Crystal Growth & Design最新文献

{"title":"Strategy for Regulation from Heterogeneous Nucleation to Homogeneous Nucleation: Application of Ultrasound","authors":"Rongxi Guo,&nbsp;Mengyang Cai,&nbsp;Jingjing Zhao,&nbsp;Pengpeng Yang,&nbsp;Hanjie Ying and Keke Zhang*,&nbsp;","doi":"10.1021/acs.cgd.4c0118010.1021/acs.cgd.4c01180","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c01180https://doi.org/10.1021/acs.cgd.4c01180","url":null,"abstract":"<p >In this study, the nucleation rate and the corresponding nucleation parameters were calculated by measuring the induction time of isonicotinamide (INA) in ethanol, and it was demonstrated that the nucleation of INA is controlled by kinetics. We found that ultrasound can control the nucleation rate of INA in different supersaturated INA–ethanol systems and play a promoting or inhibiting role. The underlying mechanism for those phenomena was supposed to be the jointly effects of ultrasonics, where the cavitation bubbles generated by ultrasonic pretreatment undergo rupture leading to the collision of solute molecules in solution or the dispersion of solute molecules, and the energy generated by ultrasonics can influence the intermolecular hydrogen bond interaction in solution. In addition, the introduction of ultrasonics was found to promote the nucleation mechanism transformation from heterogeneous nucleation to homogeneous nucleation, through the homogeneous dispersion of solute molecules in solution, which we believe to be due to the micromixing mechanism of the ultrasonic. The transition from heterogeneous nucleation to homogeneous nucleation through introduction of ultrasonics provides a feasible approach to avoid heterogeneous nucleation and promote homogeneous nucleation and also provides a new perspective for controlling the crystallization process.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585907","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Luminescent Organic Single Crystals for Flexible Optical Fiber Scintillators and X-ray Imaging","authors":"Huapeng Liu,&nbsp;Hongyun Wang,&nbsp;Shuyu Li,&nbsp;Qi Di,&nbsp;Lingsong Wang,&nbsp;Hongyu Zhang*,&nbsp;Xiaotao Zhang* and Wenping Hu,&nbsp;","doi":"10.1021/acs.cgd.4c0105710.1021/acs.cgd.4c01057","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c01057https://doi.org/10.1021/acs.cgd.4c01057","url":null,"abstract":"<p >Optical fiber-based glass scintillators are high-efficiency scintillators with excellent light collection and transmission properties. However, the performance of optical fiber scintillators is constrained by structural defects in silicate glass and reduced transparency due to doping. To overcome this limitation, we report a high-quality elastic crystal of a Schiff base, (<i>E</i>)-1-(((4-bromophenyl)imino)methyl)naphtha-len-2-ol (BPIN). The one-dimensional crystal exhibits exceptional elasticity and high fracture strength. The dominant π···π interactions and C–H···Br interactions in the crystal contribute significantly to the bending behavior. Moreover, owing to the heavy atom effect that enhances X-ray absorption capability, BPIN demonstrates outstanding scintillation performance with a fast radiative lifetime of 2.90 ns and low detection of 0.11 μGy_air s^–1. Based on the waveguiding and scintillation properties of BPIN, we propose a flexible crystal optical fiber scintillator. Furthermore, by expanding the crystal morphology to two dimensions, a high-resolution X-ray imaging screen is realized. Our study introduces an innovative approach for utilizing organic crystals in high-performance flexible X-ray detectors and imaging.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585908","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Structural Integrities of Symmetric and Unsymmetric trans-Bis-pyridyl Ethylene Powders Exposed to Gamma Radiation: Packing and Electronic Considerations Assisted by Electron Diffraction","authors":"Samantha J. Kruse,&nbsp;Pierre Le Magueres,&nbsp;Eric W. Reinheimer,&nbsp;Tori Z. Forbes and Leonard R. MacGillivray*,&nbsp;","doi":"10.1021/acs.cgd.4c0089510.1021/acs.cgd.4c00895","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c00895https://doi.org/10.1021/acs.cgd.4c00895","url":null,"abstract":"<p >Radiation detection (dosimetry) most commonly uses scintillating materials in a wide array of fields, ranging from energy to medicine. Scintillators must be able to not only fluoresce owing to the presence of a suitable chromophore but also withstand damage from radiation over prolonged periods of time. While it is inevitable that radiation will cause damage to the physical and chemical properties of materials, there is limited understanding of features within solid-state scintillators that afford increased structural integrity upon exposure to gamma (γ) radiation. Even fewer studies have evaluated both physical- and atomistic-level properties of organic solid-state materials. Previous work demonstrated cocrystalline materials afford radiation resistance in comparison to the single component counterparts, as realized by <i>trans</i>-1,2-bis(4-pyridyl)ethylene (<b>4,4′-bpe</b>). To support the rational design of radiation-resistant scintillators, we have examined all symmetric and unsymmetric isomers of <i>trans</i>-1-(<i>n</i>-pyridyl)2-(<i>m</i>-pyridyl)ethylene (<i>n,m</i>′<i>-</i>bpe, where <i>n</i> and/or <i>m</i> = 2, 3, or 4) solid-state crystalline materials. Experimental methods employed include single-crystal, powder, and electron diffraction as well as solid-state fluorimetry. Periodic density functional theory (DFT) calculations were used to understand the atomistic-level differences in bond lengths, bond orders, and packing. Electron diffraction was also utilized to determine the structure of a nanocrystalline sample. The results provide insights into possible trends involving factors such as molecular symmetry which provides radiation resistance as well as information for rationally designing single and multicomponent scintillators with the intent of minimizing changes upon γ-radiation exposure.</p><p >The introduction of ionizing radiation to the complete series <i>trans</i>-1-(<i>n</i>-pyridyl)2-(<i>m</i>-pyridyl)ethylenes (where <i>n</i> and/or <i>m</i> = 2, 3, 4) is used to assess structural stability and is determined to enhance fluorescence.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.cgd.4c00895","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585906","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-Throughput Screening, Crystal Structure Prediction, and Carrier Mobility Calculations of Organic Molecular Semiconductors as Hole Transport Layer Materials in Perovskite Solar Cells","authors":"Md Omar Faruque,&nbsp;Suchona Akter,&nbsp;Dil K. Limbu,&nbsp;Kathleen V. Kilway,&nbsp;Zhonghua Peng* and Mohammad R. Momeni*,&nbsp;","doi":"10.1021/acs.cgd.4c0096510.1021/acs.cgd.4c00965","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c00965https://doi.org/10.1021/acs.cgd.4c00965","url":null,"abstract":"<p >Using a representative translational dimer model, high throughput calculations are implemented for fast screening of a total of 74 diacenaphtho-extended heterocycle (DAH) derivatives as hole transport layer (HTL) materials in perovskite solar cells (PVSCs). Different electronic properties, including band structures, band gaps, and band edges compared to methylammonium and formamidinium lead iodide perovskites, along with reorganization energies, electronic couplings, and hole mobilities are calculated in order to decipher the effects of different parameters, including the polarity, steric and π-conjugation, as well as the presence of explicit hydrogen bond interactions on the computed carrier mobilities of the studied materials. Full crystal structure predictions and hole mobility calculations of the top candidates resulted in some mobilities exceeding 10 cm²/V·s, further validating the employed translational dimer model as a robust approach for inverse design and fast high-throughput screening of new HTL organic semiconductors with superior properties. The studied models and simulations performed in this work are instructive in designing next-generation HTL materials for higher-performance PVSCs.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585904","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"4-Nitro-phenylalanine Bromides: D−π–A Structural Features and Their Nonlinear and Linear Optical Properties","authors":"Gao-Yu Zhao*,&nbsp;Mao-Jing Tian,&nbsp;Rui-Xi Wang,&nbsp;Yan Deng,&nbsp;Yan-Ling Zhao,&nbsp;Shu-Chang Luo and Ling Chen*,&nbsp;","doi":"10.1021/acs.cgd.4c0122310.1021/acs.cgd.4c01223","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c01223https://doi.org/10.1021/acs.cgd.4c01223","url":null,"abstract":"<p >Nonlinear optical materials have important applications in optical communication, information processing, biomedicine, and other fields. Herein, two organic chiral 4-nitro-<span>d</span>(<span>l</span>)-phenylalanine bromides (4NDPAB and 4NLPAB) were successfully synthesized and fully characterized. Single-crystal X-ray diffraction data reveal the <i>P</i>2₁ non-centrosymmetric structure, in which the chiral cations and Br^– anions are linked through four intermolecular hydrogen bonds. Chirality is identified by circular dichroism spectroscopy. One enantiomer, 4NDPAB, is described as an example. It exhibits an absorption edge at 435 nm (<i>E</i>_g = 2.85 eV) and demonstrates a high thermal stability up to 230 °C. Additionally, 4NDPAB shows strong second harmonic generation (SHG), 1.8 times higher than that of commercial KDP, and large birefringence (Δ<i>n</i>_exp = 0.178). Density functional theoretical calculations and analyses confirm that the strong SHG intensity and excellent anisotropy performance are due to the D−π–A structural nature of 4-nitro-phenylalanine and its parallel crystal packing arrangement.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585905","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Charge-Tunable Bismuth-Hydroxamate Metal–Organic Frameworks for Photocatalytic Cr(VI) Mitigation","authors":"Chaozhi Xiong,&nbsp;Zhen-Wu Shao,&nbsp;Zhiyuan Zhang,&nbsp;Yue Dong,&nbsp;Li Xiong,&nbsp;Yuqing Qiu,&nbsp;Xiangping Duan,&nbsp;Yuxin Liu and Chong Liu*,&nbsp;","doi":"10.1021/acs.cgd.4c0117210.1021/acs.cgd.4c01172","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c01172https://doi.org/10.1021/acs.cgd.4c01172","url":null,"abstract":"<p >This study presents three bismuth-hydroxamate metal–organic frameworks (MOFs), namely, SUM-90A/B/C (SUM = Sichuan University Materials), prepared from Bi³⁺ and the same bridging ligand (1,4-benzenedihydroxamic acid). By varying the synthetic conditions, the charge states of the framework backbones and the coordination environments of the Bi³⁺ centers were finetuned, resulting in distinct structures and properties. The performances of MOFs as heterogeneous photocatalysts for Cr(VI) mitigation were comparatively studied, using both theoretical and experimental methods, and they exhibited remarkable kinetic stability in aqueous media and varied electronic structures. Specifically, SUM-90C, with an experimental band gap of 1.92 eV, was identified as a promising photocatalyst that could effectively convert Cr(VI) within 4 h and retain 96% of its capability over 3 cycles.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585851","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Viologen-Based MOF: Photoresponsive Discoloration Property and Selective Fluorescence Detection of Nitrofurans and Lysine","authors":"Shi Zhang,&nbsp;Yanping Zhao,&nbsp;Ying Wang,&nbsp;Guojian Chen,&nbsp;Qingfu Zhang,&nbsp;Yanli Gai* and Kecai Xiong*,&nbsp;","doi":"10.1021/acs.cgd.4c0122610.1021/acs.cgd.4c01226","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c01226https://doi.org/10.1021/acs.cgd.4c01226","url":null,"abstract":"<p >A metal–organic framework featuring a 3-fold interpenetrating diamondoid structure has been constructed utilizing a viologen derivative, 1,1′-bis(4-carboxyphenyl)-(4,4′-bipyridinium) dichloride. This compound demonstrates good performance as a multifunctional colorimetric and fluorescence sensor. The incorporation of viologen imparts the compound with a visible photoresponsive discoloration property. Furthermore, this compound exhibits the ability to detect nitrofurans and lysine through fluorescence turn-off and turn-on mechanisms, respectively.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585850","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Role of Molecular Packing in Solvent-Mediated Ellagic Acid·Phenazine Co-Crystals Toward Biological Activity Enhancement and Rational Drug Design","authors":"Jianghu Chen,&nbsp;Chunhua Qiu,&nbsp;Haohong Li and Xiaochun Zheng*,&nbsp;","doi":"10.1021/acs.cgd.4c0080510.1021/acs.cgd.4c00805","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c00805https://doi.org/10.1021/acs.cgd.4c00805","url":null,"abstract":"<p >Ellagic acid (EA), a biologically active polyphenol abundant in various natural plants, has been widely applied in diverse pharmacological systems. This study investigates cocrystals formed by EA with common pharmaceutical intermediates, yielding crucial insights into their atomic-level biological performance. Three novel cocrystals of EA·Phenazine were synthesized in different solvents (cocrystal <b>1</b>: EA·Phenazine; cocrystal <b>2</b>: EA·Phenazine·2MeOH; cocrystal <b>3</b>: EA·Phenazine·2H₂O). In addition, their structures are characterized using single-crystal X-ray diffraction. Co-crystal <b>1</b> without lattice solvent and cocrystal <b>3</b> containing lattice H₂O, exhibited intriguing EA–EA and phenazine–phenazine π–π stacking interactions. Conversely, cocrystal <b>2</b> bearing methanol can illustrate robust interligand EA/phenazine π–π stacking interactions. Thus, cocrystal <b>2</b> displayed a wider absorption range and a more negative oxidation potential, indicative of enhanced functional performance. The superior properties of cocrystal <b>2</b> were attributed to the lower energy level of the lowest unoccupied molecular orbital, particularly the p−π* antibonding orbitals of phenazine, owing to the potent π–π interactions, as unveiled by theoretical calculations. In summary, the presence of interligand interactions emerges as a pivotal factor in augmenting the biological activities of cocrystals, with the extent of enhancement contingent on specific packing modes. This structure–property relationship allows a profound understanding of the polymorphism observed in drug molecules.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"On the Design of the Metal–Support Interface in Methanol Electrocatalytic Oxidation","authors":"Bartłomiej M. Szyja*,&nbsp; and ,&nbsp;Joanna Zasada,&nbsp;","doi":"10.1021/acs.cgd.3c0146610.1021/acs.cgd.3c01466","DOIUrl":"https://doi.org/10.1021/acs.cgd.3c01466https://doi.org/10.1021/acs.cgd.3c01466","url":null,"abstract":"<p >In this work, we present a theoretical investigation of the SrTiO₃ perovskite-supported Pd catalyst in the methanol electro-oxidation reaction. In order to determine the metal–support interactions, we designed a system consisting of a Pd (100) double layer supported on one of the two possible terminations of the (100) perovskite surface. These terminations are characterized by different reducibilities of the layers directly interacting with the Pd bilayer and result in the difference in the stability of the surface-bound intermediates. Despite the fact that the Pd surface is identical in terms of geometry, we observed significant differences in the overpotential required for the reaction; in the case of TiO₂ termination, the overpotential has been determined to be 0.68 V, while in the case of SrO termination, it amounts to as much as 1.35 V. We further investigate the charge transfers within the components of the system and the geometries of the intermediates to unravel the role of the electron structure on the overall efficiency of the process.</p><p >This work investigates a SrTiO₃ perovskite-supported Pd catalyst for methanol electro-oxidation. A Pd (100) double layer is supported on two surface terminations (TiO₂ and SrO), leading to different reaction overpotentials. Despite identical Pd geometry, TiO₂ termination shows a lower overpotential compared to SrO. The study analyzes charge transfers and intermediate structures to understand the impact of the electronic structure on reaction efficiency.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.cgd.3c01466","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585690","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Microfluidic Synthesis of Defective and Hierarchical Pore Zr Metal–Organic Framework Materials and CO2 Adsorption Performance Study","authors":"Xuehui Ge,&nbsp;Zihan Liu,&nbsp;Nanjie Wei,&nbsp;Xiaocheng Lin* and Cejun Hu*,&nbsp;","doi":"10.1021/acs.cgd.4c0110610.1021/acs.cgd.4c01106","DOIUrl":"https://doi.org/10.1021/acs.cgd.4c01106https://doi.org/10.1021/acs.cgd.4c01106","url":null,"abstract":"<p >Microfluidic synthesis has emerged as a promising method for synthesizing metal–organic frameworks (MOFs). It overcomes the limitations of the traditional solvothermal method to regulate the structure and function of the MOFs. This study synthesized various MOFs with different structures and functions by controlling the reaction time and the ratio of metal ions to organic ligands through microfluidics and investigated their CO₂ adsorption properties. The results showed that the microfluidic synthesized defective and hierarchical pore MOF-808 improved the adsorption performance of CO₂ by nearly 110% and 30%, respectively, compared with solvothermal synthesized MOF-808.</p>","PeriodicalId":34,"journal":{"name":"Crystal Growth & Design","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585689","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}