Inorganics
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2023
·Vol. 11
·期 11
·422
·
IF 2.9
Yunpeng Xia,Yi Shen,Yang-Rong Yao,Qingyu Meng,Ning Chen
A novel Non-Isolated-Pentagon-Rule (non-IPR) isomer of thorium-based endohedral mono-metallofullerenes (mono-EMFs), Th@C1(17418)-C76, was successfully synthesized and characterized using MALDI-TOF mass spectroscopy, single-crystal X-ray diffraction, UV-vis-NIR spectroscopy, and Raman spectroscopy. The molecular structure of this non-IPR isomer was determined unambiguously as Th@C1(17418)-C76using a single-crystal X-ray diffraction analysis. The crystallographic results further revealed that the optimal Th site resided at the intersection of two adjacent pentagons, similar to that of U@C1(17418)-C76. Additionally, the UV-vis-NIR spectra of Th@C1(17418)-C76exhibited distinct differences compared to the previously reported U@C1(17418)-C76, highlighting the distinctive electronic structure of actinium-based endohedral metallofullerenes (EMFs). The Raman spectrum of Th@C1(17418)-C76exhibited similarities to that previously reported for thorium-based EMFs, indicating the analogous strong metal–cage interactions of thorium-based EMFs.Keywords:endohedral metallofullerenes;mono-metallofullerenes;thorium;X-ray crystallography
研究领域:
化学
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材料科学
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纳米技术
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高影响因子
Inorganics
·
2023
·Vol. 11
·期 8
·323
·
IF 2.9
Huichao Zhang,Jinpeng Xin,Huaimin Jin,Wenhao Xiang,Muqing Chen,Yang-Rong Yao,Shangfeng Yang
Metal cyanide clusterfullerenes (CYCFs) are formed via the encapsulation of a single metal atom and a cyanide unit inside fullerene cages, endowing them with excellent properties in various applications. In this work, we report the synthesis, isolation, and characterizations of the first cases of thulium (Tm)-based CYCFs with the popular C82carbon cages. The structural elucidation of the two TmCN@C82isomers was achieved via diverse analytical techniques, including mass spectrometry, Vis-NIR spectroscopy, single-crystal X-ray crystallography, and cyclic voltammetry. The crystallographic analyses unambiguously confirmed the molecular structures of the two TmCN@C82isomers as TmCN@Cs(6)-C82and TmCN@C2v(9)-C82. Both TmCN clusters adopt a well-established triangular configuration, with the Tm ion located on the symmetrical plane of the carbon cages. The electronic structures of both TmCN@C82isomers adopt a Tm3+(CN)−@(C82)2−configuration, exhibiting characteristic spectral and electrochemical properties reminiscent of divalent endohedral metallofullerenes (EMFs). Intriguingly, unlike the divalent Tm2+ion observed in the mono-metallofullerenes Tm@C2n, a higher oxidation state of Tm3+is identified in the monometallic TmCN cluster due to bonding with the cyanide anion. This result provides valuable insight into the essential role of the non-metallic endo-units in governing the oxidation state of the metal ion and the electronic behaviors of EMFs.Keywords:endohedral metallofullerenes;cyanide clusterfullerenes;thulium;X-ray crystallography
研究领域:
材料科学
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化学
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高影响因子
Inorganics
·
2023
·Vol. 11
·期 9
·349
·
IF 2.9
Xinyi Zhou,Yang-Rong Yao,Yajing Hu,Le Yang,Shaoting Yang,Yilu Zhang,Qianyan Zhang,Ping Peng,Peng Jin,Fang-Fang Li
The reactivity of the open-shell Gd@C2v-C82with different charge states towards benzyl bromide was investigated. [Gd@C2v-C82]3−exhibited enhanced activity relative to Gd@C2v-C82and [Gd@C2v-C82]−. The structural characterizations, including MALDI-TOF MS, UV-vis-NIR, and single crystal X-ray diffraction, indicate the formation of isomeric benzyl monoadducts of Gd@C2v-C82. All three monoadducts contain 1:1 mirror-symmetric enantiomers. Additionally, the addition of the benzyl group and its specific position result in distinct electrochemical behavior of the products compared to the parent Gd@C2v-C82. Theoretical studies demonstrate that only [Gd@C2v-C82]3−has a HOMO energy level that matches well with the LUMO energy level of the PhCH2radical, providing a rationalization for the observed significantly different reactivity.Keywords:endohedral metallofullerene;open shell;electrosynthesis;fullerene anion;Gd@C2v-C82
研究领域:
化学
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材料科学
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2020
·Vol. 34
·期 12
·e5978
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IF 3.14
Ying Hou,Yinxu Pan,Chunhong Dong,Bei Nie
We observed the unusual crystal transformation from solid AgNO 3 to Ag(I)-encapsulated fullerene (C 60 ) microcrystal by a coordination-driven crystallization, when casting C 60 solution on AgNO 3 crystal. The strong binding of Ag + -C 60 ruptures electrostatic interactions within AgNO 3 lattice, forming a binary hybrid material, which was characterized by XRD, Raman spectroscopy and mass spectrometry. Our results support the fact that AgNO 3 crystal can directly interact with fullerene C 60 molecules, other than through solvated metal cations. Two major factors, namely sturdy Ag + -olefin interaction and an enclosed cage effect play the dominating roles in crystal transformation. Adding to the regular solution-based crystallization, this facial protocol is expected to render an additional dimension in fabrication of exohedral metallofullerene architecture, regardless of solubility of metal cation in anti-solvent.
研究领域:
材料科学
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化学
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Hanhui Yan,Yinna Liang,Tao Liu,Ciyuan Huang,Shangfei Yao,Haoran Huang,Yuwen Peng,Jianhua Xiong,Ke Sun,Hongxiang Zhu,Bingsuo Zou,Shuangfei Wang
The photocatalytic degradation of polychlorinated biphenyls (PCBs) is advancing, yet the efficiency of degradation within the visible spectral range continues to encounter significant challenges. In this study, two biochar-based organic semiconductor photocatalysts, Active Carbon@PTQ10 (5,8-Dibromo-6,7-difluoro-2-(2-hexyldecoxy)quinoxaline; trimethyl-(5-trimethylstannylthiophen-2-yl)stannane): ITIC-Th (Propanedinitrile,2,2′-[[6,6,12,12-tetrakis(5-hexyl-2-thienyl)-6,12-dihydrodithieno[2,3-d: 2′,3′-d’] −s-indaceno[1,2-b:5,6-b’] dithiophene-2,8-diyl] bis[methylidyne(3-oxo-1H-indene-2,1(3H)-diylidene)]] bis-) ( AC@PI ) and Active Carbon@PTQ10: PC 71 BM (6,6)-phenyl C 71 butyric acid methyl ester), were synthesized using a wide bandgap material, PTQ10, as the electron donor, along with a non-fullerene material, ITIC-Th, and a fullerene material, PC 71 BM, as the acceptors, respectively. Under optimized conditions, AC@PI degraded 93.4 % of 2,2 ’,4,4 ’-tetrachlorobiphenyl (PCB 47) within 60 min. By incorporating a non-fullerene acceptor (ITIC-Th), AC@PI exhibits a larger surface photopressure, a lower hole-electron transfer ratio, a broader absorption spectrum (400 – 1000 nm), and enhanced structural stability. AC@PI can generate photogenerated electrons and holes, as well as superoxide anions ( O 2 − ) and hydroxyl radicals ( OH), through type II heterojunctions, which contributes to its exceptional properties. This study synthesized novel organic semiconductor catalysts that offer a green, efficient, and non-toxic method for the degradation of aromatic pollutants, such as polychlorinated biphenyls.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
LANGMUIR
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2020
·
IF 3.557
Renxuan Liu,Ying Hou,Shangjun Jiang,Bei Nie
We report a facile approach to fabricate an Ag-embedded fullerene (C60) catalyst by the chemical reduction of the AgNO3 complex encapsulated fullerene microcrystal, which showed an enhanced catalytic reduction of 4-nitrophenol because of the strong absorption and propagation of H2 along the fullerene surface. With the aid of visible-light radiation, photodegradation of orange G dye is achieved through the formation of an electron donor–acceptor dyad between plasmon Ag nanostructures and fullerene molecules, which effectively offsets the “electron–hole” recombination. Neither Ag nanoparticle nor fullerene crystal used in isolation could perform this chemical conversion, implying that the metal–fullerene hybrid structure is imperative for performing the catalytic reaction. The obtained Ag-embedded fullerene crystal is characterized by scanning electron microscopy (SEM), associated energy-dispersive X-ray spectroscopy (EDX) imaging, and X-ray photoelectron spectroscopy (XPS) and demonstrates that the present hybrid materials would add a supplemental member to a family of photocatalysts toward the organic synthesis and wastewater remediation.
研究领域:
材料科学
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环境科学
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催化化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Li Xia,Wenxi Zhou,Yifan Xu,Zhengqiang Xia,Xinzhi Wang,Qi Yang,Gang Xie,Sanping Chen,Shengli Gao
The introduction of rich-electron ligands is a promising strategy to improve the ligand-to-metal charge transfer (LMCT) ability of metal–organic frameworks (MOFs) for efficient photocatalytic CO 2 reduction reactions (CO 2 RR), while the resulting impaired Lewis acid sites go against stable bonding with CO 2 and hinder the electron transfering to CO 2 . It is thus the key to search a trade-off between increasing LMCT and frustrating Lewis acid. Herein, the ferrocene (Fc) modified UiO-66 series MOFs, NH 2 -UiO-66-Fc, have been prepared to optimize LMCT for boosting CO 2 RR through a simple solvent-assisted ligand incorporation (SALI) method. Theoretical calculation and systematic experiments, including photoelectrochemical measures, in situ electron paramagnetic resonance, fluorescence probe analysis and X-ray photoelectron spectroscopy indicate that with increasing Fc content, the LMCT energy of MOFs significantly decreases from 2.66 to 2.10 eV based on the established electron transfer double-channel mechanism, while the Lewis acidity of Zr sites reduces with the CO 2 adsorption energy ( E ad ) ranging from −1.061 to −0.632 eV. Through introducing an optimal Fc content, NH 2 -UiO-66-Fc (2.0) integrating satisfactory LMCT ability and Lewis acidity shows superior photocatalytic CO 2 RR performance (CO yield: 90.65 μmol·g −1 ·h −1 ), about 13 times higher than that of the unmodified MOF and superior to most reported pristine MOF photocatalysts. DFT calculation demonstrates that the excellent performance of NH 2 -UiO-66-Fc (2.0) is attributed to the lowest energy barrier of 1.50 eV for the rate-limiting step of *COOH formation. In this work, such a simple post-modification strategy for facilitating the whole electron transfer path of photocatalytic CO 2 RR will provide a new way to construct high-performance MOFs-based CO 2 RR photocatalysts.
研究领域:
材料科学
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环境科学
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化学
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高影响因子
DALTON TRANSACTIONS
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2013
·Vol. 43
·期 3
·982-989
·
IF 3.806
Bo Chai,Xiang Liao,Fakun Song,Huan Zhou
Fullerene modified C3N4 (C60/C3N4) composites with efficient photocatalytic activity under visible light irradiation were fabricated by a simple adsorption approach. The as-prepared C60/C3N4 composites were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), UV-vis diffuse reflectance absorption spectra (DRS), Fourier transform infrared spectroscopy (FTIR) and photoluminescence spectra (PL). The photocatalytic degradation of rhodamine B (RhB) by the C60/C3N4 composites was investigated and optimized, suggesting that the optimal amount of C60 in the composites was 1 wt%. The significantly enhanced photocatalytic activity could be attributed to the efficient separation of photogenerated electrons and holes in the C60/C3N4 composites. A possible mechanism of C60/C3N4 composites as photocatalysts was proposed.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
DYES AND PIGMENTS
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2024
·
IF 4.1
Jinyu Wu,Shaolong Han,Sichen Li,Rui Zhu,Shuaibo Shi,Shishen Zhang,Kun Zhang
Till now, there is still a lack of the convenient and efficient approach to implement identification and quantitation of fullerenes in various domains. This work provides the first example for detecting fullerenes by an adequate fluorescent probe, in parallel with the new methodology for detecting fullerenes by the fluorescent chemosensing approach. Using a multi-emission lanthanide-disalicylaldehyde coordination hybrid H 2 Q j2 /Tb 0.91 Eu 0.09 , the rapid, selective and discriminative detection of analogous C 60 and C 70 can be easily achieved after the spectral and statistical analyses of fluorescent sensing signals on four emission bands (416, 543, 447 and 615 nm), excited by two irradiation lights (370 and 394 nm). Titration experiments further verify the very high linearity for both C 60 and C 70 and allow their detection at concentrations as low as 1.72 μM (C 60 ) and 0.09 μM (C 70 ). Moreover, this fluorescent probe also shows its reliable abilities to identify proportional C 60 /C 70 mixtures and monitor C 60 and C 70 contents in actual soil sample. It is believed that our proposed lanthanide-base fluorescent matrix not only verify the feasibility and potential of fluorescent chemosensing methodology for the fullerene detection but also provide a valuable tool for potential applications.
研究领域:
化学
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材料科学
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分析化学
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DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2016
·
IF 2.74
Muhammad Asim Akhtar,Sara Riaz,Akhtar Hayat,Muhammad Nasir,Nawshad Muhammad,Abdur Rahim,Mian Hasnain Nawaz
trans -Porphyrin containing phenyl group at both ends was synthesized via corresponding dipyrromethanes (DPM) in the presence of TFA and DDQ. The polyethyleneglycole (PEG) chains were attached at the trans positions of ABA type porphyrinic moiety. The prepared PEGylated porphyrin (with PEG arms at the periphery) P-(PEO) 2 was self-assembled into spheres of uniform diameter while their DMF solution was dialyzed into water. Furthermore, the addition of fullerene (C 60 ) to P-(PEO) 2 caused complexation between porphyrin and fullerene which lead to interesting and trenchant morphology having worm like lateral aggregates. The assembly process and the as-prepared edifices were characterized using UV–vis absorption spectroscopy and the morphology of these assemblies was investigated using transmission electron microscope (TEM). Furthermore, the DNA binding with porphyrin aggregates has been demonstrated via electrochemical (cyclic voltammetric) response of screen printed electrodes modified . The obvious increase in redox current disclosed the intermolecular interactions of the adducts with the DNA. These studies of unprecedented adducts can further be explored for potential applications in biosensors .
研究领域:
生物化学
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材料科学
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分子生物学
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高影响因子
JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 34
·17833-17841
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IF 5.968
Cheng-Xiong Yang,Xiu-Ping Yan
The adsorption and extraction of fullerenes on the metal–organic framework MIL-101(Cr) were studied in detail in terms of kinetics, thermodynamics, adsorption isotherms, competitive adsorption, and breakthrough curves. The adsorption of C60 and C70 on MIL-101(Cr) follows a pseudo-second-order kinetic model. The adsorption rate constant for C70 is 3 to 5 times that for C60, showing faster and easier adsorption of C70 over C60 on MIL-101(Cr). Intraparticle diffusion model analysis reveals that the adsorption of C60 and C70 on MIL-101(Cr) proceeds by two phases, surface sorption and intraparticle/pore diffusion. The adsorption of fullerenes on MIL-101(Cr) is controlled by entropy changes. The maximum adsorption capacity for C70 at 30 °C (198.4 mg g−1) is 29 times that for C60 (6.76 mg g−1). MIL-101(Cr) shows much more favorable adsorption of C70 and higher fullerenes than C60 with a high selectivity (αC70/C60 = 24). Selective extraction of C70 and higher fullerenes from crude carbon soot can be easily achieved on MIL-101(Cr) via a simple adsorption–desorption process. The used MIL-101(Cr) can be regenerated by washing with o-dichlorobenzene under ultrasonication. The high selectivity, fast adsorption, easy desorption, and excellent reusability makes MIL-101(Cr) attractive as a novel adsorbent for the enrichment and extraction of C70 and higher fullerenes.
研究领域:
材料科学
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化学工程
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高影响因子
Food Analytical Methods
·
2014
·Vol. 7
·期 9
·1729-1736
·
IF 1.802
Chao Mingyong,Chen Meifeng
Employing a graphene-modified glassy carbon electrode, a sensitive and convenient electrochemical method for the determination of phoxim by linear sweep voltammetry was developed. The electrochemical behavior of phoxim at the modified electrode was studied by cyclic voltammetry. In citric acid–phosphate buffers, the modified electrode exhibited excellent electrocatalytical effect on the reduction of phoxim and this was further used for the determination of phoxim. Under optimized analytical conditions, the reduction peak current showed a linear relationship with the concentration of phoxim in a range of 5.97 to 5,966 μg L −1 , with a correlation coefficient of 0.9993 and a detection limit of 2.39 μg L −1 . The proposed method shows excellent sensitivity, selectivity, and linearity and has been successfully applied for the determination of phoxim in a variety of food samples with satisfactory results.
研究领域:
分析化学
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食品安全
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DOI
高影响因子
危险品化学品经营许可证（带存储）