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学者姓名：陈鸿铭
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Abstract ：
The architectural design and fabrication of low-cost, high-performance organic scintillators are critical for medical imaging and material/device analysis. However, achieving large-area and high-transparency organic scintillators in a low-cost and easy-to-implement method remains a challenge. Herein, a new design strategy for regulating the side chain length of maleimide derivatives is demonstrated to develop organic scintillators for achieving low-cost, large-area, and high spatial resolution in X-ray imaging. The effective intermolecular interactions and relatively twisted molecular structure endow PAM-M4 molecule with outstanding scintillator properties. More importantly, as demonstrated for the first time, pure organic glassy films with a diameter over 10 cm and high optical transparency can be prepared by the developed melt-quenched method using PAM-M4 crystal powder as a raw material. This glassy film exhibits excellent X-ray imaging ability with a spatial resolution as high as 27.0 lp mm-1 at MTF = 0.20, which is one of the best results among reported organic scintillators. The results of this work not only develop a new design strategy for high-performance organic scintillators but also demonstrate a reliable approach to fabricating large area screens with superior spatial resolution for medical or industrial X-ray imaging applications. A maleimide-based scintillator can be easily synthesized and exhibits a fast scintillation decay time of 12.38 ns, a high PLQY of 87.6%, and a low detection limit of 0.14 mu Gy s-1. By using the melt-quenched method, PAM-M4 crystal can turn into a large-area glassy film. This glassy film exhibits a transmittance of over 90%, along with a resolution of 27.0 lp mm-1 for X-ray imaging, which represents the state-of-the-art performance for organic scintillators. image
Keyword ：
fluorescence fluorescence maleimide derivatives maleimide derivatives organic glassy scintillators organic glassy scintillators X-ray imaging X-ray imaging
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| GB/T 7714 | Quan, Xin , Zhang, Guo-Zhen , Zhang, Yang et al. Low-Cost, Large-Area, and Highly Transparent Organic Glassy Scintillators for High Resolution X-Ray Imaging [J]. | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
| MLA | Quan, Xin et al. "Low-Cost, Large-Area, and Highly Transparent Organic Glassy Scintillators for High Resolution X-Ray Imaging" . | ADVANCED OPTICAL MATERIALS 12 . 18 (2024) . |
| APA | Quan, Xin , Zhang, Guo-Zhen , Zhang, Yang , Liao, Qing , Chen, Hong-Ming , Lin, Mei-Jin . Low-Cost, Large-Area, and Highly Transparent Organic Glassy Scintillators for High Resolution X-Ray Imaging . | ADVANCED OPTICAL MATERIALS , 2024 , 12 (18) . |
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Cuprous complex scintillators show promise for X-ray detection with abundant raw materials, diverse luminescent mechanisms, and adjustable structures. However, their synthesis typically requires a significant amount of organic solvents, which conflict with green chemistry principles. Herein, we present the synthesis of two high-performance cuprous complex scintillators using a simple mechanochemical method for the first time, namely [CuI(PPh3)(2)R] (R = 4-phenylpyridine hydroiodide (PH, Cu-1) and 4-(4-bromophenyl)pyridine hydroiodide (PH-Br, Cu-2). Both materials demonstrated remarkable scintillation performances, exhibiting radioluminescence (RL) intensities 1.52 times (Cu-1) and 2.52 times (Cu-2) greater than those of Bi4Ge3O12 (BGO), respectively. Compared to Cu-1, the enhanced RL performance of Cu-2 can be ascribed to its elevated quantum yield of 51.54%, significantly surpassing that of Cu-1 at 37.75%. This excellent luminescent performance is derived from the introduction of PH-Br, providing a more diverse array of intermolecular interactions that effectively constrain molecular vibration and rotation, further suppressing the nonradiative transition process. Furthermore, Cu-2 powder can be prepared into scintillator film with excellent X-ray imaging capabilities. This work establishes a pathway for the rapid, eco-friendly, and cost-effective synthesis of high-performance cuprous complex scintillators.
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| GB/T 7714 | Chen, Yue-Chen , Yuan, Si-Qi , Zhang, Guo-Zhen et al. Mechanochemical Synthesis of Cuprous Complexes for X-ray Scintillation and Imaging [J]. | INORGANIC CHEMISTRY , 2024 , 63 (7) : 3572-3577 . |
| MLA | Chen, Yue-Chen et al. "Mechanochemical Synthesis of Cuprous Complexes for X-ray Scintillation and Imaging" . | INORGANIC CHEMISTRY 63 . 7 (2024) : 3572-3577 . |
| APA | Chen, Yue-Chen , Yuan, Si-Qi , Zhang, Guo-Zhen , Di, Yi-Ming , Qiu, Qiang-Wen , Yang, Xi et al. Mechanochemical Synthesis of Cuprous Complexes for X-ray Scintillation and Imaging . | INORGANIC CHEMISTRY , 2024 , 63 (7) , 3572-3577 . |
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Correction for 'Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging' by Yu-Hua Chen et al., Chem. Sci., 2024, https://doi.org/10.1039/d4sc00735b.
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| GB/T 7714 | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging (20 Apr, 10.1039/d4sc00735b, 2024) [J]. | CHEMICAL SCIENCE , 2024 , 15 (21) : 8249-8249 . |
| MLA | Chen, Yu-Hua et al. "Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging (20 Apr, 10.1039/d4sc00735b, 2024)" . | CHEMICAL SCIENCE 15 . 21 (2024) : 8249-8249 . |
| APA | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai , Zhang, Shu-Quan , Fang, Xin , Chen, Hong-Ming et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging (20 Apr, 10.1039/d4sc00735b, 2024) . | CHEMICAL SCIENCE , 2024 , 15 (21) , 8249-8249 . |
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Phosphates are ideal candidates in the search for deep ultraviolet (DUV) nonlinear optical (NLO) materials due to their wide DUV transmission. However, the small optical anisotropy of the highly symmetric [PO4](3-) tetrahedron hinders phase matching (PM) in the DUV wavelength range. In this work, the polar tetrahedron [PO2(NHCONH2)(2)](-), which combines the pi-conjugated urea unit and the non-pi-conjugated [PO4](3-) unit via covalent bonds, is proposed as a new DUV NLO-active unit. [PO2(NHCONH2)(2)](-) tetrahedron exhibits greatly improved polarizability, anisotropy, and hyperpolarizability while maintaining a large highest occupied molecular orbital-lowest unoccupied molecular orbital gap. Accordingly, two DUV transparent alkali metal N, N-bis(aminocarbonyl)-phosphorodiamidates [A[PO2(NHCONH2)(2)] (A = K, Rb)] are screened out, and their nonlinear properties are systematically evaluated by first-principles methods. The results show that K[PO2(NHCONH2)(2)] (KPOU) achieves significant enhancements in multiple properties compared to the existing phosphate DUV NLO materials, including a strong SHG effect (3.44 x KDP) and the largest birefringence (0.088@532 nm) for DUV PM. Moreover, the shortest PM wavelength (lambda(PM)) of KPOU is 196 nm, making it a promising DUV NLO candidate for practical applications. This work proposes an excellent NLO-active unit and offers a new direction for exploring novel high-performance DUV NLO materials.
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| GB/T 7714 | Chen, Fuhai , Mo, Fuxiang , Chen, Hongming et al. KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]- Tetrahedra [J]. | CHEMISTRY OF MATERIALS , 2024 , 36 (6) : 2985-2992 . |
| MLA | Chen, Fuhai et al. "KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]- Tetrahedra" . | CHEMISTRY OF MATERIALS 36 . 6 (2024) : 2985-2992 . |
| APA | Chen, Fuhai , Mo, Fuxiang , Chen, Hongming , Lin, Mei-Jin , Chen, Yong . KPO2(NHCONH2)2: A Promising Deep-Ultraviolet Nonlinear Optical Phosphate Containing Polar [PO2(NHCONH2)2]- Tetrahedra . | CHEMISTRY OF MATERIALS , 2024 , 36 (6) , 2985-2992 . |
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Organic scintillators, pivotal in security and medical applications, face challenges due to limited X-ray absorption and exciton utilization. Herein, a novel class of organic scintillators is introduced, named guest-induced thermally activated delayed fluorescence (TADF) within supramolecular macrocycles via host-guest through-space charge transfer (TSCT). Four co-crystals are obtained through orthogonal crystallizations involving calix[3]acridan (C[3]A) and calix[3]phenothiazine (C[3]P) macrocycles as hosts, along with 1,2-dicyanobenzene (DCB) and 4-bromo-1,2-benzenedicarbonitrile (BrDCB) as guests. Interestingly, DCB@C[3]A and BrDCB@C[3]A co-crystals exhibit strong host-guest TSCT with reduced single-triplet energy gap for efficient TADF emission, which leads to enhanced exciton utilization and X-ray absorption, yielding radioluminescence intensities over 29 and 25 times higher than C[3]A. Similarly, substituting C[3]A with C[3]P, the obtained TADF co-crystals also outperform C[3]P in scintillation performance. Additionally, the scintillation color of co-crystals can be adjusted by varying the electron-donating abilities of macrocycles and the electron-accepting abilities of guests, offering a simpler color-tuning mechanism than covalent-bonded scintillators. Furthermore, the flexible film based on DCB@C[3]A exhibits promising application in X-ray radiography, showcasing a high spatial resolution of 20 lp mm-1 @MTF = 0.77. The innovative strategy of fabricating organic scintillators via reversible non-covalent interactions presents a novel solution for designing color-tunable and high-performance scintillators. The Table of Contents (TOC) image illustrates that novel organic supramolcular macrocycle scintillators with guest-induced TADF emission via host-guest through-space charge transfers, enabling efficient and color-tunable X-ray luminescence, as well as high-resolution imaging of 20 lp mm-1 in devices. image
Keyword ：
organic scintillators organic scintillators supramolecular macrocycles supramolecular macrocycles thermally activated delayed fluorescence thermally activated delayed fluorescence through-space charge transfers through-space charge transfers X-ray imaging X-ray imaging
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| GB/T 7714 | Zhang, Guozhen , Chen, Fuhai , Di, Yiming et al. Guest-Induced Thermally Activated Delayed Fluorescence Organic Supramolcular Macrocycle Scintillators for High-Resolution X-Ray Imaging [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (41) . |
| MLA | Zhang, Guozhen et al. "Guest-Induced Thermally Activated Delayed Fluorescence Organic Supramolcular Macrocycle Scintillators for High-Resolution X-Ray Imaging" . | ADVANCED FUNCTIONAL MATERIALS 34 . 41 (2024) . |
| APA | Zhang, Guozhen , Chen, Fuhai , Di, Yiming , Yuan, Siqi , Zhang, Yang , Quan, Xin et al. Guest-Induced Thermally Activated Delayed Fluorescence Organic Supramolcular Macrocycle Scintillators for High-Resolution X-Ray Imaging . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (41) . |
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Organic thermally activated delayed fluorescent (TADF) scintillators hold promising potential for applications in medical radiography and security detection, but the poor X-ray absorption ability and inferior radioluminescence (RL) hampered their progression. Herein, the study has pioneered the development of high-performance TADF Ag(I)-based scintillators from M2X2(dppb)2 (M = Ag, Cu; X = Cl, Br, I) complexes with 1,2-Bis(diphenylphosphino)benzene (dppb) ligand. In comparison with Cu(I) complexes, the Ag(I) series generally exhibited superior scintillation performance. Notably, Ag2Cl2(dppb)2 (Ag1) stands out with exceptionally high RL intensity (approximate to 125% higher than that of CsI:Tl) and a low detection limit of 59.8 nGy s-1. The outstanding scintillation performance of Ag1 is primarily attributed to the synergistic effect of the high exciton utilization efficiency origin from a small singlet-triplet energy gap, enhanced X-ray absorption capacity by heavy atoms, and the high photoluminescence quantum yield (76.47% in ambient atmosphere). By fabricating a flexible film constructed with Ag1 submicron crystalline powders, a high spatial resolution of 25.0 lp mm-1 for X-ray imaging is obtained. It offers new opportunities for utilizing TADF metal-organic complexes for highly efficient X-ray scintillation and imaging. Scintillators with good radioluminescence performance are prepared by combining the TADF mechanism to optimize the utilization of triplet excitons, coupled with increased X-ray absorption through heavy atoms, verifying the advantages of Ag(I)-halide complexes on radioluminescence. Besides, the influence of halogens on photoluminescence and radioluminescence are investigated. As a practical application, Ag2Cl2(dppb)2 is applied to fabricate flexible scintillator films, achieving high-resolution imaging of 25 lp mm-1. image
Keyword ：
scintillators scintillators silver-based complexes silver-based complexes thermally activated delayed fluorescence thermally activated delayed fluorescence X-ray imaging X-ray imaging
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| GB/T 7714 | Yuan, Siqi , Zhang, Guozhen , Chen, Fuhai et al. Thermally Activated Delayed Fluorescent Ag(I) Complexes for Highly Efficient Scintillation and High-Resolution X-Ray Imaging [J]. | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (33) . |
| MLA | Yuan, Siqi et al. "Thermally Activated Delayed Fluorescent Ag(I) Complexes for Highly Efficient Scintillation and High-Resolution X-Ray Imaging" . | ADVANCED FUNCTIONAL MATERIALS 34 . 33 (2024) . |
| APA | Yuan, Siqi , Zhang, Guozhen , Chen, Fuhai , Chen, Jingru , Zhang, Yang , Di, Yiming et al. Thermally Activated Delayed Fluorescent Ag(I) Complexes for Highly Efficient Scintillation and High-Resolution X-Ray Imaging . | ADVANCED FUNCTIONAL MATERIALS , 2024 , 34 (33) . |
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The development of high-quality organic scintillators encounters challenges primarily associated with the weak X-ray absorption ability resulting from the presence of low atomic number elements. An effective strategy involves the incorporation of halogen-containing molecules into the system through co-crystal engineering. Herein, we synthesized a highly fluorescent dye, 2,5-di(4-pyridyl)thiazolo[5,4-d]thiazole (Py2TTz), with a fluorescence quantum yield of 12.09%. Subsequently, Py2TTz was co-crystallized with 1,4-diiodotetrafluorobenzene (I2F4B) and 1,3,5-trifluoro-2,4,6-triiodobenzene (I3F3B) obtaining Py2TTz-I2F4 and Py2TTz-I3F3. Among them, Py2TTz-I2F4 exhibited exceptional scintillation properties, including an ultrafast decay time (1.426 ns), a significant radiation luminescence intensity (146% higher than Bi3Ge4O12), and a low detection limit (70.49 nGy s-1), equivalent to 1/78th of the detection limit for medical applications (5.5 mu Gy s-1). This outstanding scintillation performance can be attributed to the formation of halogen-bonding between I2F4B and Py2TTz. Theoretical calculations and single-crystal structures demonstrate the formation of halogen-bond-induced rather than pi-pi-induced charge-transfer cocrystals, which not only enhances the X-ray absorption ability and material conductivity under X-ray exposure, but also constrains molecular vibration and rotation, and thereby reducing non-radiative transition rate and sharply increasing its fluorescence quantum yields. Based on this, the flexible X-ray film prepared based on Py2TTz-I2F4 achieved an ultrahigh spatial resolution of 26.8 lp per mm, underscoring the superiority of this strategy in developing high-performance organic scintillators. Two organic halogen co-crystal scintillators with strong halogen-bond-induced charge-transfer interactions enable a fast response, low detection limit and ultra-high-resolution imaging.
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| GB/T 7714 | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging [J]. | CHEMICAL SCIENCE , 2024 , 15 (20) : 7659-7666 . |
| MLA | Chen, Yu-Hua et al. "Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging" . | CHEMICAL SCIENCE 15 . 20 (2024) : 7659-7666 . |
| APA | Chen, Yu-Hua , Zhang, Guo-Zhen , Chen, Fu-Hai , Zhang, Shu-Quan , Fang, Xin , Chen, Hong-Ming et al. Halogen-bonded charge-transfer co-crystal scintillators for high-resolution X-ray imaging . | CHEMICAL SCIENCE , 2024 , 15 (20) , 7659-7666 . |
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Rylene diimides are an attractive class of organic dyes owing to their exceptional optical properties and optoelectronic applications. Herein, we extend their applications to the realm of X-ray imaging. The emissive 1,1′-bi(2-naphthol-4,5-dicarboximide) (BiND-OH) and its phenyl/methyl derivatives, BiND-OPh and BiND-OMe, have been selected to investigate the structure-activity relationships between their crystal packing and X-ray scintillation properties. Single crystal X-ray diffraction results indicate that BiND-OH forms a tightly structured conformation with two interlocks by hydrogen bonding, leading to a charge transfer state and resulting in nearly non-scintillation. In contrast, the radioluminescence intensities of BiND-OPh and BiND-OMe have increased by about 73 and 537 times, respectively, owing to the disruption of hydrogen bonding control and the formation of a J-aggregation fraction dominated by π-π interactions. Remarkably, BiND-OMe displays superior scintillation properties, marked by reduced non-radiative transitions, attributed to greater π-π plane distances, extended slip distances, and diminished π-plane overlap areas. It demonstrates a low detection limit of 70.68 nGy s−1 and a short decay time of 4.37 ns. When applied to X-ray imaging, it produces a high spatial resolution of 11.0 lp mm−1. This finding provides valuable insights into the profound impact of molecular structure and aggregation state on the organic scintillation properties. (Figure presented.) © Science China Press 2024.
Keyword ：
crystal packing crystal packing fluorescence fluorescence molecular structures molecular structures organic scintillators organic scintillators X-ray imaging X-ray imaging
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| GB/T 7714 | Chen, J. , Liu, G. , Chen, F. et al. Binaphthol diimide scintillators for X-ray imaging; [用于X射线成像的联萘酚二酰亚胺闪烁体] [J]. | Science China Materials , 2024 , 67 (8) : 2583-2589 . |
| MLA | Chen, J. et al. "Binaphthol diimide scintillators for X-ray imaging; [用于X射线成像的联萘酚二酰亚胺闪烁体]" . | Science China Materials 67 . 8 (2024) : 2583-2589 . |
| APA | Chen, J. , Liu, G. , Chen, F. , Chen, Y. , Fang, X. , Chen, H. et al. Binaphthol diimide scintillators for X-ray imaging; [用于X射线成像的联萘酚二酰亚胺闪烁体] . | Science China Materials , 2024 , 67 (8) , 2583-2589 . |
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Energy storage devices with high power and energy density are in demand owing to the rapidly growing population, and lithium-ion batteries (LIBs) are promising rechargeable energy storage devices. However, there are many issues associated with the development of electrode materials with a high theoretical capacity, which need to be addressed before their commercialization. Extensive research has focused on the modification and structural design of electrode materials, which are usually expensive and sophisticated. Besides, polymer binders are pivotal components for maintaining the structural integrity and stability of electrodes in LIBs. Polyvinylidene difluoride (PVDF) is a commercial binder with superior electrochemical stability, but its poor adhesion, insufficient mechanical properties, and low electronic and ionic conductivity hinder its wide application as a high-capacity electrode material. In this review, we highlight the recent progress in developing different polymeric materials (based on natural polymers and synthetic non-conductive and electronically conductive polymers) as binders for the anodes and cathodes in LIBs. The influence of the mechanical, adhesion, and self-healing properties as well as electronic and ionic conductivity of polymers on the capacity, capacity retention, rate performance and cycling life of batteries is discussed. Firstly, we analyze the failure mechanisms of binders based on the operation principle of lithium-ion batteries, introducing two models of “interface failure” and “degradation failure”. More importantly, we propose several binder parameters applicable to most lithium-ion batteries and systematically consider and summarize the relationships between the chemical structure and properties of the binder at the molecular level. Subsequently, we select silicon and sulfur active electrode materials as examples to discuss the design principles of the binder from a molecular structure point of view. Finally, we present our perspectives on the development directions of binders for next-generation high-energy-density lithium-ion batteries. We hope that this review will guide researchers in the further design of novel efficient binders for lithium-ion batteries at the molecular level, especially for high energy density electrode materials. © 2024 The Royal Society of Chemistry.
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| GB/T 7714 | He, Q. , Ning, J. , Chen, H. et al. Achievements, challenges, and perspectives in the design of polymer binders for advanced lithium-ion batteries [J]. | Chemical Society Reviews , 2024 , 53 (13) : 7091-7157 . |
| MLA | He, Q. et al. "Achievements, challenges, and perspectives in the design of polymer binders for advanced lithium-ion batteries" . | Chemical Society Reviews 53 . 13 (2024) : 7091-7157 . |
| APA | He, Q. , Ning, J. , Chen, H. , Jiang, Z. , Wang, J. , Chen, D. et al. Achievements, challenges, and perspectives in the design of polymer binders for advanced lithium-ion batteries . | Chemical Society Reviews , 2024 , 53 (13) , 7091-7157 . |
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Organic fluorescence scintillators, owing to the ultrafast response time, versatile chemical structures, low processing temperature, and low cost, are considered as one of the promising materials for medical diagnostics, radiation detection, and X-ray astronomy. However, the low radioluminescence (RL) intensity and low sensitivity hinder their practical applications. In this work, a highly efficient organic fluorescent scintillator, 4,4 '-bis(9-carbazolyl)biphenyl (CBP), is presented, exhibiting a high X-ray RL intensity, narrow full width at half-maximum of 49 nm, and ultrafast decay time of 1.15 ns. More importantly, it has a low detection limit of 25.5 nGy s(-1), which is only 1/215 dose rate compared with the commercial X-ray diagnostics. Such an excellent scintillation performance is mainly attributed to its high photoluminescence quantum yield (PLQY = 61.92%) and good carrier transport (average hole mobility of 0.094 cm(2) V-1 s(-1)). By mixing the CBP into polydimethylsiloxane, the fabricated large area flexible film can be applied in X-ray radiography, which exhibits a high spatial resolution of 14.3 lp mm(-1) at MTF > 0.2. This work paves a way for the implementation of organic fluorescence dyes with high PLQY, high carrier mobility in efficient X-ray scintillation and imaging.
Keyword ：
carbazole derivatives carbazole derivatives fluorescence fluorescence organic scintillators organic scintillators X-ray imaging X-ray imaging
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| GB/T 7714 | Chen, Hongming , Lin, Miao , Zhao, Changbin et al. Highly Efficient, Low-Dose, and Ultrafast Carbazole X-Ray Scintillators [J]. | ADVANCED OPTICAL MATERIALS , 2023 , 11 (10) . |
| MLA | Chen, Hongming et al. "Highly Efficient, Low-Dose, and Ultrafast Carbazole X-Ray Scintillators" . | ADVANCED OPTICAL MATERIALS 11 . 10 (2023) . |
| APA | Chen, Hongming , Lin, Miao , Zhao, Changbin , Zhang, Dongwei , Zhang, Yang , Chen, Fuhai et al. Highly Efficient, Low-Dose, and Ultrafast Carbazole X-Ray Scintillators . | ADVANCED OPTICAL MATERIALS , 2023 , 11 (10) . |
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