Structural transformation of metal–organic framework with constructed tetravalent nickel sites for efficient water oxidation

Wu, Weijian; Gao, Zi; Li, Qun; Wang, Zhiya; Liu, Shiyin; Wu, Hongbo; Zhao, Yuanchun; Jiao, Yalong; Zhao, Xiaojia

doi:10.1016/j.jechem.2022.07.040

Cited by 28 publications

(4 citation statements)

References 41 publications

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“…More significantly, there exist two broad bands between 470 and 530 cm −1 for the NH 3 -treated sample, which is indexed to the Ni(Fe)-O vibration of the Ni(Fe) oxides or hydroxides. 16,22,36,39,42 It further supports the surface migration of the Ni(Fe)-O species after the NH 3 reduction, which might also account for the following rapid surface reconstruction. The signals are then taken from 1.2 to 1.5 V vs. RHE (similarly hereinafter) with a step of 50 mV, and for each step it is recorded until reaching a steady state to obtain the time-resolved spectra.…”

Section: In Situ Investigation Of the Reconstructionmentioning

confidence: 57%

Regulation of bulk reconstruction of FeNiMoO₄via NH₃ treatment for high performance water oxidation

Wang

Deng

et al. 2023

Inorg. Chem. Front.

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Section: In Situ Investigation Of the Reconstructionmentioning

confidence: 57%

Regulation of bulk reconstruction of FeNiMoO₄via NH₃ treatment for high performance water oxidation

Wang

Deng

et al. 2023

Inorg. Chem. Front.

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“…Therefore, 33 % NiFeMOF/NFF has a lower transition potential to MOOH compared to NiMOF/NF. This disparity can be attributed to the strong synergistic interaction between Fe and Ni species, which effectively reduces the oxidation potential required to form highly valent active species, [32] thus improving the OER performance of 33 % NiFeMOF/NFF.…”

Section: Resultsmentioning

confidence: 99%

Self‐etching assembly of designed NiFeMOF nanosheet arrays as high‐efficient oxygen evolution electrocatalyst for water splitting

Zhang,

Liao,

Huang

et al. 2024

ChemSusChem

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2D metal‐organic frameworks (MOFs) have emerged as potential candidates for electrocatalytic oxygen evolution reactions (OER) due to their inherent properties like abundant coordination unsaturated active sites and efficient charge transfer. Herein, a versatile and massively synthesizable self‐etching assembly strategy wherein nickel‐iron foam (NFF) acts as a substrate and a metal ion source. Specifically, by etching the nickel‐iron foam (NFF) surface using ligands and solvents, Ni/Fe metal ions are activated and subsequently reacted under hydrothermal conditions, resulting in the formation of self‐supporting nanosheet arrays, eliminating the need for external metal salts. The obtained 33% NiFeMOF/NFF exhibits remarkable OER performance with ultra‐low overpotentials of 188/231 mV at 10/100 mA cm−2, respectively, outperforming most recently reported catalysts. Besides, the built 33% NiFeMOF/NFF(+) || Pt/C(−) electrolyzer presents low cell voltages of 1.55/1.83 V at 10/100 mA cm−2, superior to the benchmark RuO2(+) || Pt/C(−), implying good industrialization prospects. The excellent catalytic activity stems from the modulation of the electronic spin state of the Ni active site by the introduction of Fe, which facilitates the adsorption process of oxygen‐containing intermediates and thus enhances the OER activity. This innovative approach offers a promising pathway for commercial‐scale sustainable energy solutions.

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“…To further reveal the active center of UOR of Mo‐NT@NF, in situ electrochemical Raman characterization was performed for Mo1 and NM in the OER and UOR processes, respectively. From the evolution of the OER process of NM ( Figure a), it can be seen that NM converts to Ni(OH) 2 in alkaline electrolyte, and as the potential increased, the conversion of Ni(OH) 2 to Ni 3+ occurs when the voltage is increased to 1.32 V. [ 25 ] The characteristic peaks of NiOOH (475 and 558 cm −1 ) appear when the voltage is over 1.37 V. [ 26 ] The peak appearing at ≈983 cm −1 belongs to the oxidation peak of S, and the oxidation of S can protect the metal sites to some extent at high voltages. In contrast, the peak appearing at 1002 cm −1 in the UOR process of NM (Figure 5b) belongs to the CN stretching vibration of the absorbed urea molecule, and the intensity of this peak decreases with potential increased indicating the decomposition of urea.…”

Section: Resultsmentioning

confidence: 99%

Identifying And Unveiling the Role of Multivalent Metal States for Bidirectional UOR and HER Over Ni, Mo‐Trithiocyanuric Based Coordination Polymer

Liu

Zou

Cong

et al. 2023

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Urea oxidation reaction (UOR), an ideal alternative to oxygen evolution reaction (OER), has received increasing attention for realizing energy‐saving H2 production and relieving pollutant degradation. Normally, most studied Ni‐based UOR catalysts pre‐oxidate to NiOOH and then act as active sites. However, the unpredictable transformation of the catalyst's structure and its dissolution and leaching, may complicate the accuracy of mechanism studies and limit its further applications. Herein, a novel self‐supported bimetallic Mo‐Ni‐C3N3S3 coordination polymers (Mo‐NT@NF) with strong metal–ligand interactions and different H2O/urea adsorption energy are prepared, which realize a bidirectional UOR/hydrogen evolution reaction (HER) reaction pathway. A series of Mo‐NT@NF is prepared through a one‐step mild solvothermal method and their multivalent metal states and HER/UOR performance relationship is evaluated. Combining catalytic kinetics, in situ electrochemical spectroscopic characterization, and density‐functional theory (DFT) calculations, a bidirectional catalytic pathway is proposed by N, S‐anchored Mo5+ and reconstruction‐free Ni3+ sites for catalytic active center of HER and UOR, respectively. The effective anchoring of the metal sites and the fast transfer of the intermediate H* by N and S in the ligand C3N3S3H3 further contribute to the fast kinetic catalysis. Ultimately, the coupled HER||UOR system with Mo‐NT@NF as the electrodes can achieve energy‐efficient overall‐urea electrolysis for H2 production.

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Structural transformation of metal–organic framework with constructed tetravalent nickel sites for efficient water oxidation

Cited by 28 publications

References 41 publications

Regulation of bulk reconstruction of FeNiMoO₄via NH₃ treatment for high performance water oxidation

Regulation of bulk reconstruction of FeNiMoO₄via NH₃ treatment for high performance water oxidation

Self‐etching assembly of designed NiFeMOF nanosheet arrays as high‐efficient oxygen evolution electrocatalyst for water splitting

Identifying And Unveiling the Role of Multivalent Metal States for Bidirectional UOR and HER Over Ni, Mo‐Trithiocyanuric Based Coordination Polymer

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Structural transformation of metal–organic framework with constructed tetravalent nickel sites for efficient water oxidation

Cited by 28 publications

References 41 publications

Regulation of bulk reconstruction of FeNiMoO4via NH3 treatment for high performance water oxidation

Regulation of bulk reconstruction of FeNiMoO4via NH3 treatment for high performance water oxidation

Self‐etching assembly of designed NiFeMOF nanosheet arrays as high‐efficient oxygen evolution electrocatalyst for water splitting

Identifying And Unveiling the Role of Multivalent Metal States for Bidirectional UOR and HER Over Ni, Mo‐Trithiocyanuric Based Coordination Polymer

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Regulation of bulk reconstruction of FeNiMoO₄via NH₃ treatment for high performance water oxidation

Regulation of bulk reconstruction of FeNiMoO₄via NH₃ treatment for high performance water oxidation