Emerging on-chip microcells in electrocatalysis: functions of window and circuit

Wang, Jinbo; Qiu, Mengyi; Jiang, Yubin; Xia, Hang; An, Xiuyun; Wang, Shuangyin; He, Yongmin

doi:10.1039/d3ey00168g

Cited by 3 publications

(3 citation statements)

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“…The ESF gating onto the metallic TMD catalysts can also tune the distribution of the ions at the electrolyte-catalyst interface. 209 For example, Mai et al employed the metallic VSe 2 as the catalyst and investigated the distribution of the ions at the electrolyte−VSe 2 interface using four-electrode OCEM microcells (Figure 45a,b). 210 It is noteworthy that the adsorption of H atoms would result in the decreased resistance of TMD catalysts, consistent with the phenomenon observed in Pt nanowire catalysts.…”

Section: Modulation Of Ion Distributionmentioning

confidence: 99%

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Spatially Confined Microcells: A Path toward TMD Catalyst Design

Guo,

Ma,

Wang

et al. 2024

Chem. Rev.

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With the ability to maximize the exposure of nearly all active sites to reactions, two-dimensional transition metal dichalcogenide (TMD) has become a fascinating new class of materials for electrocatalysis. Recently, electrochemical microcells have been developed, and their unique spatial-confined capability enables understanding of catalytic behaviors at a single material level, significantly promoting this field. This Review provides an overview of the recent progress in microcell-based TMD electrocatalyst studies. We first introduced the structural characteristics of TMD materials and discussed their site engineering strategies for electrocatalysis. Later, we comprehensively described two distinct types of microcells: the window-confined on-chip electrochemical microcell (OCEM) and the droplet-confined scanning electrochemical cell microscopy (SECCM). Their setups, working principles, and instrumentation were elucidated in detail, respectively. Furthermore, we summarized recent advances of OCEM and SECCM obtained in TMD catalysts, such as active site identification and imaging, site monitoring, modulation of charge injection and transport, and electrostatic field gating. Finally, we discussed the current challenges and provided personal perspectives on electrochemical microcell research.

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Section: Modulation Of Ion Distributionmentioning

confidence: 99%

“…The ESF gating onto the metallic TMD catalysts can also tune the distribution of the ions at the electrolyte-catalyst interface . For example, Mai et al employed the metallic VSe 2 as the catalyst and investigated the distribution of the ions at the electrolyte–VSe 2 interface using four-electrode OCEM microcells (Figure a,b) .…”

Section: Applicationsmentioning

confidence: 99%

Spatially Confined Microcells: A Path toward TMD Catalyst Design

Guo,

Ma,

Wang

et al. 2024

Chem. Rev.

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“…This allowed us to achieve up to a 30-fold increase in the electron transfer rate to outer-sphere redox couples from a 5 nm ZnO back-gated electrode at V G values less than 8 V, for example . Collectively, these early demonstrations, and those of others, − have encouraged us to continue exploring the utility of back-gated 2D working electrodes for enhancing electrochemical reaction rates.…”

Section: Introductionmentioning

confidence: 99%

Four-Terminal Electrochemistry: A Back-Gate Controls the Electrochemical Potential of a 2D Working Electrode

Wang,

Frisbie

2024

J. Phys. Chem. C

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We demonstrate that ultrathin semiconductor working electrodes integrated into metal−insulator−semiconductor (MIS) stacks are an enabling platform for understanding non-Faradaic semiconductor electrochemistry. Here, 5 nm thick ZnO electrodes were deposited on 30 nm HfO 2 dielectric on a Pd "gate" electrode. Application of a bias V G between the Pd gate and the ZnO electrode causes electrons to accumulate in the ZnO layer as measured by recording the in-plane sheet conductance. By contacting the top surface of the ZnO layer with the electrolyte in a conventional three-electrode electrochemical cell, we show that the gate voltage V G modulates the electrochemical potential V ZnO of the ZnO film with respect to a reference electrode. Electrochemical potential changes ΔV ZnO up to −1 V vs Ag/Ag + are achieved for V G = +7 V. Furthermore, by measuring V ZnO vs V G , we extract the quantum capacitance C Q of the ZnO film as a function of the Fermi-level position, which provides a direct measure of the ZnO electronic density of states (DOS). Finally, we demonstrate that the gated ZnO working electrodes can disentangle the two principal components of electrochemical potential, namely, the Fermilevel shift Δδ and the double-layer charging energy eΔϕ EDL . This disentanglement hinges on a fundamental difference between backgating and normal electrochemical control, namely, that electrochemical control requires double-layer charging, while back-gate control does not. Collectively, the results show that the backside gate electrode is an effective fourth terminal that enables measurements that are difficult to achieve in conventional three-terminal electrochemical setups.

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Stimulus of Work Function on Electron Transfer Process of Intermetallic Nickel–Antimonide Toward Bifunctional Electrocatalyst for Overall Water Splitting

Mariappan,

Krishnamoorthy,

Pazhamalai

et al. 2024

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Engineering the intermetallic nanostructures as an effective bifunctional electrocatalyst for hydrogen and oxygen evolution reactions (HER and OER) is of great interest in green hydrogen production. However, a few non‐noble metals act as bifunctional electrocatalysts, exhibiting terrific HER and OER processes reported to date. Herein the intermetallic nickel–antimonide (Ni─Sb) dendritic nanostructure via cost‐effective electro‐co‐deposition method is designed and their bifunctional electrocatalytic property toward HER and OER is unrevealed. The designed Ni─Sb delivers a superior bifunctional activity in 1 m KOH electrolyte, with a shallow overpotential of ≈119 mV at ‐10 mA for HER and ≈200 mV at 50 mA for OER. The mechanism behind the excellent bifunctional property of Ni─Sb is discussed via “interfacial descriptor” with the aid of Kelvin probe force microscopy (KPFM). This study reveals the rate of electrocatalytic reaction depends on the energy required for electron and proton transfer from the catalyst's surface. It is noteworthy that the assembled Ni─Sb‐90 electrolyzer requires only a minuscule cell voltage of ≈1.46 V for water splitting, which is far superior to the art of commercial catalysts.

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Emerging on-chip microcells in electrocatalysis: functions of window and circuit

Abstract: An electrocatalytic process that efficiently converts the reactants into high-value-added chemicals has attracted increasing attention in renewable energy fields. Specifically, understanding such a process at a single-material level will be...

Cited by 3 publications

References 105 publications

Spatially Confined Microcells: A Path toward TMD Catalyst Design

Spatially Confined Microcells: A Path toward TMD Catalyst Design

Four-Terminal Electrochemistry: A Back-Gate Controls the Electrochemical Potential of a 2D Working Electrode

Stimulus of Work Function on Electron Transfer Process of Intermetallic Nickel–Antimonide Toward Bifunctional Electrocatalyst for Overall Water Splitting

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