Assessing the impacts of dynamic soft-templates innate to switchable ionic liquids on nanoparticulate green rust crystalline structures

Zheng, Jian; Yu, Xiao‐Ying; Nguyen, Manh‐Thuong; Lao, David; Zhu, Yulong; Wang, Feng; Heldebrant, David J.

doi:10.1039/c9cc04581c

Cited by 7 publications

(4 citation statements)

References 39 publications

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“…Besides, the new catalytic intermediate (π → π*) was found after OER reaction (Figure S12f, Supporting Information), indicating that there is π‐π stacking interaction. [ 62 ] The formation of π → π* could be attributed to the change of local electronic structure by electron‐withdrawing functional groups. [ 63 ] In addition, XRD diffraction (Figure S13, Supporting Information) after anode durability tests showed that no additional crystallization signals were detected, indicating that the M–OOH in the transition state is amorphous.…”

Section: Resultsmentioning

confidence: 99%

3D‐Stretched Film Ni₃S₂ Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting

Chen

Jiang

et al. 2021

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Transition metal sulfide (TMSs) has been one of the most promi sing candidate materials to replace noble metals for OWS because of advantages such as costeffectiveness, abundance, facile fabrication, among others. [4][5][6] How ever, the poor conductivity and stability of TMSs based electrocatalysts hinder their practical application in largescale sustain able hydrogen production.Composite engineering is an excellent strategy to raise the catalytic performance of TMSs further, [7,8] and the composite of TMSs and carbon materials has attracted much attention due to their superior sta bility and conductivity. Carbon materials with macrocyclic frameworks, graphite and graphitelike structures have been widely studied. [2,9,10] Because of the chem ical stability, thermal stability and highly adjustable photoelectric properties, as carriers of catalyst, this kind of carbon material have been used for electrochemical applications such as OWS, oxygen evolution reaction (OER), carbon dioxide reduction, and hydrogen evolution reaction (HER). [11,12] The study also shows that the macrocyclic carbon framework material enhances the crystallization ability of ZIF 8, [13] which solves the problem of low crystallinity of metal organic frameworks prepared by traditional benzene derivatives (BZD). As a significant natural and synthetic compound with a macrocyclic skeleton structure, anthraquinone derivatives For the first time, a new polymer electrode AQS/S is prepared by compositing Ni 3 S 2 nanosheets and macromolecular anthraquinone derivative (AQD) supported on nickel foam with flying colors. The AQS/S exhibits high crystalline structure and abundant S defects. Density of state calculation shows that AQD has stable internal bonding and easy external bonding with metals, conducive to the dispersion of metal reaction sites, ensuring excellent activity and high stability. Under 1.0 m KOH solution, ultralow overpotentials of 62 and 133 mV at 10 mA cm −2 on AQS/S for hydrogen evolution reaction and on activated AQS/S (A-AQS/S) for oxygen evolution reaction, respectively, are achieved. 100 h chronopotentiometry and the cyclic voltammetry tests show that catalysts have high durability. The AQS/S‖A-AQS/S two-electrode system is also found to have good electrocatalytic activity for 1.43 V to get 10 mA cm −2 in overall water splitting, better than the state-of-the-art 20% Pt/C‖RuO 2 combination.

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Section: Resultsmentioning

confidence: 99%

3D‐Stretched Film Ni₃S₂ Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting

Chen

Jiang

et al. 2021

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“…X-ray absorption spectroscopy (XAS) and density function theory (DFT) modelling were used to 4 determine possible products of GR synthesis in another related research effort (Figure S2). [5] Compared to previous results, in situ liquid ToF-SIMS provides valuable three-dimensional (3D) visualization of the chemical compounds formed via different synthesis paths in this effort.…”

Section: Andmentioning

confidence: 99%

“…[12][13][14][15] The results of TEM, Helium Ion Microscopy (HIM), and Mössbauer spectroscopy have been reported in our earlier papers. [4,5] The novel synthesis of nano GRs including nano GR-CO 3 * in the presence of CO 2 and methanol employs SWIL solvents .…”

Section: Andmentioning

confidence: 99%

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Revealing the Structural Evolution of Green Rust Synthesized in Ionic Liquids by In Situ Molecular Imaging

Shen

Yao

et al. 2020

Adv Materials Inter

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Ionic liquids are green solvents that have wide applications in material synthesis, catalysis, and separation. A model switchable ionic liquid (SWIL) consisting of 1,8-diazabicycloundec-7-ene (DBU) and 1-hexanol with carbon dioxide (CO 2 ) as the trigger gas was chosen to synthesize nanocrystalline green rust. Under anoxic conditions, by adding iron (II) acetate (Fe(C 2 H 3 O 2 ) 2 ) and methanol to the degassed SWIL, a nanoparticulate green rust with carbonate (nano GR) was synthesized. More importantly, the molecular structural change of the ionic liquid resulting in green rust crystallines has been first characterized using in situ liquid using time-of-flight secondary ion mass spectrometry (ToF-SIMS) coupled with the System for Analysis at the Liquid Vacuum Interface (SALVI), a vacuum compatible microfluidic reactor in this work. Dimers and ionic clusters consisting ferric and ferrous ions have been identified in liquid ToF-SIMS spectra. We used spectral principal component analysis to confirm that these ion pairs including dimers and cluster ions are different from non-ionic liquids. Our results show that liquid ToF-SIMS can be a useful tool to study complex liquids at the molecular level providing insights into predicative synthesis of nanomaterials using environmentally friendly green solvents and giving unique visualization of the evolving material interface due to nucleation.

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Deciphering Ligand Controlled Structural Evolution of Prussian Blue Analogues and Their Electrochemical Activation during Alkaline Water Oxidation

et al. 2022

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Herein, we have demonstrated the control over the structure of precatalysts to tune the properties of the active catalysts and their water oxidation activity. The reaction of K 3 [Fe(CN) 6 ] and Na 2 [Fe(CN) 5 (NO)] with Co(OH) 2 @CC produced precatalysts PC-1 and PC-2, respectively, with distinct structural and electronic features. The replacement of the À CN group with strong π-acceptor À NO modulates the electronic and atomic structure of PC-2. As a result, a facile electrochemical transformation of PC-2 into active catalyst FeÀ Co-(OH) 2 -Co(O)OH (AC-2) has been attained only in 15 CV cycles while 600 CV cycles are required for the electrochemical activation of PC-1 into AC-1. The X-ray absorption studies reveal the contraction of the CoÀ O and FeÀ O bond in AC-2 because of the presence of a higher amount of Co 3 + and Fe 3 + than in AC-1. The high valent Co 3 + and Fe 3 + modulates the electronic properties of AC-2 and assists in the OÀ O bond formation, leading to the improved water oxidation activity.

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Assessing the impacts of dynamic soft-templates innate to switchable ionic liquids on nanoparticulate green rust crystalline structures

Abstract: This experimental and theoretical study investigates how dynamic solvation environments in switchable ionic liquids regulate the composition of nanoparticulate green rust.

Cited by 7 publications

References 39 publications

3D‐Stretched Film Ni₃S₂ Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting

3D‐Stretched Film Ni₃S₂ Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting

Revealing the Structural Evolution of Green Rust Synthesized in Ionic Liquids by In Situ Molecular Imaging

Deciphering Ligand Controlled Structural Evolution of Prussian Blue Analogues and Their Electrochemical Activation during Alkaline Water Oxidation

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Assessing the impacts of dynamic soft-templates innate to switchable ionic liquids on nanoparticulate green rust crystalline structures

Abstract: This experimental and theoretical study investigates how dynamic solvation environments in switchable ionic liquids regulate the composition of nanoparticulate green rust.

Cited by 7 publications

References 39 publications

3D‐Stretched Film Ni3S2 Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting

3D‐Stretched Film Ni3S2 Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting

Revealing the Structural Evolution of Green Rust Synthesized in Ionic Liquids by In Situ Molecular Imaging

Deciphering Ligand Controlled Structural Evolution of Prussian Blue Analogues and Their Electrochemical Activation during Alkaline Water Oxidation

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Product

Resources

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3D‐Stretched Film Ni₃S₂ Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting

3D‐Stretched Film Ni₃S₂ Nanosheet/Macromolecule Anthraquinone Derivative Polymers for Electrocatalytic Overall Water Splitting