Atomic uranium modified graphdiyne as catalytic material for hydrogen evolution reaction: An interfacial descriptor led mechanistic study

Bacha, Raza Ullah Shah; Cai, Hong-Xue; Wang, Jianqiang; Pan, Qing‐Jiang

doi:10.1016/j.ijhydene.2020.06.153

Cited by 9 publications

(9 citation statements)

References 84 publications

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“…carried out DFT calculations on U/GDY ACs for catalytic HER (Figure 9a). [56] The U single atoms prefer to reside in the mid‐corner sites of the 18‐C ring ofGDY and form eight coordination with the acetylenic carbons with the organometallic bond lengths of U−C in the range of 2.34–2.44 Å (Figure 9b). Due to the charge transfer between the sp orbitals of acetylenic carbons and 5 f orbitals of U, the valence state of U on GDY is +1.47≈+1.83.…”

Section: Coordination Engineering Of Gdy‐based Acs In Various Catalyt...mentioning

confidence: 99%

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Graphdiyne‐Based Single‐Atom Catalysts with Different Coordination Environments

Zhao

et al. 2023

Angew Chem Int Ed

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As a special carbon material, graphdiyne (GDY) features the superiorities of incomplete charge transfer effect on the atomic level, tunable electronic structure and anchoring metal atoms directly with organometallic coordination bonds M (metal)-C (alkynyl carbon in GDY), providing it an ideal platform to construct single-atom catalysts (ACs). The coordination environment of single atoms anchored on GDY plays a key role in their catalytic performance. The mini-review highlights state-of-the-art progress in the rational design of GDY-based ACs and their applications, and mainly reveals the relationship between the coordination engineering of the GDY-based ACs and corresponding catalytic performance. Finally, some prospects concerning the future development of GDY-based ACs in energy conversion are also discussed.

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Section: Coordination Engineering Of Gdy‐based Acs In Various Catalyt...mentioning

confidence: 99%

“…b) Optimized structures of sites labeled GDY‐U with chemosorbed H on uranium and four labeled acetylenic sites and GDY. c) Possible reaction pathways and corresponding zero potential free [56] . Copyright 2020, Elsevier.…”

Section: Coordination Engineering Of Gdy‐based Acs In Various Catalyt...mentioning

confidence: 99%

Graphdiyne‐Based Single‐Atom Catalysts with Different Coordination Environments

Zhao

et al. 2023

Angew Chem Int Ed

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“…Based on the above-mentioned results and literature data, it is expected that the HER at the UTBrImPc− MWCNTs/GCE electrode follows the Volmer−Heyrovsky mechanism, where the Heyrovsky step is commonly considered a rate-determining step in acidic medium. 53,54 Here, the catalyst follows the adsorption and desorption process (eqs 4 and 5) to promote the electrochemical production of H 2 . First, the hydrogen atom adsorbs on the catalytic site (*U acts as the major active site) of the electrode surface via the Volmer reaction (eq 4).…”

Section: Mechanism Of the Her And Oer Activitymentioning

confidence: 99%

Uranium Phthalocyanine-Anchored Acid-Functionalized Multiwalled Carbon Nanotubes for Water Electrolysis

Giddaerappa,

Puttaningaiah,

Aralekallu

et al. 2023

ACS Appl. Nano Mater.

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One of the major challenges in the commercial production of hydrogen and oxygen from the electrochemical water splitting reaction is the nonavailability of potential and low-cost electrocatalysts for the enhancement of both the half-cell reactions. The bifunctional catalyst capable of demonstrating lower overpotentials for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) eliminates the usage of a membrane, simplifies the overall system design, reduces the cost, and enhances the electrochemical water splitting activity. Here, a bifunctional hybrid composite catalyst comprising an organic N4 macrocycle and acid-functionalized multiwalled carbon nanotubes (MWCNTs) is fabricated and tested for the water splitting reaction to produce H2 and O2. The uranium tetra[4-(2-{(E)-[(4-bromophenyl)imino]methyl}phenoxy)]phthalocyanine (UTBrImPc) is synthesized via a two-step process of imine and oxy-bridge linkage formation. The synthesized ligands and phthalocyanine macrocycle are characterized using various spectroscopic and analytical techniques. The glassy carbon electrode (GCE) and Ni foam are used as the conducting substrate for the fabrication of the UTBrImPc/MWCNT bifunctional electrode to generate H2 and O2. Surprisingly, the fabricated bifunctional hybrid catalyst on the GCE exhibited a lesser overpotential of 15 mV for the HER, which is close to that of the benchmark Pt/C catalyst. Furthermore, the Ni/UTBrImPc/MWCNT displayed a lower overpotential of 368 (±2) mV at a current density of 10 mA·cm–2 for the OER, which is close to the overpotential shown by the precious benchmark catalyst IrO2. In addition, the fabricated electrodes showed remarkable long-term stability for more than 20 h by a chronoamperometric method. The superior results for both the HER and OER at the composite organic hybrid catalyst may be due to the collusive effect of the acid-functionalized MWCNTs with UTBrImPc, which enhances the electronic conductivity and surface area. The developed state-of-the-art catalyst can be employed as a bifunctional catalyst in water electrolyzers.

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“…29,30 For example, uranium-modified graphdiyne exhibits hydrogen evolution reaction (HER) activity in theoretical calculations and the experimentally prepared U/Th-graphene hybrids show excellent electrocatalytic properties for both oxygen and hydrogen peroxide reduction. 31,32 Besides the comparatively large ionic radius, U has 5f orbitals to participate in covalent bonding for interactions. 33 It has been shown that N 2 molecules can be activated by uranium complexes mainly because the valence 5f-electrons of uranium are contributing to coordination.…”

Section: Introductionmentioning

confidence: 99%

“…39 However, the application of uranium in catalysis is still in its infancy compared with ordinary metal because of the presence of various oxidation states and complicated redox reactions. 31 Therefore, the search for efficient, simple, and eco-friendly U-catalysts for the conversion of N 2 to NH 3 under ambient conditions is essential.…”

Section: Introductionmentioning

confidence: 99%

N₂reduction in uranium-doped C₂N/C₃N₄monolayers: a DFT computational study

Sun¹,

Liu²,

Qu³

et al. 2023

New J. Chem.

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Atomic uranium modified graphdiyne as catalytic material for hydrogen evolution reaction: An interfacial descriptor led mechanistic study

Cited by 9 publications

References 84 publications

Graphdiyne‐Based Single‐Atom Catalysts with Different Coordination Environments

Graphdiyne‐Based Single‐Atom Catalysts with Different Coordination Environments

Uranium Phthalocyanine-Anchored Acid-Functionalized Multiwalled Carbon Nanotubes for Water Electrolysis

N₂reduction in uranium-doped C₂N/C₃N₄monolayers: a DFT computational study

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Atomic uranium modified graphdiyne as catalytic material for hydrogen evolution reaction: An interfacial descriptor led mechanistic study

Cited by 9 publications

References 84 publications

Graphdiyne‐Based Single‐Atom Catalysts with Different Coordination Environments

Graphdiyne‐Based Single‐Atom Catalysts with Different Coordination Environments

Uranium Phthalocyanine-Anchored Acid-Functionalized Multiwalled Carbon Nanotubes for Water Electrolysis

N2reduction in uranium-doped C2N/C3N4monolayers: a DFT computational study

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N₂reduction in uranium-doped C₂N/C₃N₄monolayers: a DFT computational study