Reversible transition of an amorphous Cu-Al oxyfluoride into a highly active electrocatalyst for NO3− reduction to NH3

Guiet, Amandine; Simonin, Alexandre; Bemana, Hossein; Al‐Mahayni, Hasan; Li, Junnan; Kuruvinashetti, Kiran; Moury, Romain; Hémon-Ribaud, Annie; Chartrand, Daniel; Maisonneuve, Vincent; Lhoste, Jérôme; Seifitokaldani, Ali; Rochefort, Dominic; Kornienko, Nikolay

doi:10.1016/j.checat.2023.100595

Cited by 4 publications

(3 citation statements)

References 57 publications

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“…The literature proved possible to form this hydrated copper phase with multiple M 3+ cations through different synthesis techniques, such as solvothermal synthesis or direct precipitation, both using HF aq . 40 Starting from the LDH cationic ratio, Cu 3 Fe 1.5 Al 0.5 F 12 (H 2 O) 12 was explored as a possibility, with Fe 3+ and Al 3+ filling both 1c and 1f crystallographic sites at 75% and 25%, respectively, a possibility leading to a correct refinement taking into account the poor pattern intensity and crystallinity (Fig. 7a).…”

Section: Resultsmentioning

confidence: 99%

Intimately mixed copper, cobalt, and iron fluorides resulting from the insertion of fluorine into a LDH template

Rouag,

Porhiel,

Lemoine

et al. 2024

Dalton Trans.

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Section: Resultsmentioning

confidence: 99%

Intimately mixed copper, cobalt, and iron fluorides resulting from the insertion of fluorine into a LDH template

Rouag,

Porhiel,

Lemoine

et al. 2024

Dalton Trans.

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“…− in aqueous solutions, NO 3 RR provides a feasible method for NH 3 production with high efficiency and selectivity. [9][10][11][12][13][14][15] More importantly, NO 3 − has become one of the most widely existing water contaminations, arising from the cumulation of agricultural runoffs and the discharging of industrial sewage. [16][17][18][19] Therefore, electrochemical NO 3 RR is a versatile strategy for NH 3 synthesis along with pollutant removal from water bodies.…”

Section: Introductionmentioning

confidence: 99%

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Wang,

Hao,

Sun

et al. 2024

Advanced Materials

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Electrocatalytic nitrate reduction reaction (NO3RR) toward ammonia synthesis is recognized as a sustainable strategy to balance the global nitrogen cycle. However, it still remains a great challenge to achieve highly efficient ammonia production due to the complex proton‐coupled electron transfer process in NO3RR. Here, the controlled synthesis of RuMo alloy nanoflowers (NFs) with unconventional face‐centered cubic (fcc) phase and hexagonal close‐packed/fcc heterophase for highly efficient NO3RR is reported. Significantly, fcc RuMo NFs demonstrate high Faradaic efficiency of 95.2% and a large yield rate of 32.7 mg h−1 mgcat−1 toward ammonia production at 0 and −0.1 V (vs reversible hydrogen electrode), respectively. In situ characterizations and theoretical calculations have unraveled that fcc RuMo NFs possess the highest d‐band center with superior electroactivity, which originates from the strong Ru─Mo interactions and the high intrinsic activity of the unconventional fcc phase. The optimal electronic structures of fcc RuMo NFs supply strong adsorption of key intermediates with suppression of the competitive hydrogen evolution, which further determines the remarkable NO3RR performance. The successful demonstration of high‐performance zinc‐nitrate batteries with fcc RuMo NFs suggests their substantial application potential in electrochemical energy supply systems.

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“…The direct synthesis of oxyfluorides can be carried out by solid-state reaction, , metal dissolution in aqueous HF solution following by evaporation, solvothermal methods, , high pressure, and solid–gas reaction under fluorination agents. , Later, the mechanosynthesis route provided a simple and scalable alternative to directly prepare oxyfluorides with three or more 3d transition metals such as for Li 1.3 Mn 2+ 0.1 Co 2+ 0.1 Mn 3+ 0.1 Cr 3+ 0.1 Ti 0.1 Nb 0.2 O 1.7 F 0.3 and Li x (Co 0.2 Cu 0.2 Mg 0.2 Ni 0.2 Zn 0.2 )OF x . Otherwise, it is also possible to prepare some oxyfluorides by an indirect method, consisting of decomposition of a hydroxyl or hydrated fluorides under an inert atmosphere In this way, our group successfully synthesized various multimetallic oxyfluorides from M 2+ M 3+ F 5 (H 2 O) 2 , M 2+ M 3+ 2 F 8 (H 2 O) 2 or M 2+ 3 M 3+ 2 F 12 (H 2 O) 12 (M 2+ = Fe, Co, Ni, Mn, Cu; M 3+ = Al, V, Fe). − More recently, Co 0.5 Fe 0.5 O 0.5 F 1.5 has been obtained by thermal treatment under air of the hydrated fluoride precursor CoFeF 5 (H 2 O) 7 , initially prepared by the evaporation of a HF concentrated solution with Co 2+ and Fe 3+ metallic salts …”

Section: Introductionmentioning

confidence: 99%

Simple and Scalable Synthetic Route for Tunable Compositions of Multimetallic Oxyfluorides as Oxygen Evolution Reaction Catalysts

Terry,

Mathiot,

Guiet

et al. 2024

ACS Appl. Energy Mater.

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This work suggests a simple and scalable synthetic route to prepare multimetallic oxyfluorides, without requiring high temperature, high pressure, and a specific atmosphere (F 2 , N 2 , Ar, vacuum, etc.). For that, tunable compositions of Ni 2+ −Co 2+ −Fe 3+based oxyfluorides Co (1−x)/2 Ni x/2 Fe 0.5 O 0.5 F 1.5 have been prepared by calcination at moderate temperature under ambient air of Co 1−x Ni x FeF 5 (H 2 O) 7 precursors, prepared beforehand through coprecipitation at room temperature, across the whole range of the solid solution (0 ≤ x ≤ 1). Structural and thermal analyses confirmed the successful substitution for both hydrated fluoride precursors and oxyfluorides. Finally, we evaluated the electrocatalytic performance of the different Ni 2+ −Co 2+ −Fe 3+ oxyfluorides for oxygen evolution reaction. Among these, the trimetallic Co 0.25 Ni 0.25 Fe 0.5 O 0.5 F 1.5 exhibits the lowest overpotential (290 and 370 mV respectively at 10 and 100 mA cm −2 ) and the highest specific activity (3.9 A m −2 at 1.53 V vs RHE). These results highlight the need for compositional tunability to maximize performance.

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Reversible transition of an amorphous Cu-Al oxyfluoride into a highly active electrocatalyst for NO3− reduction to NH3

Cited by 4 publications

References 57 publications

Intimately mixed copper, cobalt, and iron fluorides resulting from the insertion of fluorine into a LDH template

Intimately mixed copper, cobalt, and iron fluorides resulting from the insertion of fluorine into a LDH template

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Simple and Scalable Synthetic Route for Tunable Compositions of Multimetallic Oxyfluorides as Oxygen Evolution Reaction Catalysts

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