenum Sulfide for Robust Dual-pH Hydrogen Evolution

Liu

Wang

et al. 2021

Preprint

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Molybdenum disulfide, as an electronic highly-adjustable catalysts material, tuning its electronic structure is crucial to enhance its intrinsic hydrogen evolution reaction (HER) activity. Nevertheless, there are yet huge challenges to the understanding and regulation of the surface electronic structure of molybdenum disulfide-based catalysts. Here we address these challenges by tuning its electronic structure of phase modulation synergistic with interfacial chemistry and defects from phosphorus or sulfur implantation, and we then successfully design and synthesize electrocatalysts with the multi-heterojunction interfaces (e.g., 1T0.81-MoS2@Ni2P), demonstrating superior HER activities and good stabilities with a small overpotentials of 38.9 and 98.5 mV at 10 mA/cm2, a low Tafel slopes of 41 and 42 mV/dec in acidic as well as alkaline surroundings, outperforming commercial Pt/C catalyst and other reported Mo-based catalysts. Theoretical calculation verified that the incorporation of metallic-phase and intrinsic HER-active Ni-based materials into molybdenum disulfide could effectively regulate its electronic structure for making the bandgap narrower. Additionally, reduced nickel possesses empty orbitals, which is helpful for additional H binding ability. All these factors can decrease Mo-H bond strength, greatly improving the HER catalytic activity of these materials.

show abstract

Simultaneous interfacial chemistry and inner Helmholtz plane regulation for superior alkaline hydrogen evolution

Abstract: Developing highly efficient and durable alkaline hydrogen evolution reaction (HER) electrocatalysts composed of earth-abundant materials is crucial for large-scale electrochemical hydrogen production. Herein, interfacial chemistry engineering is employed to decoupling...

Cited by 96 publications

References 45 publications

Interfacial electronic structure engineering on molybdenum sulfide for robust dual-pH hydrogen evolution

Interfacial electronic structure engineering on molybdenum sulfide for robust dual-pH hydrogen evolution

V-doped Ni3N/Ni heterostructure with engineered interfaces as a bifunctional hydrogen electrocatalyst in alkaline solution: Simultaneously improving water dissociation and hydrogen adsorption

Interfacial Electronic Structure Engineering on Molybdenum Sulfide for Robust Dual-pH Hydrogen Evolution

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