Differentiated Oxygen Evolution Behavior in MOF-Derived Oxide Nanomaterials Induced by Phase Transition

Li, Zhong; Wang, Xian; Guo, Yuanyuan; Ding, Jixiang; Huang, Qi; Li, Tingting; Hu, Yue; Qian, Jinjie; Huang, Shaoming

doi:10.1021/acsami.1c17229

Cited by 18 publications

(16 citation statements)

References 42 publications

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“…Besides, the peaks at 710.7 and 723.2 eV belonged to Fe(II). [ 47 ] The Fe 2p XPS analysis recorded on Fe(II)Cu(II)Fe(III)‐LDH verified the presence of Fe(II), in accordance with the colorimetric method. However, the XPS signals of Cu(II)Fe(III)‐LDH could be only disintegrated into the peaks at 712.8 and 725.3 eV for Fe(III).…”

Section: Resultsmentioning

confidence: 57%

Engineering Reductive Iron on a Layered Double Hydroxide Electrocatalyst for Facilitating Nitrogen Reduction Reaction

Kong

et al. 2022

Adv Materials Inter

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new catalysts to decrease the utilization of noble metal while simultaneously maintaining efficient nitrogen fixation performance becomes an important tendency in this field. [15][16][17][18][19] Chemists have suggested that lowvalence metal species with electron-rich characteristics play an essential role in catalytic process. [20] For instance, Ti (III), [21] Fe (II), [22] Cu (I), [23] Co (II), [24] Mn (III), [25] Ni (I), [26] and Zn (I) [27] act as catalytic centers or impetuses to facilitate the kinetics of multifarious thermodynamically unfavorable processes, including water splitting and nitrogen reduction. Among these low-valence nonprecious 3d transition metals (3d TMs), Fe desires particular attention. [28,29] As one of the cheapest and most abundant metals on the earth, Fe also exists in biological nitrogenases for natural N 2 fixation. [30] The Fe compounds have been widely utilized as catalysts for artificial N 2 fixation in the Haber-Bosch and electrochemical reactions, [31] endowing Fe-based catalysts with immense potential for electrocatalytic NRR under ambient conditions.Recently, layered double hydroxides (LDHs), one kind of 2D nanomaterials, have emerged as promising candidates of NRR electrocatalysts due to their adjustability of morphology, electronic structure, and composition. [32,33] However, the poor conductivity and weak nitrogen activation ability of LDHs handicap their electrocatalytic activities in ammonia synthesis. Numerous research focused on doping a transition metal electrocatalyst by heteroatoms, such as boron, phosphorus, or copper, which could generate defects or adjust electronic structure to improve the NRR activity. [34][35][36] Previous work have also proved that the unsaturated metal sites with electron-rich properties could boost nitrogen absorption, lower the reaction energy barrier, thus leading to an high NH 3 yield as well as FE. [37] According to Lewis acid-base theory, the dinitrogen molecule is a soft base that inclines to react with soft acid. Theoretical and experimental results demonstrated that low-valence 3d TMs could serve as Lewis acid sites. It will be in favor of the adsorption and activation of nitrogen, thereby promoting the catalytic performance. [38,39] Nevertheless, there lacks of attempts on Fe-based LDHs catalysts engineered low-valence metals, inspiring in-depth study.Herein, ferrous iron replacing copper layered double hydroxide (Fe(II)Cu(II)Fe(III)-LDH) was successfully synthesized by a modified solvothermal method. In neutral media, the catalyst reached Ammonia is an indispensable chemical, of which the industrial production is still dominated by Haber-Bosch process operated at harsh conditions. The ecofriendly electrocatalytic N 2 reduction reaction (NRR) emerges as an alternative, however, such technique currently suffers from tough dynamics on account of difficulties in the adsorption or protonation of N 2 on catalysts. To eliminate the obstacle, a simple and valid strategy of ferrous iron replacing copper is proposed to regulate the electron...

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Section: Resultsmentioning

confidence: 57%

Engineering Reductive Iron on a Layered Double Hydroxide Electrocatalyst for Facilitating Nitrogen Reduction Reaction

Kong

et al. 2022

Adv Materials Inter

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“…Metal organic frameworks (MOFs) are considered as a major appeal for electrochemical applications because of their high surface area, porosity, and tuneable chemical composition. − However, MOFs are limited in their use as electrodes because of their poor intrinsic conductivity. Therefore, MOFs are more commonly used as precursors for the preparation of advanced electrocatalysts through carbonization at high temperatures. − By pyrolyzing the organic ligands in the MOF, a graphitized/amorphous carbon matrix can be formed, which could act as a possible electron flow pathway and thus increase the electrochemical activity for both OER and HER .…”

Section: Introductionmentioning

confidence: 99%

MOF-Derived Porous Fe₃O₄/RuO₂-C Composite for Efficient Alkaline Overall Water Splitting

Shekhawat

Samanta

Barman

2022

ACS Appl. Energy Mater.

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Development of highly active, durable, bifunctional electrocatalysts for overall water splitting is of great importance to enhance the use of hydrogen energy. Herein, we synthesize a porous and interfaces-rich Fe3O4/RuO2-C composite from the Metal organic frameworks (MOF) material for overall water splitting in alkaline media. The Fe3O4/RuO2-C catalyst showed superior oxygen evolution reaction (OER) with high faradic efficacy. It requires 268 mV overpotential to achieve the current density of 20 mA/cm2. The catalyst also exhibited good hydrogen evolution reaction (HER) with a current density of 10 mA/cm2 at an overpotential of 94 mV. The stability test confirmed a remarkable long-term OER and HER stability of this catalyst in alkaline media. In addition, the Fe3O4/RuO2-C catalyst was also used as cathode and anode material for overall water splitting. It showed superior activity and stability in alkaline media with 10 mA/cm2 current density at 1.595 V cell potential. The excellent electrocatalytic activity of the Fe3O4/RuO2-C catalyst can be attributed to its porous structure, synergistic interaction between the components, the presence of hetero-interfaces, high electrochemical surface area etc. This work may provide an opportunity to design a bifunctional electrocatalyst for the development of anion exchange membrane water electrolyzers (AEMWEs).

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“…Two-dimensional (2D) nanomaterials, such as graphene, graphitic carbon nitride, black phosphorus, metal oxides/hydroxides/transition-metal dichalcogenides, and MoS 2 , have been attracting increasing research interest on account of their distinctive physicochemical properties. − Their unique characteristics, such as an extended lateral surface, a large specific surface area, and a high surface-to-volume atom ratio as well as high conductivity and mechanical strength, make them applicable to a variety of advanced research fields with great promise, including electronics, biosensors, and energy storage and conversion devices, especially in electrochemical catalysis. − Particularly, 2D structured electrocatalytic metal–organic framework (MOF) nanosheets may possess a large surface area, abundant exposed surface atoms (coordinatively unsaturated metal sites and/or structural defects), and rapid electron and mass transport and thus have high potential as preeminent electrocatalysts for the oxygen evolution reaction (OER). − However, the simple and effective synthesis of 2D MOF nanosheets still remains a great problem because the growth of MOF crystals should be confined within a several-nanometer in thickness without affecting the lateral growth direction.…”

Section: Introductionmentioning

confidence: 99%

Ligand-Assisted Controllable Growth of Self-Supporting Ultrathin Two-Dimensional Metal–Organic Framework Nanosheet Electrodes for an Efficient Oxygen Evolution Reaction

Wang

Fan

et al. 2022

Inorg. Chem.

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Rational design of metal–organic frameworks (MOFs) into ultrathin two-dimensional (2D) nanosheets with controllable thickness is significantly attractive but is also a significant challenge. Herein, the authors report, for the first time, the synthesis of ultrathin 2D nickel-based MOF nanosheets with a thickness of only about 2 nm via a ligand-assisted controllable growth strategy, which cannot be acquired from the exfoliation of their bulky counterparts or the conventional hydrothermal method. The correlation between 2D nanosheets and crystal growth preference was demonstrated through a judicious choice of a specific [Ni(BIP)(p-BDC)(H2O)2] n framework (BIP = (3,5-bis(1-imidazoly)pyridine), p-H2BDC = terephthalic acid) to underlie the geometry of the resultant morphology. Under the modulation by the dosage of terephthalic acid through a corrosion–dissolution–coordination process, the nanosheets of Ni-MOFs with a controllable thickness can be tuned to 50 and 100 nm. Ultrathin 2D Ni-MOF nanosheet-derived N-doped Ni@carbon exhibits a satisfactory electrocatalytic performance with a small overpotential of 170 mV to achieve a current density of 10 mA cm–2, much outperforming the bulk Ni-MOF and the most reported non-noble-metal oxygen evolution reaction electrocatalysts to date. It is believed that this ligand-assisted controllable growth strategy represents a novel and simple path to prepare high-performance MOF-based electrocatalysts for wide applications.

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Differentiated Oxygen Evolution Behavior in MOF-Derived Oxide Nanomaterials Induced by Phase Transition

Cited by 18 publications

References 42 publications

Engineering Reductive Iron on a Layered Double Hydroxide Electrocatalyst for Facilitating Nitrogen Reduction Reaction

Engineering Reductive Iron on a Layered Double Hydroxide Electrocatalyst for Facilitating Nitrogen Reduction Reaction

MOF-Derived Porous Fe₃O₄/RuO₂-C Composite for Efficient Alkaline Overall Water Splitting

Ligand-Assisted Controllable Growth of Self-Supporting Ultrathin Two-Dimensional Metal–Organic Framework Nanosheet Electrodes for an Efficient Oxygen Evolution Reaction

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Differentiated Oxygen Evolution Behavior in MOF-Derived Oxide Nanomaterials Induced by Phase Transition

Cited by 18 publications

References 42 publications

Engineering Reductive Iron on a Layered Double Hydroxide Electrocatalyst for Facilitating Nitrogen Reduction Reaction

Engineering Reductive Iron on a Layered Double Hydroxide Electrocatalyst for Facilitating Nitrogen Reduction Reaction

MOF-Derived Porous Fe3O4/RuO2-C Composite for Efficient Alkaline Overall Water Splitting

Ligand-Assisted Controllable Growth of Self-Supporting Ultrathin Two-Dimensional Metal–Organic Framework Nanosheet Electrodes for an Efficient Oxygen Evolution Reaction

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Product

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MOF-Derived Porous Fe₃O₄/RuO₂-C Composite for Efficient Alkaline Overall Water Splitting