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学者姓名：郑彦臻
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Abstract ：
Here we use a pseudoallyl ligand, N,N '-chelating amidinate (Am), together with pentamethylcyclopentadienyl (Cp*) to give two dysprosium(III) single-molecule magnets (SMMs): [{(AmiPr)-DyCp*(mu-Cl)}2] and [AmdippDyCp*(Cl)(mu-Cl)Li(THF)3] with dis-tinct energy barriers (Ueff) of 97 and 472 K, respectively. The latter Ueff value is similar to the homoleptic Cp*-based Dy-SMM.
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| GB/T 7714 | Wang, Yidian , Luo, Qian-Cheng , Zhai, Yuan-Qi et al. Heteroleptic Dysprosium(III) Single-Molecule Magnets with Amidinate and Cyclopentadienyl Ligands [J]. | CRYSTAL GROWTH & DESIGN , 2022 , 22 (11) : 6398-6404 . |
| MLA | Wang, Yidian et al. "Heteroleptic Dysprosium(III) Single-Molecule Magnets with Amidinate and Cyclopentadienyl Ligands" . | CRYSTAL GROWTH & DESIGN 22 . 11 (2022) : 6398-6404 . |
| APA | Wang, Yidian , Luo, Qian-Cheng , Zhai, Yuan-Qi , Jin, Peng-Bo , Fu, Zhendong , Sun, Qi et al. Heteroleptic Dysprosium(III) Single-Molecule Magnets with Amidinate and Cyclopentadienyl Ligands . | CRYSTAL GROWTH & DESIGN , 2022 , 22 (11) , 6398-6404 . |
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Abstract ：
Due to the industrial requirements for high production and high quality of ethylene, efficient purification of ethylene from acetylene and ethane is of prime importance but challenging. Dynamic metal-organic frameworks (MOFs) have demonstrated intriguing structural dynamics and diverse applications recently. Among them, although a few flexible ones have exhibited interesting ethylene purification capability, rigid ones were yet barely investigated for such purpose. In this regard, a cerium(III)-based MOF was solvothermally synthesized, which is rigid and assembled from rod molecular building blocks associated with coordinative N,N-dimethylformamide (DMF) molecules. After liberating different degrees of DMF ligands via heating under vacuum or acetone exchange, both partially desolvated compounds of Ce-MOF-1 and Ce-MOF-2 were concertedly isolated in a fashion of single-crystal to single-crystal transformation. Although both newly generated materials crystallize in the same space group, they exhibit dissimilar unit cell parameters and slightly distinct ultramicropore sizes and pore microenvironments, thanks to the discrepancy in the desolvation degree. Consequently, Ce-MOF-1 and Ce-MOF-2 individually demonstrate C2H2- and C2H6-selective adsorption behavior, resulting in the potential tandem separation of C2H4 from C2H2 and C2H6 mixtures. The above results were successfully supported by not only single gas adsorption isotherms but also grand canonical Monte Carlo (GCMC) calculation studies and dynamic breakthrough experiments. The present work may pave the way for rigid MOFs aiming at advancing applications via solid-state structural dynamics.
Keyword ：
adsorptive separation dynamic metal-organic frameworks ethylene purification single-crystal to single-crystal transformation structural dynamics
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| GB/T 7714 | Fang, Han , Zheng, Bin , Zhang, Zong-Hui et al. Desolvation-Degree-Induced Structural Dynamics in a Rigid Cerium-Organic Framework Exhibiting Tandem Purification of Ethylene from Acetylene and Ethane [J]. | ACS APPLIED MATERIALS & INTERFACES , 2022 . |
| MLA | Fang, Han et al. "Desolvation-Degree-Induced Structural Dynamics in a Rigid Cerium-Organic Framework Exhibiting Tandem Purification of Ethylene from Acetylene and Ethane" . | ACS APPLIED MATERIALS & INTERFACES (2022) . |
| APA | Fang, Han , Zheng, Bin , Zhang, Zong-Hui , Jin, Peng-Bo , Li, Hong-Xin , Zheng, Yan-Zhen et al. Desolvation-Degree-Induced Structural Dynamics in a Rigid Cerium-Organic Framework Exhibiting Tandem Purification of Ethylene from Acetylene and Ethane . | ACS APPLIED MATERIALS & INTERFACES , 2022 . |
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Abstract ：
A family of fully sandwiched arachno-lanthanacarborane complexes formulated as {eta(6)-[mu-1,2-[o-C6H4(CH2)(2)]-1,2-C2B10H10](2)Ln}{Li-5(THF)(10)} (Ln =Tb, Dy, Ho, Er, Y) is successfully synthesized, where the "carbons-adjacent" carboranyl ligand (arachno-R-2-C2B10H104-) bears four negative charges and coordinates to the central lanthanide ions using the hexagonal eta(C2B4)-C-6 face. Thus, the central lanthanide cations are pseudo-twelve-coordinate and have an approximate pseudo-D-6h symmetry or hexagonal-prismatic geometry. As the crystal field effect imparted by this geometry is still unknown, we thoroughly investigated the magnetic properties of this series of complexes and found that the crystal field imposed by this ligand causes a relation of Tb > Dy > Ho > Er for the energy gaps between the ground and the first excited states, which is of striking resemblance to the ferrocenophane and phthalocyanine ligands although the latter two ligands give disparate local coordination geometries. Moreover, the effective energy barrier to magnetization reversal of 445(10) K, the observable hysteresis loop up to 4 K and the relaxation time of the yttrium-diluted sample reaching 193(17) seconds at 2 K under an optimized field for the Tb analogue of this family of arachno-lanthanacarborane complexes, render a new benchmark for Tb3+-based single-molecule magnets.
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| GB/T 7714 | Jin, Peng-Bo , Yu, Ke-Xin , Luo, Qian-Cheng et al. Tetraanionic arachno-Carboranyl Ligand Imparts Strong Axiality to Terbium(III) Single-Molecule Magnets [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2022 , 61 (29) . |
| MLA | Jin, Peng-Bo et al. "Tetraanionic arachno-Carboranyl Ligand Imparts Strong Axiality to Terbium(III) Single-Molecule Magnets" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 61 . 29 (2022) . |
| APA | Jin, Peng-Bo , Yu, Ke-Xin , Luo, Qian-Cheng , Liu, Ye-Ye , Zhai, Yuan-Qi , Zheng, Yan-Zhen . Tetraanionic arachno-Carboranyl Ligand Imparts Strong Axiality to Terbium(III) Single-Molecule Magnets . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2022 , 61 (29) . |
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Abstract ：
Comprehensive Summary Molecules with long preserved magnetic moments are perceived as the smallest units for storing bytes, which could bring a new revolution for information technology. However, the rational design of such molecules remains challenging. Here two rigid adamantanol ligand based dysprosium(III) complexes ([Dy(1-AdO)(2)(py)(5)]BPh4 - 1 and [Dy(2-AdO)(2)(py)(5)]BPh4 - 2) with pentagonal-bipyramidal coordination geometry and local D-5h symmetry were successfully prepared, which display excellent single-molecule magnet (SMM) behavior (U-eff approximate to 1835 K, T-B(ZFC) approximate to 24 K, T-B(100s) approximate to 17 K and T-B(H) = 23 K for 1; U-eff approximate to 1756 K, T-B(ZFC) approximate to 20 K, T-B(100s) approximate to 16 K and T-B(H) = 23 K for 2) due to the much weakened vibration in low energy regimes. Remarkably, the large energy barriers and high blocking temperatures for these two complexes in solid states are well preserved in solution. This is never observed in previous studies of SMMs, indicating that the adamantanol is rigid and can be introduced to make the composed molecules stable enough to maintain the solid state magnetic property in solution.
Keyword ：
D-5h-symmetry Lanthanide Molecular magnets Solution Superparamagnetism
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| GB/T 7714 | Ding, Xiali , Luo, Qiancheng , Zhai, Yuanqi et al. Rigid Dysprosium(III) Single-Molecule Magnets Exhibit Preserved Superparamagnetism in Solution [J]. | CHINESE JOURNAL OF CHEMISTRY , 2022 , 40 (5) : 563-570 . |
| MLA | Ding, Xiali et al. "Rigid Dysprosium(III) Single-Molecule Magnets Exhibit Preserved Superparamagnetism in Solution" . | CHINESE JOURNAL OF CHEMISTRY 40 . 5 (2022) : 563-570 . |
| APA | Ding, Xiali , Luo, Qiancheng , Zhai, Yuanqi , Zhang, Xufeng , Lv, Yi , Zhang, Xinliang et al. Rigid Dysprosium(III) Single-Molecule Magnets Exhibit Preserved Superparamagnetism in Solution . | CHINESE JOURNAL OF CHEMISTRY , 2022 , 40 (5) , 563-570 . |
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Abstract ：
Data carriers using spin waves in spintronic and magnonic logic devices offer operation at low power consumption and free of Joule heating yet requiring noncollinear spin structures of small sizes. Heterometallic rings can provide such an opportunity due to the controlled spin-wave transmission within such a confined space. Here, we present a series of {ScnGdn} (n = 4, 6, 8) heterometallic rings, which are the first Sc-Ln clusters to date, with tunable magnetic interactions for spin-wave excitations. By means of time- and temperature-dependent spin dynamics simulations, we are able to predict distinct spin-wave excitations at finite temperatures for Sc4Gd4, Sc6Gd6, and Sc8Gd8. Such a new model is previously unexploited, especially due to the interplay of antiferromagnetic exchange, dipole-dipole interaction, and ring topology at low temperatures, rendering the importance of the latter to spin-wave excitations.
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| GB/T 7714 | Zhang, Hao-Lan , Zhai, Yuan-Qi , Nojiri, Hiroyuki et al. {ScnGdn} Heterometallic Rings: Tunable Ring Topology for Spin-Wave Excitations [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2022 , 144 (33) : 15193-15202 . |
| MLA | Zhang, Hao-Lan et al. "{ScnGdn} Heterometallic Rings: Tunable Ring Topology for Spin-Wave Excitations" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 144 . 33 (2022) : 15193-15202 . |
| APA | Zhang, Hao-Lan , Zhai, Yuan-Qi , Nojiri, Hiroyuki , Schroeder, Christian , Hsu, Hung-Kai , Chan, Yi-Tsu et al. {ScnGdn} Heterometallic Rings: Tunable Ring Topology for Spin-Wave Excitations . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2022 , 144 (33) , 15193-15202 . |
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Abstract ：
The fast Raman relaxation process via a virtual energy level has become a puzzle for how to chemically engineer single-molecule magnets (SMMs) with better performance. Here, we use the trifluoromethyl group to systematically substitute the methyl groups in the axial position of the parent bis-butoxide pentapyridyl dysprosium(III) SMM. The resulting complexes-[Dy(OLA)(2)py(5)][BPh4] (L-A=CH(CF3)(2)(-) 1, CH2CF3- 2, CMe2CF3- 3)-show progressively enhanced T-B(hys) (@100 Oe s(-1)) from 17 K (for 3), 20 K (for 2) to 23 K (for 1). By experimentally identifying the varied under barrier relaxation energy in the 5-500 cm(-1) regime, we are able to identify that the C-F bond related vibration energy of the axial ligand ranging from 200 to 350 cm(-1) is the key variant for this improvement. Thus, this finding not only reveals a correlation between the structure and the Raman process but also provides a paradigm for how to apply the vibronic barrier model to analyze multi-phonon relaxation processes in lanthanide SMMs.
Keyword ：
Lanthanides Raman Process Single-Molecule Magnets Two-Phonon Relaxation Vibronic Barrier Model
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| GB/T 7714 | Ma, Yan , Zhai, Yuan-Qi , Luo, Qian-Cheng et al. Ligand Fluorination to Mitigate the Raman Relaxation of Dy-III Single-Molecule Magnets: A Combined Terahertz, Far-IR and Vibronic Barrier Model Study [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2022 , 61 (26) . |
| MLA | Ma, Yan et al. "Ligand Fluorination to Mitigate the Raman Relaxation of Dy-III Single-Molecule Magnets: A Combined Terahertz, Far-IR and Vibronic Barrier Model Study" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 61 . 26 (2022) . |
| APA | Ma, Yan , Zhai, Yuan-Qi , Luo, Qian-Cheng , Ding, You-Song , Zheng, Yan-Zhen . Ligand Fluorination to Mitigate the Raman Relaxation of Dy-III Single-Molecule Magnets: A Combined Terahertz, Far-IR and Vibronic Barrier Model Study . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2022 , 61 (26) . |
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Abstract ：
Lead-free hybrid perovskite materials have attracted tremendous consideration due to their applications in photovoltaics, optoelectronics, thermal sensors, etc. Herein, we isolated a new stable semiconductive 2D bismuth(iii)-silver(i) iodide hybrid double perovskite formulated as (H2MPP)(2)[BiAgI8], where H2MPP = 1-methylpiperidinium-4-amine, with reversible solid-state thermochromism, a narrow bandgap and considerable temperature-dependent conductivity. Upon heating from 150 K to 450 K, (H2MPP)(2)[BiAgI8] crystals exhibit a reversible colour change between orange and dark red. The associated structural changes were monitored using in situ single-crystal X-ray diffraction (SCXRD), powder X-ray diffraction (PXRD), UV-visible absorption and Raman spectroscopy. Besides, the electrical conductivity of (H2MPP)(2)[BiAgI8] changes over four orders of magnitude upon thermochromism (up to 1.51 x 10(-6) S cm(-1) at 450 K) and showed an efficiently enhanced photocurrent switching on/off ratio. Moreover, the (H2MPP)(2)[BiAgI8] crystals can be processed into thin films via spin coating and exhibit high stability under heat and moisture, which is indicative of their potential optoelectronic applications based on thermochromism.
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| GB/T 7714 | Lassoued, Mohamed Saber , Wang, Tengbo , Faizan, Ahmad et al. Reversible thermochromism, temperature-dependent conductivity and high stability for a laminated bismuth(iii)-silver(i) hybrid double perovskite [J]. | JOURNAL OF MATERIALS CHEMISTRY C , 2022 , 10 (35) : 12574-12581 . |
| MLA | Lassoued, Mohamed Saber et al. "Reversible thermochromism, temperature-dependent conductivity and high stability for a laminated bismuth(iii)-silver(i) hybrid double perovskite" . | JOURNAL OF MATERIALS CHEMISTRY C 10 . 35 (2022) : 12574-12581 . |
| APA | Lassoued, Mohamed Saber , Wang, Tengbo , Faizan, Ahmad , Li, Qian-Wen , Chen, Wei-Peng , Zheng, Yan-Zhen . Reversible thermochromism, temperature-dependent conductivity and high stability for a laminated bismuth(iii)-silver(i) hybrid double perovskite . | JOURNAL OF MATERIALS CHEMISTRY C , 2022 , 10 (35) , 12574-12581 . |
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Abstract ：
A C,S bonded quasi-two-coordinate Cr(ii) complex, Cr(SAr*)(2) (HSAr* = HSC6H3-2,6(C6H2-2,4,6-Pr-3(i))(2)), has been synthesized according to literature precedent. Magnetic measurements, high-frequency/field electron paramagnetic resonance (HF-EPR) experiments and ab initio calculation studies show that the field-induced slow magnetic relaxation behaviour is caused by relatively weak axial magnetic anisotropy.
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| GB/T 7714 | Luo, Qian-Cheng , Ge, Ning , Zhai, Yuan-Qi et al. A C,S bonded quasi-two-coordinate chromium(ii) complex showing field-induced slow magnetic relaxation behaviour [J]. | DALTON TRANSACTIONS , 2022 , 51 (24) : 9218-9222 . |
| MLA | Luo, Qian-Cheng et al. "A C,S bonded quasi-two-coordinate chromium(ii) complex showing field-induced slow magnetic relaxation behaviour" . | DALTON TRANSACTIONS 51 . 24 (2022) : 9218-9222 . |
| APA | Luo, Qian-Cheng , Ge, Ning , Zhai, Yuan-Qi , Wang, Teng-Bo , Sun, Lin , Sun, Qi et al. A C,S bonded quasi-two-coordinate chromium(ii) complex showing field-induced slow magnetic relaxation behaviour . | DALTON TRANSACTIONS , 2022 , 51 (24) , 9218-9222 . |
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Abstract ：
External stimuli-responsive phase transition of metal-organic frameworks (MOFs) introduces intriguing functions for diverse applications under practical settings. Herein, we reported a phase transition from cubic Ce-UiO-66 to triclinic Ce-BDC-OH under light irradiation. Such a phase transition underwent a ligand-to-metal charge transfer process, which was unambiguously revealed by Fourier transform infrared spectroscopy, nuclear magnetic resonance, electron paramagnetic resonance, etc. We proposed a phase transition mechanism through (1) the photoreduction of the metal core from Ce4+ into Ce3+; (2) the photogeneration of (OH)-O-center dot and hydroxylation of BDC into BDC-OH; and (3) the carboxylate migration and lattice rearrangement for transitions. The phenomenon of the Ce4+-to-Ce3+ reduction also enables a diamagnetism-to-paramagnetism transition, suggesting its potential as a photostimulus-responsive magnetic switch.
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| GB/T 7714 | Guo, Zhixiong , Luo, Qian-Cheng , Qin, Lei et al. Photoinduced Phase Transition of Ce-UiO-66 to Ce-BDC-OH [J]. | INORGANIC CHEMISTRY , 2022 . |
| MLA | Guo, Zhixiong et al. "Photoinduced Phase Transition of Ce-UiO-66 to Ce-BDC-OH" . | INORGANIC CHEMISTRY (2022) . |
| APA | Guo, Zhixiong , Luo, Qian-Cheng , Qin, Lei , Tian, Zhimin , Zheng, Yan-Zhen , Ma, Yuanyuan et al. Photoinduced Phase Transition of Ce-UiO-66 to Ce-BDC-OH . | INORGANIC CHEMISTRY , 2022 . |
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| GB/T 7714 | Chen, Weipeng , Han, Tian , Zheng, Yanzhen . Dodecanuclear {Co10Ln2} metallorings [J]. | Inorganica Chimica Acta , 2021 , 516 . |
| MLA | Chen, Weipeng et al. "Dodecanuclear {Co10Ln2} metallorings" . | Inorganica Chimica Acta 516 (2021) . |
| APA | Chen, Weipeng , Han, Tian , Zheng, Yanzhen . Dodecanuclear {Co10Ln2} metallorings . | Inorganica Chimica Acta , 2021 , 516 . |
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