摘要：
The exploration of the structure and properties of the luminescent materials in OLED devices using Multiple Resonance Thermally Activated Delayed Fluorescence (MR-TADF) is constrained by challenges related to long cycles and high experimental costs, making it a key obstacle in the development of new materials. In response to this challenge, we propose an innovative approach by constructing a graph convolutional neural network model named SOGCN to quickly determine whether an unsynthesized material has the potential to become an MR material, and accurately predict its energy gap and half-peak width, thereby expediting the development process of MR-TADF materials. We constructed the MR220 dataset for training the model based on 220 MR-TADF molecules reported in experiments. To ensure the reliability of the SOGCN model in predicting new samples, we have established a rigorous set of theoretical calculation evaluation standards, providing crucial references for the model. In the prediction of the properties of 37 new samples of MR-TADF molecules, SOGCN successfully predicted the singlet-triplet energy gap (LEST) of some samples, demonstrating a good trend in FWHM prediction as well. Finally, we have synthesized our designed molecule, Design3 (DtCzB-Boz), the organic light-emitting diodes based on DtCzB-Boz exhibit an emission peak at 508 nm, with the FWHM is 27 nm. The result of photophysical characterization is highly consistent with the predicted value of SOGCN. Notably, the mean absolute errors (MAE) between our model predictions and experimental/computational values were as low as 0.037 eV and 10 nm, respectively. This indicates that SOGCN exhibits higher efficiency and accuracy in predicting the properties of MR-TADF materials.
摘要：
Green tea is one of people's favorite drinks. However, pesticide residues in green tea can cause harm to the human body, and therefore, detection of pesticide residues in green tea is very important. In recent years, the detection of pesticide residues in tea has become a research hotspot. In this paper, a gas chromatography-mass spectrometry/mass spectrometry (GC-MS/MS) detection method of tolfenpyrad pesticide residues in green tea was established by using acetonitrile extractant, dispersive solid-phase extraction purification, temperature programming and application retention time lock with the database. After the sample was extracted with acetonitrile, then the sample was purified by QuEChERS extraction purification tube, afterward isomer B was used as the internal standard for the determination by multiple reaction monitoring mode (MRM) of GC-MS/MS. The results indicated that the experimental data accorded with the criterion on quality control of laboratoris(chemical testing of food), and the requirements of recovery, calibration curve, precision.This method was used to detect tolfenpyrad residues in actual green tea samples in multiple batches, and the satisfactory results were obtained.
作者机构：
[Qun-Yan Wu; Lei Mei; Li-Wen Zeng; Zhi-Wei Huang; Ji-Pan Yu; Zhi-Fang Chai; Kong-Qiu Hu; Wei-Qun Shi] Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049;[Chang-Ming Nie] School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001;[John K. Gibson] Chemical Sciences Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, California 94720;[Xiang-He Kong] Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001
作者机构：
[Shao, Dadong; Ouyang, Jiafeng; Shao, DD] Nanjing Univ Sci & Technol, Sch Environm & Biol Engn, Nanjing 210094, Peoples R China.;[Ouyang, Jiafeng; Yuan, Liyong; Shi, Weiqun; Guo, Wenlu; Wang, Lin] Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China.;[Guo, Wenlu; Nie, Changming] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.
通讯机构：
[Shao, DD ] N;[Yuan, LY ] C;Nanjing Univ Sci & Technol, Sch Environm & Biol Engn, Nanjing 210094, Peoples R China.;Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China.
关键词：
magnetic nanoparticle;3D mesoporous silica;amino functionalization;adsorption of U(VI);acid resistance
摘要：
Although mesoporous silica with magnetically hybridized two-dimensional channel structures has been well studied in recent years, it remains a challenge to fabricate the counterpart with macroporous three-dimensional cubic structures since the highly acidic preparation conditions lead to dissolution of magnetic particles. Herein, we successfully prepared magnetic KIT-6 nano-composite and its amino derivatives by bearing acid-resistant iron oxide. The prepared materials exhibited excellent properties for U(VI) ions removal from aqueous solutions under various conditions. The experimental data show that the U(VI) adsorption features fast adsorption kinetics, high adsorption capacity and ideal selectivity toward U(VI). The adsorption process is of spontaneous and endothermic nature and ionic strength independence, and the adsorbents can be easily regenerated by acid treatment. Compared to pristine KIT-6, the introduction of magnetism does not reduce the efficiency of the material to remove U(VI) while exerting its role as a recovery adsorbent. The findings of this work further demonstrate the potential broad application prospects of magnetic hybrid mesoporous silica in radionuclide chelation.
期刊：
Nuclear Engineering and Technology,2023年55(7):2556-2566 ISSN：1738-5733
通讯作者：
Nie, CM;Shi, WQ
作者机构：
[Liang, Ru-Ting; Nie, Chang-Ming; Nie, CM; Yin, Wan-Qiu] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;[Liang, Ru-Ting; Bo, Tao; Yin, Wan-Qiu; Zhang, Lei; Chai, Zhi-Fang] Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Engn Lab Adv Energy Mat, Ningbo 315201, Zhejiang, Peoples R China.;[Bo, Tao] Songshan Lake Mat Lab, Dongguan 523808, Guangdong, Peoples R China.;[Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
通讯机构：
[Nie, CM ] U;[Shi, WQ ] C;Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Hunan, Peoples R China.;Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
作者机构：
[Lei, Xia-Ping; Nie, Chang-Ming] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Wu, Qun-Yan; Chai, Zhi-Fang; Wang, Cong-Zhi; Lan, Jian-Hui; Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
通讯机构：
[Qun-Yan Wu; Wei-Qun Shi] L;[Chang-Ming Nie] S;Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
期刊：
JOURNAL OF PHYSICAL CHEMISTRY A,2022年126(22):3445-3451 ISSN：1089-5639
通讯作者：
Nie, Chang-Ming(changmingnie@usc.edu.cn);Wang, Cong-Zhi(wangcongzhi@ihep.ac.cn);Shi, Wei-Qun(shiwq@ihep.ac.cn)
作者机构：
[Wang, Juan; Wang, Cong-Zhi; Shi, Wei-Qun] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Nie, Chang-Ming; Wu, Qun-Yan; Wang, Juan; Chai, Zhi-Fang; Lan, Jian-Hui] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
通讯机构：
[Cong-Zhi Wang; Wei-Qun Shi] L;[Chang-Ming Nie] S;Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China<&wdkj&>School of Chemistry and Chemical Engineering, University of South China, Hengyang 421001, China
关键词：
Chemical bonds;Density functional theory;Actinide metals;Boron clusters;Cluster-based;Density-functional-theory;Double ring;Effective approaches;Global minimum;Metal-doping;Orbitals;Tubulars;Metals
作者机构：
[Zhang, Nai-Xin; Nie, Chang-Ming; Li, Ai-Lin] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Zhang, Nai-Xin; Wu, Qun-Yan; Chai, Zhi-Fang; Wang, Cong-Zhi; Lan, Jian-Hui; Shi, Wei-Qun; Li, Ai-Lin] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;[Chai, Zhi-Fang] Chinese Acad Sci, Ningbo Inst Ind Technol, Engn Lab Nucl Energy Mat, Ningbo 315201, Zhejiang, Peoples R China.
通讯机构：
[Qun-Yan Wu; Wei-Qun Shi] L;Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
关键词：
Actinides;Atoms;Binary alloys;Binding energy;Bond length;Crystal atomic structure;Density functional theory;Electron affinity;Electronic structure;Electrons;Oxidation;Plutonium alloys;Quantum theory;Synthesis (chemical);Bond length variation;Donor-acceptor interaction;Electron localization function;Lone pair electrons;Quantum Theory of Atoms in Molecules;Reduction reaction;Relativistic density functional theory;Synergistic effect;Silicon compounds
期刊：
PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2021年23(47):26967-26973 ISSN：1463-9076
通讯作者：
Wang, Cong-Zhi;Shi, Wei-Qun
作者机构：
[Zhang, Nai-Xin; Wu, Qun-Yan; Wang, Cong-Zhi; Shi, Wei-Qun; Wang, Juan; Chai, Zhi-Fang; Lan, Jian-Hui] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;[Nie, Chang-Ming; Wang, Juan] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Chai, Zhi-Fang] Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Engn Lab Adv Energy Mat, Ningbo 315201, Peoples R China.
通讯机构：
[Wang, CZ; Shi, WQ] C;Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
摘要：
The exploration of metal-doped boron clusters has a great significance in the design of high coordination number (CN) compounds. Actinide-doped boron clusters are probable candidates for achieving high CNs. In this work, we systematically explored a series of actinide metal atom (U, Np, and Pu) doped B(20) boron clusters An@B(20) (An = U, Np, and Pu) by global minimum structural searches and density functional theory (DFT). Each An@B(20) cluster is confirmed to be a twenty-coordinate complex, which is the highest CN obtained in the chemistry of actinide-doped boron clusters so far. The predicted global minima of An@B(20) are tubular structures with actinide atoms as centers, which can be considered as boron molecular drums. In An@B(20), U@B(20) has a relatively high symmetry of C(2), while both Np@B(20) and Pu@B(20) exhibit C(1) symmetry. Extensive bonding analysis demonstrates that An@B(20) has σ and π delocalized bonding, and the U-B bonds possess a relatively higher covalency than the Np-B and Pu-B bonds, resulting in the higher formation energy of U@B(20). Therefore, the covalent character of An-B bonding may be crucial for the formation of these high CN actinide-centered boron clusters. These results deepen our understanding of actinide metal doped boron clusters and provide new clues for developing stable high CN boron-based nanomaterials.
作者机构：
[Mei, Lei; Wu, Qun-Yan; Hu, Kong-Qiu; Li, Ailin; Zeng, Li-Wen; Liu, Kang; Kong, Xiang-He; Chai, Zhi-Fang; Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;[Nie, Chang-Ming; Li, Ailin; Kong, Xiang-He] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Chai, Zhi-Fang] Chinese Acad Sci, Ningbo Inst Ind Technol, Engn Lab Adv Energy Mat, Ningbo 315201, Zhejiang, Peoples R China.
通讯机构：
[Kong-Qiu Hu; Wei-Qun Shi] L;Laboratory of Nuclear Energy Chemistry, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
摘要：
A novel two-dimensional double-layer anionic uranyl-organic framework, U-TBPCA {[NH(2)(CH(3))(2)][(UO(2))(TBPCA)], where H(3)TBPCA = 4,4',4″-s-triazine-1,3,5-triyltripamino-methylene-cyclohexane-carboxylate}, with abundant active sites and stability was obtained by assembling UO(2)(NO(3))(2)·6H(2)O and a triazine tricarboxylate linker, TBPCA(3-). Due to the flexibility of the ligand and diverse coordination modes between carboxyl groups and uranyl ions, U-TBPCA exhibits an intriguing topological structure and steric configuration. This double-layer anionic uranyl-organic framework is highly porous and can be used for selective adsorption of cationic dyes. Due to the presence of high-density metal ions and basic -NH- groups, U-TBPCA acts as an effective heterogeneous catalyst for the cycloaddition reaction of carbon dioxide with epoxy compounds. Moreover, the various modes of coordination between the tricarboxylic ligand and uranyl ion were studied by density functional theory calculations, and several simplified models were established to probe the influence of hydrogen bonding between carbon dioxide and U-TBPCA on the ability of U-TBPCA to bind carbon dioxide. This work should aid in improving our understanding of the coordination behavior of uranyl ion as well as the development and utilization of new actinide materials.
作者机构：
[Mei, Lei; Hu, Kongqiu; Shi, WQ; Shi, Weiqun; Kong, Xianghe; Wu, Qunyan; Yu, Jipan] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.;[Kong, Xianghe; Nie, Changming] Univ South China, Sch Chem & Chem Engn, Hengyang 421001, Peoples R China.;[Huang, Zhiwei; Chai, Zhifang] Chinese Acad Sci, Ningbo Inst Ind Technol, Engn Lab Adv Energy Mat, Ningbo 315201, Zhejiang, Peoples R China.
通讯机构：
[Hu, KQ; Shi, WQ] C;Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.
摘要：
Herein we present a new metalloligand, Th(6)L(12) [IHEP-10; L = 4-pyrazolecarboxylic acid (H(2)PyC)], which can be used to generate a novel multicomponent heterometallic metal-organic framework (MOF), [[Cu(3)(μ(3)-OH)(NO(3))(H(2)O)(2)](2)Th(6)(μ(3)-O)(4)(μ(3)-OH)(4)(PyC)(6)(HPyC)(6)(H(2)O)(6)](NO(3))(2) (IHEP-11), through further assembly with second [Cu(3)(μ(3)-OH)(PyC)(3)] clusters. In IHEP-11, six Cu(3) clusters are connected by six NO(3)(-) anions to form an unprecedented annular Cu(18) cluster, which can be viewed as a 12-connected node to link with 12 Th(6) clusters, resulting a 4,12-connected shp net. Benefiting from the cationic framework and 3D porous structure, IHEP-11 can efficiently remove ReO(4)(-) (an analogue of radioactive (99)TcO(4)(-)) from aqueous solution in a wide pH range. This work highlights the feasibility of constructing multicomponent MOFs through a step-by-step synthesis strategy based on metalloligands.
