<i>In situ</i> lattice tuning of quasi-single-crystal surfaces for continuous electrochemical modulation

Zeng, Biao-Feng; Wei, Junying; Zhang, Xia‐Guang; Liang, Qing-Man; Hu, Shu; Gan, Wang; Lei, Zhichao; Zhao, Shiqiang; Zhang, Hewei; Shi, Jia; Hong, Wenjing; Zhang, Tian; Yang, Yang

doi:10.1039/d2sc01868c

Cited by 9 publications

(11 citation statements)

References 68 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Their intriguing physical and chemical properties allow for the fabrication of versatile devices. In particular, in molecular electronics, graphene had been used to fabricate single-molecule junctions with high stability beyond the limits set by the surficial atom mobility of gold (6)(7)(8)(9). On the basis of the nanogapped graphene electrodes, a range of single-molecule devices had been demonstrated, including diode (10), sensor (11,12), field effect transistors (13,14), and so on.…”

Section: Introductionmentioning

confidence: 99%

A van der Waals heterojunction strategy to fabricate layer-by-layer single-molecule switch

Zou

Liang

et al. 2023

Sci. Adv.

Self Cite

View full text Add to dashboard Cite

Single-molecule electronics offer a unique strategy for the miniaturization of electronic devices. However, the existing experiments are limited to the conventional molecular junctions, where a molecule anchors to the electrode pair with linkers. With such a rod-like configuration, the minimum size of the device is defined by the length of the molecule. Here, by incorporating a single molecule with two single-layer graphene electrodes, we fabricated layer-by-layer single-molecule heterojunctions called single-molecule two-dimensional van der Waals heterojunctions (M-2D-vdWHs), of which the sizes are defined by the thickness of the molecule. We controlled the conformation of the M-2D-vdWHs and the cross-plane charge transport through them with the applied electric field and established that they can serve as reversible switches. Our results demonstrate that the M-2D-vdWHs, as stacked from single-layer 2D materials and a single molecule, can respond to electric field stimulus, which promises a diverse class of single-molecule devices with unprecedented size.

show abstract

Section: Introductionmentioning

confidence: 99%

A van der Waals heterojunction strategy to fabricate layer-by-layer single-molecule switch

Zou

Liang

et al. 2023

Sci. Adv.

Self Cite

View full text Add to dashboard Cite

show abstract

“…Electrodeposition of Cu has been extensively studied since it plays an important role in the electroplating and microelectronic industry. − Prior to Cu bulk electrodeposition, Cu underpotential deposition (UPD) might occur when Cu–substrate interaction is stronger than the interaction among the depositing Cu atoms. The behaviors of Cu UPD on foreign metal substrates are of particular interest. − Generally, Cu UPD could form a monolayer of Cu atoms on the metallic substrate, which provides an important subject for understanding transitions from single atoms to a monolayer of condensed metal phase and also help to understand the subsequent Cu overpotential deposition (OPD) process. , In addition, UPD provides an effective way of surface modification to prepare new materials for catalysis, − the modification of nanoparticles, and other applications . Therefore, a deeper understanding of Cu UPD is crucial for both fundamental research and practical applications …”

Section: Introductionmentioning

confidence: 99%

Unconventional Electrochemical Behaviors of Cu Underpotential Deposition in a Chloride-Based Deep Eutectic Solvent: High Underpotential Shift and Low Coverage

Tan

et al. 2023

Anal. Chem.

View full text Add to dashboard Cite

The (5 × 5) Moiré pattern resulting from coadsorption of Cu atoms and chloride ions on the Au(111) electrode is one of the most classical structures for underpotential deposition (UPD) in electrochemical surface science. Although two models have been proposed to describe the pattern, the details of the structure remain ambiguous and controversial, leading to a question that remains to be answered. In this work, we investigate the UPD behaviors of Cu on the Au(111) electrode in a chloride-based deep eutectic solvent ethaline by in situ scanning tunneling microscopy (STM). Benefiting from the properties of the ultraconcentrated electrolyte, we directly image not only Cu but also Cl adlayers by finely tuning tunneling conditions. The structure is unambiguously determined for both Cu and Cl adlayers, where an incommensurate Cu layer is adsorbed on the Au(111) surface with a Cu coverage of 0.64, while the Cl coverage is 0.32 (only half of the expected value); i.e., the atomic arrangement of the observed (5 × 5) Moiré pattern in ethaline matches neither of the models proposed in the literature. Meanwhile, STM results confirm the origin of the cathodic peak in the cyclic voltammogram, which indicates that the underpotential shift of Cu UPD in ethaline indeed increases by ca. 0.40 V compared to its counterpart in a sulfuric acid solution, resulting in a significant deviation from the linear relation between the underpotential shift and the difference in work functions proposed in the literature. The unconventional electrochemical behaviors of Cu UPD reveal the specialty of both the bulk and the interface in the chloride-based deep eutectic solvent.

show abstract

“…[22] However, the deformation of surface geometry caused by different strain effects has not been studied on the electrocatalytic process. [20,23] Therefore, it is important to study the CO reduction reaction and CÀ C coupling mechanism on the copper electrode subjected to strain without deformation, which is helpful to understand the strain effect in the reaction.…”

Section: Introductionmentioning

confidence: 99%

“…Currently, some change surface strain methods have been developed to accurate regulate the atomic arrangement and lattice structure of electrocatalysts and used to improve catalytic activity, [17] including but not limited to build core-shell structures, [18] defects-induced strategy, [19] and mechanically controllable surface strain method. [20] Yang groups build the relationship between the strain effect and the CÀ C coupling by using ab initio molecular dynamics (AIMD) simulation at Cu(111) surface. [21] Wang groups found that the lattice tension can enhance CO adsorption ability and promote carbon-carbon coupling on copper electrode at high CO coverages.…”

Section: Introductionmentioning

confidence: 99%

Lattice Tuning of Copper Single‐Crystal Surface for Electrochemical Carbon Monoxide Coupling Reaction: A Density Functional Theory Simulation

Zhang,

Chen,

Zheng

et al. 2023

ChemElectroChem

Self Cite

View full text Add to dashboard Cite

CO is a key intermediate of electrocatalytic CO2 reduction reaction, which determines the product species. Understanding the effect of metal electrode structure on the adsorption ability and reaction activity of CO is helpful for the design of high selective catalysts. Herein, the DFT calculations are used to investigate the relationship between lattice structure and reaction mechanism of CO, with copper electrode of various lattice constants used as catalysts. By analyzing the adsorption and reaction energies of CO at different lattice constants of Cu(111) and Cu(100) surfaces, we found that the CO adsorption ability is proportional to the increase in lattice, and *CO dimerization to *COCO is the main reaction pathway on Cu(100) surface. Furthermore, the forecasted possible reaction mechanism and products suggest that the coupling of *CO and *CHO to *COCHO and then to C2 products is the preferred pathway on Cu(111) surface for the lattice contraction. Alternatively, reduction of *CO to C1 products through *CHO intermediate is more beneficial for the normal and expanded lattice of Cu(111). This work offers an example of the geometrical influence factor on the CO adsorption ability and reaction activity, and helps to understanding the fundamental role of lattice expansion and contraction in catalysis.

show abstract

In situ lattice tuning of quasi-single-crystal surfaces for continuous electrochemical modulation

Abstract: The ability to control the atomic-level structure of a solid represents a straightforward strategy for fabricating high-performance catalysts and semiconductor materials. Herein we explore the capability of the mechanically controllable...

Cited by 9 publications

References 68 publications

A van der Waals heterojunction strategy to fabricate layer-by-layer single-molecule switch

A van der Waals heterojunction strategy to fabricate layer-by-layer single-molecule switch

Unconventional Electrochemical Behaviors of Cu Underpotential Deposition in a Chloride-Based Deep Eutectic Solvent: High Underpotential Shift and Low Coverage

Lattice Tuning of Copper Single‐Crystal Surface for Electrochemical Carbon Monoxide Coupling Reaction: A Density Functional Theory Simulation

Contact Info

Product

Resources

About