Article
Chemistry, Multidisciplinary
Xingyu Li, Dong Han, Tianchen Qin, Juanjuan Xiong, Jianmin Huang, Tao Wang, Honghe Ding, Jun Hu, Qian Xu, Junfa Zhu
Summary: This study reports the bottom-up fabrication of pristine NPG with Kagome topology on Ag(111) via classic Ullmann coupling using a halogenated precursor. The templating effect of organometallic intermediates for covalent coupling was identified, with reaction parameters having a significant impact on the quality and topology of the intermediates. The work confirms the generality of the organometallic template effect and offers a novel method for selective synthesis of Kagome lattice networks.
Article
Chemistry, Physical
Yuhong Gao, Zhaoyu Zhang, Zewei Yi, Chi Zhang, Wei Xu
Summary: On-surface dehalogenative coupling reactions are promising for constructing nanostructures with diverse properties and functionalities. In this study, the hierarchical evolution of aryl-metal bonding in organometallic intermediates involved in a dehalogenative coupling reaction was visualized and demonstrated. The results enhance the understanding of these reactions and contribute to the controlled construction of desired nanostructures.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Jinping Hu, Zhaofeng Liang, Kongchao Shen, Lei Xie, Huan Zhang, Chaoqin Huang, Yaobo Huang, Han Huang, Jianxin Tang, Zheng Jiang, Miao Yu, Fei Song
Summary: The study provides a comprehensive elucidation of surface Ullmann coupling of 2,7-dibromopyrene on Ag(111), revealing unique reaction paths, diverse assembled architectures, and a stepwise annealing process. It demonstrates that metal coordinated and halogen bonding motifs, as well as surface adatoms and dissociated Br atoms, play crucial roles in the coupling reactions. Additionally, it shows that weak intermolecular interactions in assembled nanostructures are immediately suppressed by strong covalent bonding during reactions.
Article
Chemistry, Physical
Yong Zhang, Jianchen Lu, Baijin Li, Weiben Chen, Wei Xiong, Zilin Ruan, Hui Zhang, Shijie Sun, Long Chen, Lei Gao, Jinming Cai
Summary: The bottom-up synthesis of well-organized covalent-organic frameworks doped with nitrogen atoms on an Ag(111) substrate has been demonstrated. Scanning tunneling spectroscopy revealed an electronic bandgap of 2.45 eV for the N-doped framework, in agreement with theoretical calculations.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Xin Zhang, Qian Shen, Haoxuan Ding, Xiaorui Chen, Hualin Yang, Bosheng Li, Xiu Liu, Haiping Lin, Qing Li, Jianzhi Gao, Gongqiang Li, Minghu Pan, Quanmin Guo
Summary: On-surface synthesis is a promising method for fabricating macromolecular nanostructures, with macrocycles being of significant interest due to their tunable topology-dependent properties. This study successfully synthesized large-sized organometallic macrocycles on the Ag(111) surface using thiophene-containing molecules as precursors. By controlling the reaction pathway, the 18-membered macrocycle was produced as the dominant product among all cyclic configurations.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Han Zhu, Xuhan Zhou, Shenwei Chen, Zizhao Liu, Ye Tao, Dingyong Zhong
Summary: The on-surface reaction processes of C6H2Br2I2 on Au(111) and Ag(100) were investigated using scanning tunneling microscopy, revealing deiodination at room temperature and the formation of organometallic intermediates connected by C-Au-C and C-Ag-C linkages. On Au(111), partial deiodination resulted in ordered structures, while on Ag(100), complete deiodination led to disordered molecular clusters. Further annealing to higher temperatures resulted in covalent C-C bonded polyphenylene chains and disordered graphene nanostructures. This study provides fundamental understanding of temperature-selective on-surface dehalogenation reactions for constructing designer covalently bonded networks.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Guilei Zhu, Guanglin Xia, Xuebin Yu
Summary: This study presents a novel cathode material for magnesium/lithium hybrid batteries, exhibiting high initial and reversible specific capacity, as well as exceptional cycling stability. Utilizing the hierarchical nanoporous array architecture and self-assembly feature, this material provides a guide for designing hierarchical nanoporous materials derived from metal-organic frameworks, and offers a novel strategy of in situ formation for fabricating binder-free cathodes.
Article
Chemistry, Multidisciplinary
Noriyuki Tsukahara, Jun Yoshinobu
Summary: We investigate the formation processes and structures of self-assembled layers of 1,3,5-tris(4-bromophenyl)benzene (TBB) molecules on Ag(111) and Si(111) (/3×/3)-Ag surfaces using STM measurements and DFT calculations. Our findings demonstrate that the interplay between intermolecular interaction and molecule-substrate interaction plays a crucial role in controlling the characteristic structures of the self-assembled layers on the surfaces.
Article
Chemistry, Physical
Dong Han, Zhiwen Zeng, Bingchu Tian, Pu Wang, Jun Hu, Honghe Ding, Qian Xu, Junfa Zhu
Summary: This work demonstrates the stepwise activation of C-Br and C-H on a precursor molecule and the formation of self-assembled nanostructures on Ag(111). Surprisingly, the C-C coupling for organometallic dimers fails to occur, but instead, the dissociation of organometallic dimers and activation of cyano ortho C-H leads to the formation of chiral organometallic multimers.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Lukas Grossmann, David A. Duncan, Samuel P. Jarvis, Robert G. Jones, Soumen De, Johanna Rosen, Michael Schmittel, Wolfgang M. Heckl, Jonas Bjork, Markus Lackinger
Summary: NIXSW analysis allows precise measurement of adsorption heights, providing new perspectives on surface interactions and molecular conformations. The study of porous covalent triazine-phenylene networks on Ag(111) reveals the evolution of molecular conformations and adsorption heights during on-surface synthesis and post-synthetic decoupling.
NANOSCALE HORIZONS
(2022)
Article
Chemistry, Physical
Caimei Gong, Yuyang Zhang, Yan Lu, Zhongping Wang, Shizhang Fu, Sheng Wei, Xiaoqing Liu, Li Wang
Summary: The water-induced assembly structures of 4-aminobenzoic acid (PABA) on Au(111) and Ag(111) surfaces were studied using scanning tunneling microscopy and density functional theory calculations. Water molecules can break the weak-hydrogen bonded Kagome' structure on Au(111) and the four-leaf clover structure formed by intermediate hydrogen bonds between PABA molecules, leading to the release of water molecules. The adsorption energy of the hydrated structure formed on Ag(111) is significantly lower than that on Au(111), resulting in the selective formation of the water-involved structure on Ag(111).
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Goutam Nandi, Rohith Phaneendra Bandaru, Ranjan Patra, Ananda Kumar Jami, Bharat Kumar Tripuramallu
Summary: This study developed novel supramolecular structures based on a custom-designed porphyrin linker Zn(II)-5,10,15,20-tetra(4-bromo-2,6-difluorophenyl) porphyrin (Zn-BFP). The inclusion of electron-withdrawing fluorine atoms near bromine atoms increased the polarizability of the bromine atoms and their participation in halogen bonding. Three new supramolecular solids were synthesized using Zn-BFP with axial linkers nicotinic acid and 5-bromonicotinic acid, exhibiting diverse halogen bonding and hydrogen bonding motifs. The influence of fluorine atoms on the porphyrin skeleton and their participation in halogen bonding were illustrated.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Spectroscopy
Kaiqiang Wang, Jinjie Li
Summary: In this study, a high-performance surface-enhanced Raman spectroscopy (SERS) analytic platform was developed through self-assembly of nanoparticles and achieved high reproducibility and accuracy for measuring chemical contaminants in various phases. The use of an internal standard to correct signal fluctuations improved point-to-point and batch-to-batch reproducibility, enabling high-sensitive detection and improved accuracy for pesticide analysis.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2021)
Article
Chemistry, Physical
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
Viktoria V. Ivanovskaya, Alberto Zobelli, Andrea Basagni, Stefano Casalini, Luciano Colazzo, Francesco de Boni, Dimas G. de Oteyza, Mauro Sambi, Francesco Sedona
Summary: The growth of poly-p-phenylene chains and subsequent narrow graphene ribbons on silver surfaces is investigated. The study reveals the formation of organometallic molecules and chains during the debromination step, unlike on gold surfaces. The presence of intercalated bromine atoms hinders the formation of well-structured graphene ribbons at the dehydrogenation temperature.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
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.
Article
Chemistry, Physical
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.
Article
Chemistry, Physical
Yuxuan Lin, Mengxiao Diao, Jingxin Dai, Zhen Xu, Xinwei Zhao, Xiaojie Wen, Lingbo Xing, Xiong Zhou, Qiwei Chen, Jing Liu, Kai Wu
Summary: A molecular investigation reveals that Cu adatoms embedded in DCTP-Cu chains on Cu(111) surface are located at the hollow and bridge sites, leading to stepwise elimination of Cu adatoms in the chains. The interchain interaction plays an important role in the Cu-elimination process and promotes the cooperative Cu-elimination and C-C coupling of the OM segments in neighboring chains. These findings demonstrate the key role of molecule-substrate and intermolecular interactions in mediating the reaction processes of extended molecular systems on surfaces.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Multidisciplinary Sciences
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
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
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.
Article
Chemistry, Physical
Xiaoyan Bao, Dawei Lu, Zining Wang, Hao Yin, Biao Zhu, Bin Chen, Meixiang Shi, Yang Zhang, Qianxin Xu, Yumei Qin, Xing -Can Shen, Kai Wu
Summary: Using solar energy to convert CO2 into value-added chemicals has great potential to address global energy shortage and climate change. This study reports a novel strategy of preparing a boron-doped g-C3N4/TiO2-x composite catalyst (BCT) that shows extended full-spectrum absorption, rapid charge separation, and outstanding CO2 photoreduction performance. The CO2 conversion rate of BCT is 7.5 and 9.2 times higher than that of pure TiO2 and g-C3N4, respectively. Mechanistic studies reveal that the synergistic effects of BCT lower the energy barrier for CO2 conversion by altering charge density distribution. This work provides a new integrated strategy for fabricating efficient catalysts.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
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.
Article
Chemistry, Physical
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)
Letter
Multidisciplinary Sciences
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
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
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.
