4.6 Article

Self-assembly of binary molecular nanostructure arrays on graphite

Journal

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
Volume 15, Issue 30, Pages 12414-12427

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cp00023k

Keywords

-

Funding

  1. Singapore ARF [R143-000-505-112, R143-000-530-112]
  2. NUS YIA grant [R143-000-452-101]

Ask authors/readers for more resources

The controlled positioning and assembly of functional molecules into ordered nanostructures on surfaces depends on the interplay of multiple interactions on different strength and length scales. On metal surfaces, the relatively strong molecule-substrate interactions can constrain the molecules to adsorb in registry with the surface periodicity and lock them into specific adsorption sites. This can significantly reduce the structural tunability of the molecular nanostructure arrays formed. Inert graphite has a smooth potential-energy surface as well as relatively weak interfacial interactions with adsorbed molecules, and is therefore chosen as a supporting substrate for constructing molecular nanostructures with a high degree of controllability and tunability. The aim of this article is to highlight recent progress in the fabrication of self-assembled molecular nanostructures on inert graphite surfaces in ultra-high vacuum, with particular emphasis on the role of intermolecular interactions in the self-assembly process. We describe the formation of tunable two-dimensional (2D) binary molecular networks by directional and selective hydrogen bonding, as well as the templating effect of these 2D molecular networks, demonstrating the rational design and construction of long-range ordered 2D molecular nanostructures with desired functionality.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.6
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Chemistry, Physical

Visible-light stimulated synaptic plasticity in amorphous indium-gallium-zinc oxide enabled by monocrystalline double perovskite for high-performance neuromorphic applications

Fu Huang, Feier Fang, Yue Zheng, Qi You, Henan Li, Shaofan Fang, Xiangna Cong, Ke Jiang, Ye Wang, Cheng Han, Wei Chen, Yumeng Shi

Summary: In this study, an optically-stimulated artificial synapse has been demonstrated using a heterostructure of Cs2AgBiBr6 perovskite and IGZO thin film. The heterostructure significantly enhances the photoresponse and synaptic plasticity, enabling the realization of various synaptic behaviors and achieving a high accuracy rate for pattern recognition in an artificial neural network simulation.

NANO RESEARCH (2023)

Article Chemistry, Physical

Interfacial high-concentration electrolyte for stable lithium metal anode: Theory, design, and demonstration

Haotian Lu, Chunpeng Yang, Feifei Wang, Lu Wang, Jinghong Zhou, Wei Chen, Quan-Hong Yang

Summary: Lithium metal anodes have great potential for high-energy-density secondary batteries. However, uncontrolled lithium dendrite growth inhibits their practical application. This study proposes an interfacial high-concentration electrolyte induced by nitrogen- and oxygen-doped carbon nanosheets (NO-CNS) to stabilize lithium metal anodes. The interfacial high-concentration electrolyte improves charge transfer kinetics and ionic mass-transfer, leading to excellent electrochemical performance.

NANO RESEARCH (2023)

Article Chemistry, Multidisciplinary

Facet-controlled bifunctional WO3 photocathodes for high-performance photo-assisted Li-O2 batteries

Meng Wang, Jie Chen, Zhangliu Tian, Wenrui Dai, Baihua Cui, Xinhang Cui, Dong Wang, Yukun Xiao, Xu Lian, Chonglai Jiang, Haotian Yang, Yihe Wang, Zejun Sun, Yishui Ding, Yi-Yang Sun, Jia Zhang, Wei Chen

Summary: Research reveals that by adjusting the surface structure of WO3 photocathodes, the formation of Li2O2 can be controlled and the photocatalytic reaction activity can be enhanced. Additionally, the (002) facet is found to have higher oxidation ability, resulting in an ultralow polarization overpotential and high discharge capacity over the (002) facet dominated WO3 photocathode.

ENERGY & ENVIRONMENTAL SCIENCE (2023)

Article Multidisciplinary Sciences

Selective photoelectrochemical oxidation of glucose to glucaric acid by single atom Pt decorated defective TiO2

Zhangliu Tian, Yumin Da, Meng Wang, Xinyu Dou, Xinhang Cui, Jie Chen, Rui Jiang, Shibo Xi, Baihua Cui, Yani Luo, Haotian Yang, Yu Long, Yukun Xiao, Wei Chen

Summary: Photoelectrochemical oxidation provides a promising strategy for glucaric acid production. In this work, selective oxidation of glucose to glucaric acid is realized on the photoanode of defective TiO2 decorated with single-atom Pt via a photoelectrochemical strategy. By optimizing oxygen vacancies, the defective TiO2 photoanode exhibits greatly improved charge separation, significantly enhanced selectivity, and yield of C-6 products.

NATURE COMMUNICATIONS (2023)

Article Materials Science, Multidisciplinary

Dual Pt-Ni atoms dispersed on N-doped carbon nanostructure with novel (NiPt)-N4C2 configurations for synergistic electrocatalytic hydrogen evolution reaction

Yumin Da, Zhangliu Tian, Rui Jiang, Yuan Liu, Xu Lian, Shibo Xi, Yi Shi, Yongping Wang, Haotian Lu, Baihua Cui, Jinfeng Zhang, Xiaopeng Han, Wei Chen, Wenbin Hu

Summary: This paper reports the synthesis of a PtNi-NC catalyst with high catalytic activity. Density functional theory calculations reveal that PtNi dual atoms generate a synergistic effect by modulating the local electronic structure and optimizing the charge distribution, contributing to optimized adsorption properties and enhanced electrocatalytic performance. This work provides a new avenue for the fabrication of dual-atom catalysts.

SCIENCE CHINA-MATERIALS (2023)

Article Electrochemistry

In-Situ Photoelectron Spectroscopy Investigation of Sulfurization-Induced Sodiophilic Sites with Model Systems of α-sexithiophene and p-sexiphenyl

Yuan Liu, Xu Lian, Chonglai Jiang, Zejun Sun, Jinlin Yang, Yishui Ding, Wei Chen

Summary: To stabilize sodium metal anodes (SMAs), various strategies have been developed, including employing anode hosts and electrolyte additives to establish protective layers. In this study, the interaction mechanism between sodium metal and sulfur-containing functional groups was investigated using comparative model systems of alpha-sexithiophene (6T) and p-sexiphenyl (6P). The results showed that sodium atoms tend to interact with sulfur atoms and their connected carbon atoms as well as the aromatic carbon atoms of the end groups of 6T molecules, while no chemical interaction between Na and 6P molecules was observed. These findings shed light on the rational design of sulfur-containing protective materials and relevant interface engineering to stabilize SMAs.

BATTERIES-BASEL (2023)

Article Chemistry, Physical

In-situ near-ambient-pressure photoelectron spectroscopy investigations of high-work-function MoO3 on 4H-SiC(0001)

Li Peize, Lian Xu, Gou Jian, Duan Sisheng, Ding Yishui, Niu Yuxiang, Chen Wei

Summary: Realizing effective Ohmic contact to SiC is a major challenge in high-power and high-frequency SiC electronics. Here, we grew a high-work-function interfacial molybdenum trioxide (MoO3) layer on 4H-SiC(0001) and investigated its surface properties during annealing in different gas environments. The results show that the MoO3 layer tends to be reduced and the surface work function decreases accordingly, making it a promising approach for achieving effective Ohmic contact with SiC.

SURFACE SCIENCE (2023)

Article Chemistry, Physical

Development of a Novel Pt3V Alloy Electrocatalyst for Highly Efficient and Durable Industrial Hydrogen Evolution Reaction in Acid Environment

Yumin Da, Rui Jiang, Zhangliu Tian, Ganwen Chen, Yukun Xiao, Jinfeng Zhang, Shibo Xi, Yida Deng, Wei Chen, Xiaopeng Han, Wenbin Hu

Summary: Alloying platinum with early transition metals is a promising approach to optimize catalyst adsorption behaviors. A strategy combining thermal shock technique with electrochemical activation is reported for the first time to prepare Pt3V alloy as a hydrogen evolution reaction catalyst. The as-prepared catalyst exhibits exceptional catalytic activity and durability, outperforming the state-of-the-art Pt/C catalyst. This work may inspire future research on Pt-based early transition metal alloy catalysts for electrocatalysis.

ADVANCED ENERGY MATERIALS (2023)

Article Chemistry, Multidisciplinary

Single-Atom Pt Doping Induced p-Type to n-Type Transition in NiO Nanosheets toward Self-Gating Modulated Electrocatalytic Hydrogen Evolution Reaction

Yumin Da, Zhangliu Tian, Rui Jiang, Ganwen Chen, Yuan Liu, Yukun Xiao, Jinfeng Zhang, Shibo Xi, Wei Chen, Xiaopeng Han, Wenbin Hu

Summary: In this research, a highly efficient electrocatalyst for the hydrogen evolution reaction was developed by using Pt single atoms supported on ultrathin NiO nanosheets. A self-gating phenomenon was induced in the nanosheets, resulting in the formation of active and inert regions. The active region allows for the HER process to occur, while the inert region accumulates charge carriers, leading to high conductivity and stability of the electrocatalyst.

ACS NANO (2023)

Article Chemistry, Physical

Ultrathin Pt and Mo films on Al1-xScxN: an interface investigation

Yishui Ding, Xiangyu Hou, Tengyu Jin, Yanan Wang, Xu Lian, Yuan Liu, Yihe Wang, Sisheng Duan, Xiangrui Geng, Meng Wang, Jingyu Mao, Yuanyuan Zhang, Peirong Tang, Minghua Li, Huamao Lin, Yao Zhu, Siewlang Teo, Qiang Zhu, Ming Lin, Wei Chen

Summary: In this study, the growth mechanism and interfacial chemistry of ultrathin platinum and molybdenum films on high-crystalline Al1-xScxN surface were investigated. The chemical and electronic structure evolution of the interface during the deposition process were examined using in-situ X-ray photoelectron spectroscopy and ultraviolet photoelectron spectroscopy. The structural properties of the interface were characterized by cross-sectional transmission electron microscopy, X-ray diffraction spectroscopy, and atomic force microscopy. The study reveals the formation of ionic Pt2+-N bonds at the Pt/Al1-xScxN interface, while molybdenum does not bond with the substrate. Furthermore, electron transfer induces upward band-bending effects on the Al1-xScxN surface upon both platinum and molybdenum interactions. The research on the chemical and structural properties of ultrathin metal electrodes and Al1-xScxN interfaces provides guidance for designing high-performance micro-electromechanical devices.

APPLIED SURFACE SCIENCE (2023)

Article Chemistry, Multidisciplinary

Achieving High-Performance Electrocatalytic Water Oxidation on Ni(OH)2 with Optimized Intermediate Binding Energy Enabled by S-Doping and CeO2-Interfacing

Xiang Chen, Xinyue Xu, Yuwen Cheng, He Liu, Dongdong Li, Yumin Da, Yongtao Li, Dongming Liu, Wei Chen

Summary: The study presents a facile strategy to enhance the oxygen evolution reaction (OER) activity of Ni-based materials through doping and interfacial modulation. Experimental and theoretical results demonstrate that this strategy can effectively tune the binding energies of OER intermediates and reduce the energy barrier, leading to significantly improved OER activity.

SMALL (2023)

Article Chemistry, Physical

Surface evolution of Pt/MoO3/4H-SiC(0001) investigated by in situ near-ambient pressure X-ray photoelectron spectroscopy

Xiangrui Geng, Yishui Ding, Yuan Liu, Xiangyu Hou, Tengyu Jin, Wei Chen

Summary: Achieving effective Ohmic contact between SiC and metal electrodes remains a challenge due to the high Schottky barrier. One promising approach is to introduce a high-work-function interfacial layer. However, the interaction mechanisms between the interfacial layer and the SiC substrate have been rarely studied. In this work, layers of high-work-function MoO3 and Pt were grown on the SiC surface, and the evolutions of the system during annealing under different environments were studied. The results provide a detailed understanding of the Pt/MoO3 interface and its response to various conditions.

SURFACE SCIENCE (2023)

Letter Multidisciplinary Sciences

Reply to: Reassessing the existence of soft X-ray correlated plasmons

T. J. Whitcher, A. D. Fauzi, C. Diao, X. Chi, A. Syahroni, T. C. Asmara, M. B. H. Breese, A. H. Castro Neto, A. T. S. Wee, M. A. Majidi, A. Rusydi

NATURE COMMUNICATIONS (2023)

Article Electrochemistry

Interaction Mechanisms Between Nitrogen-Containing Groups and Alkali Metals with Molecular Model System of HATCN

Yuan Liu, Xu Lian, Xiaojiang Yu, Yuxiang Niu, Jinlin Yang, Yishui Ding, Wei Chen

Summary: This study investigates the interaction processes between alkali metal anodes (AMAs) and organic protective materials containing nitrogen groups. The results show that Li and Na preferentially interact with the outer nitrile groups of the protective material before interacting with the inner imine groups. Additionally, the sodiophilicity difference between the two nitrogen-containing groups is smaller compared to their lithiophilicity difference. These findings provide valuable insights for the development of more effective protective materials in the future.

BATTERIES & SUPERCAPS (2023)

Review Chemistry, Multidisciplinary

The applications of single-atom alloys in electrocatalysis: Progress and challenges

Yumin Da, Rui Jiang, Zhangliu Tian, Xiaopeng Han, Wei Chen, Wenbin Hu

Summary: The development of cost-effective and highly efficient electrocatalysts is crucial for achieving a low-carbon footprint in the industry. Single-atom alloys (SAAs) have unique electronic structures, well-defined active sites, and maximum atom utilization, making them promising replacements for traditional noble metal catalysts. SAAs can tailor the adsorption properties of reaction species to promote electrocatalytic behaviors.

SMARTMAT (2023)

Article Chemistry, Physical

Effect of a single methyl substituent on the electronic structure of cobaltocene studied by computationally assisted MATI spectroscopy

Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng

Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Review Chemistry, Physical

Polymer mechanochemistry: from single molecule to bulk material

Qifeng Mu, Jian Hu

Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Complex oiling-out behavior of procaine with stable and metastable liquid phases

Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li

Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Breaking the size constraint for nano cages using annular patchy particles

Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu

Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Effect of the charge rate on the mechanical response of composite graphite electrodes: in situ experiment and mathematical analysis

Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li

Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

The effect of weak π-π interactions on single-molecule electron transport properties of the tetraphenylethene molecule and its derivatives: a first-principles study

Zhiye Wang, Yunchuan Li, Mingjun Sun

Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Designed fabrication of MoS2 hollow structures with different geometries and the comparative investigation toward capacitive properties

Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang

Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Exploiting the photophysical features of DMAN template in ITQ-51 zeotype in the search for FRET energy transfer

Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez

Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Insights into the multi-functional lithium difluoro(oxalate)borate additive in boosting the Li-ion reaction kinetics for Li3VO4 anodes

Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni

Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

New insights into the structure of the Ag(111)-p(4 x 4)-O phase: high-resolution STM and DFT study

B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga

Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

ClO-driven degradation of graphene oxide: new insights from DFT calculations

S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez

Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Composition dependence of X-ray stability and degradation mechanisms at lead halide perovskite single crystal surfaces

Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel

Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Effect of porosity on rapid dynamic compaction of nickel nanopowder

Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov

Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

The effect of temperature and oxygen partial pressure on the concentration of iron and manganese ions in La1/3Sr2/3Fe1-xMnxO3-δ

Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev

Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Perovskenes: two-dimensional perovskite-type monolayer materials predicted by first-principles calculations

Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub

Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)