Buffer anion effects on water oxidation catalysis: The case of Cu(III) complex

Chen, Qifa; Du, Hao-Yi; Zhang, Mingtian

doi:10.1016/s1872-2067(20)63729-9

Cited by 18 publications

(7 citation statements)

References 56 publications

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“…Molecular hydrogen (H 2 ) has been considered as the appropriate alternative to traditional fossil fuels. − Although a few approaches have been put forward, the electrolysis of water is assumed to be the greener and more efficient method for the scalable production of H 2 (hydrogen evolution reaction; HER). , However, the anodic oxygen evolution reaction (OER) is the crucial half-cell reaction of water electrolysis and is observed to be kinetically sluggish and associated with a large activation energy barrier. − Therefore, the OER plays a key role in the efficiency determination of an electrolyzer. , The OER kinetics strictly depends on the catalytic efficiency of the electrocatalyst used . Although efforts have been paid and new electrocatalysts based on metal oxides, hydroxides, and chalcogenides have been developed, noble metal-based nanostructures (IrO 2 , RuO 2 , etc.)…”

Section: Introductionmentioning

confidence: 99%

Impact of Iron in Three-Dimensional Co-MOF for Electrocatalytic Water Oxidation

2021

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The integration of iron (Fe) into a cobalt metal− organic framework (Co-MOF) tunes the electronic structure of the parent MOF as well as enhances their electrocatalytic characteristics. By using pyrazine and hydrofluoric acid, we have synthesized threedimensional Co-MOF [CoFC 4 H 4 N 2 (SO 4 ) 0.5 ], (1), and Fe-MOF [FeFC 4 H 4 N 2 (SO 4 ) 0.5 ], (2), through a single-step solvothermal method. Further, a series of bimetallic (having both Co and Fe metal centers) MOFs [Co 1−x Fe x FC 4 H 4 N 2 (SO 4 ) 0.5 ] were synthesized with variable concentrations of Fe, and their electrocatalytic performances were analyzed. The optimized amount of Fe significantly impacted the electrocatalytic behavior of the bimetallic MOF toward water oxidation. Particularly, the Co 0.75 Fe 0.25 -MOF needs only 239 and 257 mV of overpotential to deliver 10 and 50 mA/cm 2 current density, respectively, in alkaline electrolytic conditions. The Co 0.75 Fe 0.25 -MOF shows a lower Tafel slope (42 mV/ dec.) among other bimetallic MOFs and even the commercial RuO 2 , and it has excellent durability (with ∼8 mV increases in overpotential after 18 h of electrolysis) and 97.05% Faradaic efficiency, which further evident its catalytic excellency. These findings explore the intrinsic properties of MOF-based electrocatalysts and prospect the suitability for future water electrolysis.

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Section: Introductionmentioning

confidence: 99%

Impact of Iron in Three-Dimensional Co-MOF for Electrocatalytic Water Oxidation

2021

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“…Additionally, the morphology and composition of the used ITO electrodes are also detected by scanning electron microscopy (SEM, Figure S21) and X‐ray photoelectron spectroscopy (XPS, Figures S22 and S23), and remain the same as the fresh ITO. These observations imply that no active species, such as CuO x , [21] generates and adsorbs on the electrode surface. To further evaluate the anti‐oxidation ability of the ligand framework, the catalyst solution is analyzed by mass spectrometry (MS) after 3 h CPE over one turnover number, and the MS peaks are in line with those of the fresh catalyst solution (Figure S24).…”

Section: Resultsmentioning

confidence: 94%

Pivotal Role of Geometry Regulation on O−O Bond Formation Mechanism of Bimetallic Water Oxidation Catalysts

Chen,

Xian,

Zhang

et al. 2024

Angew Chem Int Ed

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In this study, we highlight the impact of catalyst geometry on the formation of O−O bonds in Cu2 and Fe2 catalysts. A series of Cu2 complexes with diverse linkers were designed as electrocatalysts for water oxidation. Interestingly, the catalytic performance of these Cu2 complexes is enhanced as their molecular skeleton become more rigid, which contrast with the behavior observed in our previous investigation with Fe2 analogs. Moreover, mechanistic studies reveal that the reactivity of the bridging O atom results in distinct pathways for O−O bond formation in Cu2 and Fe2 catalysts. In Cu2 systems, the coupling takes place between a terminal CuIII−OH and a bridging μ−O• radical. Whereas in Fe2 systems, it involves the coupling of two terminal Fe−oxo entities. Furthermore, an in‐depth structure‐activity analysis uncovers the spatial geometric prerequisites for the coupling of the terminal OH with the bridging μ−O• radical, ultimately leading to the O−O bond formation. Overall, this study emphasizes the critical role of precisely adjusting the spatial geometry of catalysts to align with the O−O bonding pathway.

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“…[63][64][65] The CPE current shown in Figure 3a increased from 0.1 mA/cm 2 to 0.6 mA/cm 2 for the first 20 mins, which indicated new catalytic-active species (Ni oxide or molecular active intermediate) were formed. [43][44][66][67][68][69][70][71][72][73] We carefully examined the stability of our TNC-Ni complex in phosphate buffer (0.1 M, pH 7.0) by a series of controlled experiments (Figures S12-20).…”

Section: Resultsmentioning

confidence: 99%

Trinuclear Nickel Catalyst for Water Oxidation: Intramolecular Proton-Coupled Electron Transfer Triggered Trimetallic Cooperative O–O Bond Formation

Chen

Xiao

Liao³

et al. 2023

CCS Chem

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Herein we reported a molecular trinuclear nickel catalyst (defined as TNC-Ni) for water oxidation. This TNC-Ni catalyst exhibits high catalytic performance and stability under neutral conditions (pH 7). Electrochemical studies disclose that the cooperation among the three nickel sites plays a vital role in both charge accumulation and O-O bond formation. This trinuclear nickel catalyst can accomplish the 4eoxidation of water by involving all three nickel sites and the O-O bond formation is trigged by the charge distribution process from 5 to 5 dp via proton-coupled electron transfer.

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Buffer anion effects on water oxidation catalysis: The case of Cu(III) complex

Cited by 18 publications

References 56 publications

Impact of Iron in Three-Dimensional Co-MOF for Electrocatalytic Water Oxidation

Impact of Iron in Three-Dimensional Co-MOF for Electrocatalytic Water Oxidation

Pivotal Role of Geometry Regulation on O−O Bond Formation Mechanism of Bimetallic Water Oxidation Catalysts

Trinuclear Nickel Catalyst for Water Oxidation: Intramolecular Proton-Coupled Electron Transfer Triggered Trimetallic Cooperative O–O Bond Formation

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