Article
Chemistry, Multidisciplinary
Wang Li, De-Xuan Liu, Wei-Yu Hu, Qing-Yan Liu, Zi-Yi Du, Chun-Ting He, Wei-Xiong Zhang, Xiao-Ming Chen
Summary: This research presents a novel crystalline molecular rotor with two discrete polar rotators. Experimental results show that these rotators experience an enhanced rotation with increasing temperature, and can be controlled by a reversible polar-to-polar structural phase transition.
CHINESE JOURNAL OF CHEMISTRY
(2022)
Article
Nanoscience & Nanotechnology
Kristin L. Lewis, Katie M. Herbert, Valentina M. Matavulj, Jonathan D. Hoang, Eric T. Ellison, Grant E. Bauman, Jeremy A. Herman, Timothy J. White
Summary: The synthesis of liquid crystalline elastomers (LCEs) with intra-mesogenic supramolecular bonds via direct free-radical chain transfer photopolymerization enables shape change under mechanical alignment, providing functional utility in robotics, medicine, consumer goods, and photonics.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Kyle R. Schlafmann, Mohammed S. Alahmed, Kristin L. Lewis, Timothy J. White
Summary: This study constructs liquid crystalline elastomers (LCEs) with intra-mesogenic supramolecular bonds, enhancing the tunability and achieving a rate of 4.8 nm/℃ for temperature regulation. These materials incorporate liquid crystalline monomers based on dimerized oxy-benzoic acid (OBA) derivatives, and increasing the concentration of the OBA comonomers increases the red-shifting thermochromism of the selective reflection. Beyond a threshold concentration, the selective reflection in the CLCEs can disappear upon heating, similar to on-off switching. Additionally, the introduction of supramolecular bonds enables mechanical programming and one-time tunable thermochromism through a one-way shape memory process. Therefore, this research could have functional applications in low temperature sensitive optical elements, fail-safe thermal indicators for food packaging, and smart window coatings.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Jia-Rui Wu, Gengxin Wu, Dongxia Li, Ying-Wei Yang
Summary: Synthetic macrocycles have played a significant role in supramolecular chemistry, expanding the scope of organic charge transfer complexes and demonstrating practical value in the solid state. This MiniReview summarizes the research progress on macrocycle-based crystalline supramolecular assemblies driven by intermolecular charge transfer interactions (MCCAs). The assemblies are classified based on their donor-acceptor constituent elements, including simplex macrocyclic hosts, heterogeneous macrocyclic hosts, and host-guest D-A pairs. The diverse functions, applications, and underlying charge transfer mechanisms are discussed from the perspective of crystal engineering. The remaining challenges and prospects are also outlined.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yaorong Chen, Hua-Chun Wang, Yongxiang Tang, Yu Zhou, Longfeng Huang, Jian Cao, Chun Tang, Manxi Zhang, Jia Shi, Junyang Liu, Xiancheng Ren, Yun-Xiang Xu, Wenjing Hong
Summary: The presence of intramolecular hydrogen bonds promotes planarization of molecular structure, leading to higher conductance by reducing dihedral twisting. This offers a new strategy for controlling molecular switches through molecular twisting.
CHEMICAL COMMUNICATIONS
(2021)
Article
Polymer Science
Maroua Louati, Jean-Francois Tahon, David Fournier, Gregory Stoclet, Stephane Aloise, Marumi Takao, Michinori Takeshita, Jean-Marc Lefebvre, Sophie Barrau
Summary: The structural evolution of a supramolecular copolymer assembly based on multiple hydrogen bonds was investigated through in situ WAXS and SAXS experimentation. The impact of the hydrogen bonding network on structural arrangements was highlighted, with special attention to the crystallinity and crystal forms associated with ethylene sequences. Crystalline domains with an in-plane arrangement between neighboring UPy dimers were detected up to 80 degrees C.
Article
Chemistry, Multidisciplinary
Quentin Sallembien, Pamela Aoun, Sebastien Blanchard, Laurent Bouteiller, Matthieu Raynal
Summary: The study investigates the structure of mixed valence assemblies formed by irradiating triarylamine trisamide (TATA) molecules and explores the interplay between the hydrogen bonding network and the rate of electron transport. The findings suggest that hydrogen bonding is necessary but not sufficient for fast electron transfer rates, and a delicate balance between hydrogen bonds and packing is required for efficient charge transport.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Polymer Science
Jun-Guo Gao, Li-Wei Liu, Wei-Feng Sun
Summary: Polar group-modified crosslinked polyethylene (XLPE) materials are developed by grafting chloroacetic acid allyl ester (CAAE) and maleic anhydride (MAH) to polyethylene molecular chains, improving dielectric characteristics through charge-trapping mechanism. The grafted polar-group molecules introduce deep-level charge traps in XLPE materials, restrict charge injections, hinder charge carrier transports, and significantly enhance electric resistance and dielectric breakdown strength.
Article
Chemistry, Multidisciplinary
Valentina Milasinovic, Vedran Vukovic, Anna Krawczuk, Kresimir Molcanov, Christoph Hennig, Michael Bodensteiner
Summary: The investigated co-crystal of 3-chloro-N-methylpyridinium iodide with tetrabromoquinone exhibits a pi-hole interaction involving charge transfer. The quinoid ring displays partial negative charge and radical character, contributing to the black color of the crystals. X-ray charge density study confirms the interaction between iodide anions and carbon atoms in the ring. The energy of the interaction is comparable to moderate hydrogen bonding.
Article
Chemistry, Multidisciplinary
Lukas Ustrnul, Tatsiana Burankova, Mario Oeren, Kristina Juhhimenko, Jenni Iimarinen, Kristjan Siilak, Kamini A. Mishra, Riina Aav
Summary: This study demonstrated a preference for hydrogen bond-donating molecules in the binding of cyclohexanohemicucurbit[n]urils with a set of eighteen organic guests. The overall binding strength was found to be influenced by the stoichiometry of the formed complexes, the partial atomic charge on the hydrogen atom of the hydrogen bond donor, and the bulkiness of the guest. Additionally, the study did not confirm the formation of complexes with halogen anions (Cl- and Br-).
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Shengya Zhang, Peiyao Du, Hui Xiao, Ze Wang, Rongfang Zhang, Wei Luo, Juan An, Yuling Gao, Bingzhang Lu
Summary: Limited charge separation/transport efficiency is still a major challenge in achieving high-performance photoelectrochemical (PEC) water splitting. In this study, a novel coupling modification strategy was developed to achieve bidirectional carrier transport on a composite electrode, resulting in significantly improved PEC water splitting performance of a pure ZnIn2S4 photoanode. The enhanced charge separation was attributed to the stimulated bidirectional charge transfer pathways through MXene quantum dots (MQDs) as electron extractors and S-O bonds as carriers transport channels. This research enhances our understanding of interfacial charge separation and provides valuable guidance for the design and fabrication of high-performance composite electrodes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Daniel Ejarque, Teresa Calvet, Merce Font-Bardia, Josefina Pons
Summary: In this study, a rational design of cocrystals was achieved by controlling hydrogen-bonded patterns. The crystal structures of two cocrystals formed with 4-acetylpyridine and 2-hydroxypyridine were elucidated using liquid-assisted grinding. Melting point data were obtained and correlated with crystal packing and properties.
Article
Chemistry, Physical
Raka Ahmed, Arun K. Manna
Summary: This study investigated the photophysical properties of a recently synthesized modular fluorescent probe using first-principles density functional theory, revealing that the optical absorption of StyPy is minimally impacted by solvent polarity, while the emission is significantly red-shifted with increasing solvent polarity. It was also discovered that partial charge-transfer-assisted significant excited-state relaxation leads to a nearly planarized StyPy structure, causing the observed Stokes shift. Additionally, the crystalline form of StyPy demonstrates higher electron mobility compared to holes, making it a potential n-type transport material for bioimaging and electronic applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Tamara A. Vaganova, Enrico Benassi, Yurij Gatilov, Igor P. Chuikov, Denis P. Pishchur, Evgenij Malykhin
Summary: The study investigated the supramolecular structure of co-crystals formed by para- and ortho-aminobenzonitriles with 18-crown-6 ether, revealing changes in the solid-state fluorescence characteristics of the aminobenzonitriles upon co-crystallization. Advanced TD-DFT calculations provided insights into the molecular interactions during co-crystallization and their impact on photophysical properties. The research proposed a quantitative model to distinguish the behavior of ortho- and para-substituted molecules and suggested the importance of the arrangement of H-bond functionalities in modifying the molecular packing and tuning the solid-state photophysical properties.
Article
Chemistry, Multidisciplinary
Jiahui Wang, Pengfei Yang, Lingmei Liu, Bin Zheng, Jing Jiang, Jian-ping Ma, Yi Yan, Song Yang, Luo Yang, Qi-Kui Liu, Yu Han, Yin Chen
Summary: In this study, a novel metal-organic framework (MOF) IPM-1 was synthesized and found to be capable of being exfoliated into two-dimensional nanosheets with excellent thickness homogeneity and restored microporosity. These nanosheets exhibited high chemical stability and catalytic activity in the oxidation of alcohol, combining the advantages of both homogeneous and heterogeneous catalysts.
Article
Chemistry, Multidisciplinary
Huan Xue, Haolin Zhu, Jiarun Huang, Peiqin Liao, Xiaoming Chen
Summary: In this study, a novel two-dimensional metal-organic framework Cu-HHTT was reported as an electrocatalyst for CO2RR, which showed high performance in CO production with high selectivity. It was found that the desorption of CO species had a lower energy barrier compared to the hydrogenation of *CO intermediate, leading to the predominance of CO as the main product.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Multidisciplinary
De-Xuan Liu, Zhi-Hong Yu, Xiao-Xian Chen, Wei-Xiong Zhang, Xiao-Ming Chen
Summary: This paper presents two new organic-inorganic hybrid crystals, which exhibit distinct phase transitions and provide insights into the complicity of multi-component crystals. Understanding these phase transitions is important for the regulation of functional materials.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Yu Wang, Ning-Yu Huang, Hao-Yu Wang, Xue-Wen Zhang, Jia-Run Huang, Pei-Qin Liao, Xiao-Ming Chen, Jie-Peng Zhang
Summary: The electrochemical reduction of CO2 can be significantly improved by introducing amino groups alongside porphyrin cobalt centers in a metal-organic framework (MOF).
Article
Chemistry, Multidisciplinary
Yan-Tong Xu, Zi-Ming Ye, De-Xuan Liu, Xiao-Yun Tian, Dong-Dong Zhou, Chun-Ting He, Xiao-Ming Chen
Summary: Two new Zn(II) imidazolate frameworks incorporating MoO4 2- or WO4 2- units were reported, which can catalyze the cycloaddition of CO2 and epichlorohydrin at room temperature and atmospheric pressure, achieving high yields. The modulation mechanisms of the MoO4 2- unit in optimizing the electronic structure of Zn(II) center were revealed.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Yong Wang, Tong Li, Libo Li, Rui-Biao Lin, Xiaoxia Jia, Zeyu Chang, Hui-Min Wen, Xiao-Ming Chen, Jinping Li
Summary: A new fluorinated metal-organic framework (FDMOF-2) featuring precise incorporation of fluorinated functional groups into the confined pore space is successfully constructed for the separation of propane/propene. FDMOF-2 shows excellent capture capacity and selectivity, setting new benchmarks for porous materials. The breakthrough experiments demonstrate outstanding propane production with high purity.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
De-Xuan Liu, Hao-Lin Zhu, Wei-Xiong Zhang, Xiao-Ming Chen
Summary: Melt-quenched glasses of organic-inorganic hybrid crystals have gained attention as a class of hybrid materials with good processability and formability. A new hybrid crystal with thermal-induced reversible crystal-liquid-glass-crystal transitions was reported. By using mild conditions, a hybrid glass-ceramic thin film with enhanced nonlinear optical effect was successfully fabricated.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Hui Xiao, Liwen Ding, Jingyan Liu, Zhihui Jia, Liming Cao, Ziyi Du, Chunting He
Summary: The switchable molecular dynamics and order-disorder transformation of (i-PrNHMe2) thorn cation embedded in a deformable {[Ni(NCS)6]4-}& INFIN; supramolecular framework are investigated through variable-temperature tests. The confined swinging or flipping of the (iPrNHMe2) thorn cation is found to be assisted by a synergistic change of its torsion angle. This research provides insight into the solid-state molecular dynamics of moderately-sized quasi-spherical molecules/ions with a flexible inner core.
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
De-Xuan Liu, Wei-Xiong Zhang, Xiao-Ming Chen
Summary: Understanding the microscopic origin of phase transitions in hybrid crystals is crucial but challenging. This study synthesized three new hybrid crystals and comprehensively studied their crystal structures, intermolecular interactions, and phase transitions. The results demonstrate the importance of delicate and complicated intermolecular interactions in inducing nontrivial phase transitions in hybrid crystals.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Meng-Di Zhang, Jia -Run Huang, Wen Shi, Pei-Qin Liao, Xiao-Ming Chen
Summary: In this study, a stable metal-organic framework (PcNi-Co-O) was reported as a bifunctional electrocatalyst for efficient CO2 overall splitting. PcNi-Co-O achieved a commercial-scale current density of 123 mA cm-2 and a Faradic efficiency (CO) of 98% at a low cell voltage of 4.4 V when used as both cathode and anode catalysts. Mechanism studies revealed the synergistic effects between two active sites and the energy-level matching of cathode and anode catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Li-Ming Cao, Chang-Guo Hu, Hai-Hong Li, Hui-Bin Huang, Li-Wen Ding, Jia Zhang, Jun-Xi Wu, Zi-Yi Du, Chun-Ting He, Xiao-Ming Chen
Summary: Remolding the reactivity of metal active sites is crucial for efficient water electrolysis. Doping heteroatoms into a metal crystal lattice has been a promising approach, but often suffers from the loss of functional heteroatoms during harsh electrocatalytic conditions. In this study, an organoselenium ligand is used to enhance the catalytic activity and extend the catalyst lifespan, through the formation of robust C-Se-C covalent bonds in the precatalyst. The results demonstrate the great potential of molecule-enhanced catalysts for sustainable and economical water oxidation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Wei-Jian Xu, Mao-Fan Li, Ana R. Garcia, Konstantin Romanyuk, Josee M. G. Martinho, Pavel Zelenovskii, Alexander Tselev, Luis Verissimo, Wei-Xiong Zhang, Xiao-Ming Chen, Andrei Kholkin, Joao Rocha
Summary: The design and synthesis of a new metal-nitrosyl ferroelectric crystal (DMA)(PIP)[Fe(CN)(5)(NO)] with potential phototunable polarization via a dual-organic-cation molecular design strategy is reported. The crystal exhibits a large polarization and a high Curie temperature, and the reversible photoisomerization of the nitrosyl ligand is accomplished by light irradiation. The optical accessibility and controllability of different ferroelectric states via photoinduced nitrosyl linkage isomerization present a new and attractive route to optically controllable macroscopic polarization.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Jun-Xi Wu, Wen-Xing Chen, Chun-Ting He, Kai Zheng, Lin-Ling Zhuo, Zhen-Hua Zhao, Jie-Peng Zhang
Summary: In this study, asymmetric structural evolution and a dynamic hydrogen-bonding promotion mechanism of an atomically dispersed electrocatalyst were reported. Nitrogen-doped porous carbons, functionalized by atomically dispersed Co-Ni dual-metal sites with an unprecedented N8V4 structure, were obtained through the pyrolysis of Co/Ni-doped MAF-4/ZIF-8. This electrocatalyst showed remarkable activation behavior due to the in situ oxidation of the carbon substrate to form C-OH groups, which can form reversible hydrogen bonds with the oxygen evolution reaction intermediates, breaking the conventional scaling relationship.
NANO-MICRO LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Yuan-Yuan Liu, Jia-Run Huang, Hao-Lin Zhu, Pei-Qin Liao, Xiao-Ming Chen
Summary: This study demonstrates the integration of CO2 capture capability and electrochemical CO2 reduction reaction (eCO2RR) active sites using a silver-based metal-organic framework. The catalyst showed efficient CO2 capture from simulated flue gas and high conversion of adsorbed CO2 into CO during eCO2RR. The study has bridged the gap between CO2 enrichment/capture and eCO2RR.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Jing Guo, Shi-Yong Zhang, Cheng-Hui Zeng, Zhong-Gao Zhou, Miao Xie, Zi-Yi Du, Chun-Ting He, Wei-Xiong Zhang, Xiao-Ming Chen
Summary: Free accessible confined space and loose interaction can be achieved in an ionic crystal (HMIm)(3)[La(NO3)(6)], which is composed of near-spherical anions and disc-shaped ammonium cations. The confined space of (HMIm)(+) ions can be finely tuned over a broad temperature range, allowing modulation of dipolar polarization. Small-scale substitution of (HMIm)(+) ions and fine-tuning of doping ratio in the molecular solid solutions further regulate the dipole motion in the crystalline environment.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Jia Zhang, Hao Chen, Shoujie Liu, Li-Dong Wang, Xue-Feng Zhang, Jun-Xi Wu, Li-Hong Yu, Xiao-Han Zhang, Shengliang Zhong, Zi-Yi Du, Chun-Ting He, Xiao-Ming Chen
Summary: Advances in single-atom catalysts provide a new solution for designing efficient electrocatalysts. This study demonstrates the use of molecule-spaced single-atom catalysts to significantly improve the active-site numbers and mass transfer. One of the molecule-spaced single-atom catalysts exhibits outstanding mass activity and long-term durability under industrial conditions for oxygen evolution reaction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
