Hierarchical anions at the electrode-electrolyte interface for synergized neutral water oxidation

Liu, Tao; Chen, Yuxin; Hao, Yaming; Wu, Jianxiang; Wang, Ran; Gu, Lian‐Quan; Yang, Xuejing; Yang, Qiang; Lian, Cheng; Liu, Honglai; Gong, Mali

doi:10.1016/j.chempr.2022.06.012

Cited by 29 publications

(29 citation statements)

References 42 publications

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“…247 In-situ surface-enhanced Raman spectroscopy could be developed to detect the subtle EDL structure, specifically the details of ion distribution and reactant adsorption on the electrode interface. 248,249 Other inspiring techniques include electrochemical scanning probe microscopy, 250,251 enhanced spectroscopy, 252 and their combinations.…”

Section: Discussionmentioning

confidence: 99%

“…In-situ liquid time-of-flight secondary ion mass spectrometry can discriminate the ion–solvent interactions and properties in confined membrane pores, through which reactant structure and transformation inside EMs may be precisely acquired . In-situ surface-enhanced Raman spectroscopy could be developed to detect the subtle EDL structure, specifically the details of ion distribution and reactant adsorption on the electrode interface. , Other inspiring techniques include electrochemical scanning probe microscopy, , enhanced spectroscopy, and their combinations.…”

Section: Discussionmentioning

confidence: 99%

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Inorganic Electrified Membrane: From Basic Science to Performance Translation

et al. 2023

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Decentralized water systems necessitate intensified, robust, and modular water treatment technologies for enhanced efficacy and resilience of the water purification process. Inorganic electrified membranes (IEMs) are gaining momentum in decentralized water systems by combining the versatility of electro-filtration processes with the favorable properties of inorganic materials, namely, strong mechanical strength, chemical stability, and hydrophilicity. This review quantitatively assesses three mainstream IEMs (i.e., Ti4O7, carbon, and metallic IEMs) from a fundamental perspective of the intrinsic electrochemical properties of the IEM materials and their translation into the IEM performances. We specifically (i) analyze the •OH production selectivity by Ti4O7 IEMs based on electrochemical thermodynamics and material science; (ii) differentiate degradation mechanisms of carbon IEMs in the context of various water matrices and propose strategies to address major concerns of avoiding membrane passivation and improving Faradaic efficiency of carbon IEMs; and (iii) highlight metallic IEMs doped with Ag or Pd, i.e., elucidate the combined sterilization mechanism by Ag-IEM via Ag+ dissolution and electro-phenomena, and unravel the unique hydrogenolysis ability of Pd-IEM for hydrodeoxygenation and persulfate electro-activation. We conclude by identifying the remaining obstacles of IEMs and present possible interdisciplinary approaches for IEM optimization.

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Inorganic Electrified Membrane: From Basic Science to Performance Translation

et al. 2023

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“…The ionic environment at the electrode‐electrolyte interface is another critical factor that influences on the neutral water oxidation performance [7] . In our previous study, the identified hierarchical anion structure created a more compact double layer with enhanced electric field that expedited the water oxidation kinetics on a Co‐based electrocatalyst [8] . However, the interplay of the surface oxygen intermediates determined by the intrinsic catalyst structure and the local ionic environment determined by the electrolyte composition still remains elusive [9] .…”

Section: Figurementioning

confidence: 99%

“…Despite the improved performance, the IrO x /Ni(OH) 2 still exhibited an overpotential of 421 mV at 20 mA cm −2 , with a much inferior activity to the acidic or alkaline media. We further adopted the ionic additives of borate, fluoride and their mixtures to tune the interfacial structures near the oxygen intermediates [8] . At 1.60 V vs. RHE, the IrO x /Ni(OH) 2 catalyst exhibited an outstanding current density of 96.8 mA cm −2 in the electrolyte with 1.5 M KF+0.4 M KB i , compared to 4.7 mA cm −2 in 0.5 M KHCO 3 , 19.3 mA cm −2 in 1.5 M KF and 23.9 mA cm −2 in 0.4 M KB i (Figure 1e and Figure S4).…”

Section: Figurementioning

confidence: 99%

Electrode/Electrolyte Synergy for Concerted Promotion of Electron and Proton Transfers toward Efficient Neutral Water Oxidation

et al. 2023

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Neutral water oxidation is a crucial half‐reaction for various electrochemical applications requiring pH‐benign conditions. However, its sluggish kinetics with limited proton and electron transfer rates greatly impacts the overall energy efficiency. In this work, we created an electrode/electrolyte synergy strategy for simultaneously enhancing the proton and electron transfers at the interface toward highly efficient neutral water oxidation. The charge transfer was accelerated between the iridium oxide and in situ formed nickel oxyhydroxide on the electrode end. The proton transfer was expedited by the compact borate environment that originated from hierarchical fluoride/borate anions on the electrolyte end. These concerted promotions facilitated the proton‐coupled electron transfer (PCET) events. Due to the electrode/electrolyte synergy, Ir−O and Ir−OO− intermediates could be directly detected by in situ Raman spectroscopy, and the rate‐limiting step of Ir−O oxidation was determined. This synergy strategy can extend the scope of optimizing electrocatalytic activities toward more electrode/electrolyte combinations.

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“…[7][8][9] Moreover, there is a strong pH effect on the OER reaction mechanism, which can be categorized into water oxidation under acidic or neutral conditions and hydroxide oxidation under highly alkaline conditions. 10,11 Therefore, it is important to customize the OER catalyst to response various application conditions. Specifically, RuO 2 and IrO 2 exhibit excellent OER activity in both acidic and alkaline electrolytes, but they are unstable at high overpotential and will be oxidized to form RuO 4 and IrO 3 and dissolved in electrolytes, especially in acidic electrolytes because the participation of lattice oxygen may lead to structural collapse to accelerate the dissolution of Ru/Ir.…”

Section: Introductionmentioning

confidence: 99%