Coadsorption of hydrazine (N2H4) and OH on NiZn surface: A DFT-based study

Agusta, Mohammad Kemal; Saputro, Adhitya Gandaryus; Ihsan, Ahmad; Krishna, Raihan; Fathurrahman, Fadjar; Dipojono, Hermawan Kresno; Diño, Wilson Agerico

doi:10.1016/j.susc.2019.121505

Cited by 5 publications

(4 citation statements)

References 55 publications

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“…Among nonprecious transition metals, Ni SACs are found to selectively convert CO 2 to CO with a high faradaic efficiency (FE). − Ni-based catalysts demonstrate excellent activity not only in electrochemical reactions but also in numerous non-electrochemical catalytic processes. − In contrast to Ni metal electrodes, Ni SACs do not suffer from CO poisoning thanks to the unique coordination environment that provides weaker CO binding . However, the nature of Ni SAC active sites in the aspect of its position has not been well understood yet .…”

Section: Introductionmentioning

confidence: 99%

Two-Electron Electrochemical Reduction of CO₂ on B-Doped Ni–N–C Catalysts: A First-Principles Study

et al. 2021

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We evaluate the electrocatalytic activity of graphene-supported NiN4 active center in facilitating two-electron CO2 electrochemical reduction into CO and HCOOH, as well as the competing hydrogen evolution reaction. NiN4 center is found to be more stable in zigzag-edge and armchair-edge proximity of graphene, confirming experimental evidence. In an attempt to reduce the CO2 reduction overpotential, we construct a neighboring-site environment of NiN4 center and BN substitutional defect. B-doped structures are found to be capable of reducing the CO2 reduction energy barrier through direct (HCOOH pathway) or indirect (CO pathway) participation in facilitating CO2 reduction-related key intermediates. In most Ni sites, the presence of adjacent BN site is also discovered to change the product selectivity from CO to HCOOH. Our result predicts that B-doped NiN4 sites on the interior side (NiN4BN-G) and on the armchair-edge side of tilted orientation (t-NiN4BN-AGNR) are HCOOH-selective. Although the rest of zigzag-edge and armchair-edge sites have a tendency to selectively produce CO and HCOOH, respectively, the undesirable hydrogen evolution reaction is found to be more dominant and therefore obscuring the potential. Our result demonstrates that the hydrogen evolution reaction is most likely to occur on top of a neighboring C atom instead of on the Ni center, in contrast to the commonly understood mechanism. To ultimately suppress the activity of the hydrogen evolution reaction, we predict that an effective electrocatalyst optimization cannot be realized by only selecting the best metal center and dopant pair but also by altering the neighbor’s electronic structure.

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Section: Introductionmentioning

confidence: 99%

Two-Electron Electrochemical Reduction of CO₂ on B-Doped Ni–N–C Catalysts: A First-Principles Study

et al. 2021

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“…Although hydrazine is thermodynamically unstable, its decomposition in air is negligible. , Acidic conditions promote its decomposition to NH 3 , H 2 , N 2 , and HN 3 , although it occurs in alkaline pH, too . According to DFT calculations, hydrazine coordinates to transition-metal surfaces through a nitrogen lone-pair. , However, these surfaces are expected to be oxidized, and the effect of oxidation on reaction selectivity (toward N 2 /NH 3 /NO x ) is hard to predict and could be opposite on real (e.g., nanostructured) surfaces. , Moreover, in an electrolyte environment the hydrogen bonding will also affect the adsorption preferences of hydrazine, − while higher temperatures could promote faster decomposition …”

Section: Metal Surfacesmentioning

confidence: 99%

Hydrazine Oxidation Electrocatalysis

Burshtein,

Yasman,

Muñoz-Moene

et al. 2024

ACS Catal.

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The electro-oxidation of hydrazine is important for direct hydrazine fuel cells and for fundamental understanding of electrocatalysis in the nitrogen cycle. In this Review, we discuss electrocatalysis of the hydrazine oxidation reaction (HzOR), spanning a vast range of metal surfaces, nanoparticles, atomically dispersed ions, organometallic macrocycles, and enzymes. Emphasis is given to structure−activity correlations and reactivity descriptors, including the formulation of the Zagal principle, an electrochemical corollary of the Sabatier principle. In addition, we identify overarching themes that span the different subfields of HzOR electrocatalysis, hoping to inspire cross-disciplinary research avenues.

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“…Agusta et al. investigated anti ‐ and cis ‐N 2 H 4 co‐adsorption on a Ni−Zn alloy with the adsorption energies increased in site preference; atop Ni far from Zn>atop Ni near Zn>atop Zn [87] . The theoretical measurements suggested that the interaction between N 2 H 4 molecules and OH − ions was a mixture of direct chemical and electrostatic modes.…”

Section: An Overview Of Hzor Electrocatalysts: From Noble Metals To Nimentioning

confidence: 99%

“…[84][85][86] Agusta et al investigated anti-and cis-N 2 H 4 coadsorption on a NiÀ Zn alloy with the adsorption energies increased in site preference; atop Ni far from Zn > atop Ni near Zn > atop Zn. [87] The theoretical measurements suggested that the interaction between N 2 H 4 molecules and OH À ions was a mixture of direct chemical and electrostatic modes. The interaction of N 2 H 4 molecule with the Ni surfaces can be realized through a lone-pair of electrons centered on N atoms, constructing either monodentate or bidentate bonding with the catalytic surface.…”

Section: An Overview Of Hzor Electrocatalysts: From Noble Metals To Nimentioning

confidence: 99%

Development Trends on Nickel‐Based Electrocatalysts for Direct Hydrazine Fuel Cells

2020

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Low temperature hydrazine fuel cells have been advocated as potential energy carriers by virtue of their exceptional power densities and carbon free containing byproducts. However, the large‐scale application of these renewable energy systems has been extremely inhibited by the insufficient performance and high cost of the state‐of‐art platinum (Pt) catalysts. To pursue better activity, electrocatalysts must demonstrate low operating overpotentials and high tolerances to poisoning species, which are critical factors for increasing the energy conversion efficiency. Despite the tremendous progress of Pt‐based catalysts, controlling sluggish kinetics on microscopic surfaces is still a serious issue because the accumulation of reaction product slugs onto surface may impede the liquid fuel transport to catalytic sites, resulting in a low activity. Thus, the development of earth abundant electrocatalysts with an improved activity is unambiguously a principal requirement. In this review, recent trends in the rational design and synthesis of Ni‐based electrocatalysts with various compositions for hydrazine oxidation reaction (HzOR) are summarized. In particular, development of multicomponent compounds and employment of Ni‐based materials for HzOR are demonstrated to be effective approaches from tuning the electrochemical performance of Ni‐based catalyst materials. Moreover, some potential challenges and prospects are deliberated to further advance the improvement of Ni‐based materials for effective HzOR.

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Coadsorption of hydrazine (N2H4) and OH on NiZn surface: A DFT-based study

Cited by 5 publications

References 55 publications

Two-Electron Electrochemical Reduction of CO₂ on B-Doped Ni–N–C Catalysts: A First-Principles Study

Two-Electron Electrochemical Reduction of CO₂ on B-Doped Ni–N–C Catalysts: A First-Principles Study

Hydrazine Oxidation Electrocatalysis

Development Trends on Nickel‐Based Electrocatalysts for Direct Hydrazine Fuel Cells

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Coadsorption of hydrazine (N2H4) and OH on NiZn surface: A DFT-based study

Cited by 5 publications

References 55 publications

Two-Electron Electrochemical Reduction of CO2 on B-Doped Ni–N–C Catalysts: A First-Principles Study

Two-Electron Electrochemical Reduction of CO2 on B-Doped Ni–N–C Catalysts: A First-Principles Study

Hydrazine Oxidation Electrocatalysis

Development Trends on Nickel‐Based Electrocatalysts for Direct Hydrazine Fuel Cells

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Product

Resources

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Two-Electron Electrochemical Reduction of CO₂ on B-Doped Ni–N–C Catalysts: A First-Principles Study

Two-Electron Electrochemical Reduction of CO₂ on B-Doped Ni–N–C Catalysts: A First-Principles Study