Conductive Polymer Intercalation Tunes Charge Transfer and Sorption–Desorption Properties of LDH Enabling Efficient Alkaline Water Oxidation

Jiang, Min; Cai, Rongming; Ren, Jiazheng; Chen, Jinxi; Qi, Limin; Long, Xia; Yang, Shihe

doi:10.1021/acsami.1c08429

Cited by 23 publications

(15 citation statements)

References 40 publications

(60 reference statements)

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“…EQCM‐D is a powerful in situ technique to track the real‐time changes occurring at the electrode surface with nanomole or gram sensitivity. [ 19 ] First, the adsorption–desorption of the Bi/Bi 2 O 3 –O v ‐coated quartz electrode was balanced in distilled water. Then, the KHCO 3 electrolyte was injected into the cell, and a sharp increase in the electrode was observed (Figure 3F), indicating that more species including HCO 3 − and CO 3 2− were adsorbed onto the Bi/Bi 2 O 3 –O v ‐coated electrode surface.…”

Section: Resultsmentioning

confidence: 99%

Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO₂ Reduction Reaction to Formate in Wide Operable Windows

et al. 2022

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Electrocatalytic reduction of CO2 to formate is believed to be one of the most promising technologies for producing clean fuels and valuable chemicals and for tackling the global warming problem. Herein, a novel synthesis strategy is presented for Bi‐based catalyst in CO2 reduction reaction (CO2RR). With the addition of acetic acid into the mother solution, heterostructured Bi/Bi2O3 nanoplates with abundant O vacancies (Bi/Bi2O3–Ov) and tailored coordination environments of the Bi ions are successfully synthesized, which exhibit excellent catalytic activity for CO2RR and high selectivity for formate generation with wide operable windows of pH (neutral to alkaline) and potential. In particular, the faradic efficiency (HCOOH) reaches ≥90% in a wide potential range of −0.7–−1.35 V versus reversible hydrogen electrode in neutral media, which dwarf most of the state‐of‐the‐art Bi‐based catalysts for CO2RR reported to date. Combined experimental and theoretical results show that the abundant O vacancies create frustrated Lewis pairs at the heterointerfaces with favorable adsorption characteristics, thereby facilitating the CO2RR process. This work opens up a new approach to promoting the catalytic activity and selectivity of Bi‐based materials for CO2RR by combining coordination and heterointerface engineering.

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Section: Resultsmentioning

confidence: 99%

Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO₂ Reduction Reaction to Formate in Wide Operable Windows

et al. 2022

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“…The measurements were performed using 200 mM NaCl and NaNO 3 aqueous solution with a flow rate of 300 μL min −1 at 25.0 °C. For the investigation of high-viscoelastic materials, the overtone order should be considered for the QCM-D measurement 39 . Therefore, we examined the overtone orders of 1 and 3, and the data were subsequently collected with an overtone order of 3 due to the large noise in the overtone order of 1.…”

Section: Methodsmentioning

confidence: 99%

Critical role of water structure around interlayer ions for ion storage in layered double hydroxides

et al. 2022

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Water-containing layered materials have found various applications such as water purification and energy storage. The highly structured water molecules around ions under the confinement between the layers determine the ion storage ability. Yet, the relationship between the configuration of interlayer ions and water structure in high ion storage layered materials is elusive. Herein, using layered double hydroxides, we demonstrate that the water structure is sensitive to the filling density of ions in the interlayer space and governs the ion storage. For ion storage of dilute nitrate ions, a 24% decrease in the filling density increases the nitrate storage capacity by 300%. Quartz crystal microbalance with dissipation monitoring studies, combined with multimodal ex situ experiments and theoretical calculations, reveal that the decreasing filling density effectively facilitates the 2D hydrogen-bond networking structure in water around interlayer nitrate ions along with minimal change in the layered structure, leading to the high storage capacity.

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“…Scanning electrochemical microscopy (SECM) is an in situ electrochemical technology to investigate the interface reactions in the fields of corrosion, , battery, catalysis, and so forth. In the study of corrosion, most studies focused on the mapping of reaction current at the metal/solution interface using typical redox couples, like ferrocenylmethanol (FeMeOH) and its cations (FeMeOH + ), with the planar metal electrodes as the substrate electrodes.…”

Section: Introductionmentioning

confidence: 99%

In Situ Studies of Hydrogen Evolution Kinetics on Pure Titanium Surface: The Effects of Pre-Reduction and Dissolved Oxygen

Meng

Zhang

et al. 2022

J. Phys. Chem. C

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The apparent cathodic current on the Ti surface in acidic solution is composed of three reactions: the reductions of the oxide film, H+, and O2. However, classical electrochemical tests usually provide coupled multi-reaction currents. Furthermore, dissolved oxygen makes in situ measurements significant due to the thermodynamic instability of Ti. In this study, the effects of pre-reduction and dissolved oxygen on hydrogen evolution reaction (HER) kinetics on the Ti surface were investigated by electrochemical and composition characterizations. The HER current was quantitatively separated from the apparent cathodic current from Ti, including the reductions of the oxide film, H+, and O2 by scanning electrochemical microscopy. The HER transfer coefficient and standard rate constant for Ti spontaneously passivated in air (P-Ti) are both 0.48/4.9 × 10–12 cm/s in aerated and O2-saturated solutions, while those for Ti activated by electro-reduction (EA-Ti) are 0.25/3.6 × 10–7 cm/s and 0.25/3.1 × 10–7 cm/s, respectively. The variable HER behavior is caused by the changes in the film electronic structure and composition except for the competition reduction between O2 and H+ as indicated by Mott–Schottky and surface-enhanced Raman spectroscopy. The deviation from 0.5 in the transfer coefficient implies that the Tafel slope and HER mechanism should be analyzed with caution.

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Conductive Polymer Intercalation Tunes Charge Transfer and Sorption–Desorption Properties of LDH Enabling Efficient Alkaline Water Oxidation

Cited by 23 publications

References 40 publications

Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO₂ Reduction Reaction to Formate in Wide Operable Windows

Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO₂ Reduction Reaction to Formate in Wide Operable Windows

Critical role of water structure around interlayer ions for ion storage in layered double hydroxides

In Situ Studies of Hydrogen Evolution Kinetics on Pure Titanium Surface: The Effects of Pre-Reduction and Dissolved Oxygen

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Conductive Polymer Intercalation Tunes Charge Transfer and Sorption–Desorption Properties of LDH Enabling Efficient Alkaline Water Oxidation

Cited by 23 publications

References 40 publications

Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO2 Reduction Reaction to Formate in Wide Operable Windows

Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO2 Reduction Reaction to Formate in Wide Operable Windows

Critical role of water structure around interlayer ions for ion storage in layered double hydroxides

In Situ Studies of Hydrogen Evolution Kinetics on Pure Titanium Surface: The Effects of Pre-Reduction and Dissolved Oxygen

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Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO₂ Reduction Reaction to Formate in Wide Operable Windows

Defect‐Rich Heterostructured Bi‐Based Catalysts for Efficient CO₂ Reduction Reaction to Formate in Wide Operable Windows