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Inorganic Chemistry Frontiers
Royal Society of Chemistry
Inorganic Chemistry Frontiers

Royal Society of Chemistry

Inorganic Chemistry Frontiers/Journal Inorganic Chemistry FrontiersEI
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    Platinum-containing heterometallic complexes in cancer therapy: advances and perspectives

    Ma, LiliLi, LuweiZhu, Guangyu
    31页
    查看更多>>摘要：Platinum-based anticancer drugs are among the most widely used antineoplastics in clinical settings. Their therapeutic applications and outcomes are, however, greatly hampered by drug resistance, systemic toxicity, and the lack of antimetastatic and diagnostic properties. The incorporation of second metal centers with distinct biological targets and favorable physical and chemical properties into platinum complexes is a promising strategy to improve the anticancer efficacy of platinum drugs and overcome their shortcomings. This review focuses on Pt-containing heterometallic complexes Pt-M (M = Ru, Au, Ti, Fe, Rh, Pd, Cu, Ir, Gd, Eu, Re, and Tc) for cancer therapy. The design, anticancer activities, mechanism of action, and interplay between Pt and the second metal center are discussed. Many dual-pharmacophore heterometallic complexes have shown a great potential for overcoming cisplatin resistance. Besides, the incorporation of Ru(iii) or areneRu(ii) moieties into Pt complexes has been proved to inhibit cancer metastasis effectively. Moreover, theragnostic heterometallic complexes have been obtained by combining cytotoxic Pt and luminescent Eu(iii), MRI responsive Gd(iii), or radioactive Tc-99m(i) into a single molecule. We also discuss the photophysical and bioimaging properties of theragnostic heterometallic complexes. This review provides a comprehensive landscape of representative examples of Pt-containing heterometallic complexes investigated in the last decade for cancer therapy and may guide researchers in exploring the challenges and opportunities in this emerging field.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    Highly uniform Y3Al2Ga3O12-based nanophosphors for persistent luminescence bioimaging in the visible and NIR regions

    Arroyo, EncarnacionTorres Herrero, Beatrizde la Fuente, Jesus M.Ocana, Manuel...
    9页
    查看更多>>摘要：In the last few years, persistent phosphors with a garnet crystal structure have attracted a great deal of interest for a plethora of applications ranging from bioimaging to anti-counterfeiting technologies. However, the development of synthesis methods to fabricate uniform garnet-based micro and nanoparticles, that are needed for such applications, is not mature at all. This study reports the synthesis of highly uniform yttrium aluminum gallium garnet nanospheres. The method is based on homogeneous precipitation in a polyol medium followed by silica coating and calcination. The nanoparticles resulting after silica removal were also uniform and were easily functionalized with polyacrylic acid. The colloidal stability of the latter in physiological media and their biocompatibility were analyzed. The luminescence of the particles, doped with Ce3+, Cr3+, and Nd3+, was studied by recording emission and excitation spectra and persistent luminescence decay curves. Due to their uniform morphology, high colloidal stability, absence of toxicity, and persistent emission in the visible and near-infrared regions, the reported nanospheres show great potential as persistent luminescent bioimaging probes. In addition, the synthesis method paves the way for future use of this persistent material in other applications that require the phosphor to be in the form of highly uniform nanoparticles.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    KNa0.78Eu0.27In3.80B12S12: a novel hexanary thioborate featuring a B12S12 cluster and diverse InSx (x=4, 5, 6) units

    Han, Shan-ShanYu, Su-XinLiu, WenlongGuo, Sheng-Ping...
    8页
    查看更多>>摘要：Thioborates combine the advantages of sulfides and borates, and are a new type of multifunctional inorganic material with versatile structural features. Here, a thioborate KNa0.78Eu0.27In3.80B12S12 crystallizing with a new type of compound was synthesized by a high-temperature flux method. Its structure features a rarely discovered B12S12 cluster and diverse InSx (x = 4, 5, 6) units built in a three-dimensional {[In3.80B12S12](2.6-)}(infinity) polyanionic framework. The structural complexity and novelty are well elaborated. Its optical band gap was determined to be 2.28 eV, and a theoretical calculation of its electronic structure was also performed. This work not only enriches the structural chemistry of chalcogenoborates but also provides a new potential RE-B-Q family (RE = rare-earth metal; Q = S, Se). The latter may produce some interesting functionals.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    Mesoporogen-free synthesis of single-crystalline hierarchical beta zeolites for efficient catalytic reactions

    Wang, YuyaoLi, JunyanTong, WeiyiShen, Zhenhao...
    9页
    查看更多>>摘要：Single-crystalline hierarchical zeolites possess fast mass transfer, good active site accessibility, and enhanced hydrothermal stability for improved catalytic performance, which are highly desired in petro-, coal-, and fine-chemical industries. Here, we for the first time report the mesoporogen-free synthesis of single-crystalline hierarchical Beta nanozeolites, which is achieved by l-lysine-assisted regulation of zeolite growth kinetics in a two-step crystallization process. In this strategy, at low crystallization temperatures, l-lysine molecules could efficiently chelate with both silica and aluminum species, which leads to the aggregation of amorphous aluminosilicate gel particles in a non-compact manner towards forming interstitial pores. At subsequently elevated temperatures, intraparticle ripening becomes the predominant crystal growth behavior, where adjacent nanoparticles coalesce into larger ones coupled with the transformation of the initial interstitial pores into the final intracrystalline mesopores. The as-prepared hierarchical Beta nanozeolite (sample meso-Beta-23) shows a large surface area (617 m(2) g(-1)) and a large mesopore volume (0.79 cm(3) g(-1)), as well as a single-crystalline feature, thus exhibiting improved properties in both gas- and liquid-phase catalytic reactions, including cracking of 1,3,5-trimethylbenzene to produce benzene, toluene, and xylene (BTX) (26.1% BTX selectivity); ethylation of benzene to produce ethylbenzene (73% ethylbenzene selectivity); and conversion of highly concentrated lactic acid (105 wt%) to produce lactide (73% lactide yield) compared to their conventional counterparts. Such high-quality single-crystalline hierarchical Beta nanozeolites may be promising for industrial applications in the conversion of various bulky feedstocks into value-added products.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    In situ construction of a C3N5 nanosheet/Bi2WO6 nanodot S-scheme heterojunction with enhanced structural defects for the efficient photocatalytic removal of tetracycline and Cr(vi)

    Li, ShijieCai, MingjieLiu, YanpingZhang, Junlei...
    19页
    查看更多>>摘要：Building step-scheme (S-scheme) heterojunctions is newly emerging as an efficient means to obtain excellent photocatalysts for water pollution control. Herein, a 2D/0D S-scheme heterojunction of C3N5/Bi2WO6 was synthesized by in situ growing 0D Bi2WO6 nanodots on 2D C3N5 nanosheets. Photocatalytic removal of tetracycline (TC) and Cr(vi) from water was employed to evaluate the activity of C3N5/Bi2WO6 under visible light compared to that of C3N5, Bi2WO6, and their mechanical mixture. Obviously, C3N5/Bi2WO6 is much more active in the visible-light-driven removal of TC and Cr(vi), indicating strong interaction between the C3N5 nanosheets and Bi2WO6 nanodots as a result of in situ growth. Such an interaction can be illustrated as the S-scheme transfer behavior of photogenerated electrons and holes, which boosts the interfacial charge separation, retains the optimum redox ability of photo-induced charge carriers and fosters the generation of more active species. Moreover, C3N5/Bi2WO6 shows more structural defects than single C3N5 and single Bi2WO6, which may endow C3N5/Bi2WO6 with better ability in the activation and photo-oxidation of TC as well as the activation and photo-reduction of Cr(vi). In a nutshell, this work affords a deep understanding of the photocatalytic mechanism based on C3N5/Bi2WO6 as well as presents a new concept for developing highly efficient S-scheme heterojunction photocatalysts for water decontamination.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    (R)- and (S)-[C8H10NO3](2)[NbOF5]: noncentrosymmetric niobium oxyfluorides with large optical anisotropy

    Moon, JihyeonOk, Kang Min
    10页
    查看更多>>摘要：Huge crystals of noncentrosymmetric (NCS) organic-inorganic hybrid niobium oxyfluorides, (R)-[C8H10NO3](2)[NbOF5] [(R)-Nb] and (S)-[C8H10NO3](2)[NbOF5] [(S)-Nb], have been easily grown via a slow evaporation method in high yields through the systematic driving of chiral structure-directing agents, 4-hydroxy-d-(-)-2-phenylglycine [(R)-HPG] and 4-hydroxy-l-(+)-2-phenylglycine [(S)-HPG], respectively. Both (R)-Nb and (S)-Nb crystallizing in the NCS nonpolar space group, P2(1)2(1)2, exhibit pseudo-three-dimensional structures assembled via multiple hydrogen bonding interactions between distorted [Nb(O/F)(2)F-4](2-) octahedra and the respective protonated HPG cations. Interestingly, crystals of (R)-Nb and (S)-Nb exhibit large birefringence (Delta n(exp)) of 0.19-0.199@589.3 nm attributable to the strong pi-pi interactions arising from the stacked benzene rings in HPG cations. The reported materials exhibit strong stability in most solvents in a wide range of polarities. Detailed characterization studies, including thermal properties, various spectroscopic analyses, second-harmonic generation measurements, and electronic structure calculations on the reported materials, are also described.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    A long life solid-state lithium-oxygen battery enabled by a durable oxygen deficient flower-like CeO2 microsphere based solid electrolyte

    Wang, TianyuanLu, LiangSun, Chunwen
    9页
    查看更多>>摘要：Rechargeable lithium-oxygen batteries (Li-O-2) are one of the most promising candidates for energy storage and electric vehicles due to their high energy density. Nevertheless, their realistic applications are frequently restricted by the safety problems and serious side reactions caused by the use of nonaqueous liquid electrolytes, which makes the service life and safety of these batteries unable to meet the requirements. Here, a durable composite electrolyte membrane was prepared by rationally utilizing oxygen vacancies in flower-like CeO2 microspheres to promote the decomposition of lithium salts and scavenge excess oxygen radicals. The prepared composite electrolyte consists of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP), LiTFSI salt, Li7La3Zr2O12, and flower-like CeO2 microspheres. The composite electrolyte exhibits a wide electrochemical window (5.1 V vs. Li/Li+), high ionic conductivity (4.86 x 10(-4) S cm(-1)) and ionic transference number (0.65) at room temperature. The assembled solid-state lithium-oxygen battery with this composite electrolyte can be cycled stably for more than 400 times (about 2000 hours). Moreover, solid-state Li|LiFePO4 batteries assembled using this composite electrolyte exhibited good cycling stability and high coulombic efficiency as well. This work designs an extraordinary composite electrolyte with both safety and longevity for lithium-oxygen and lithium-ion rechargeable batteries.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    Popcorn-like Co3O4 nanoparticles confined in a three-dimensional hierarchical N-doped carbon nanotube network as a highly-efficient trifunctional electrocatalyst for zinc-air batteries and water splitting devices

    Yao, XiuyunWang, XueyingSun, LixinLi, Ling...
    13页
    查看更多>>摘要：A novel unique popcorn-like three-dimensional (3D) hierarchical structural electrocatalyst is synthesized by the pyrolysis of ZIF-8/ZIF-67 and polyacrylonitrile fiber composites, where popcorn-like Co3O4 nanoparticles coated with nitrogen-doped amorphous carbon anchor onto the tips of N-doped carbon nanotubes (NCNTs), and the NCNTs grow on carbon nanofiber (NAC@Co3O4/NCNTs/CNF). Owing to the positive synergistic effects of 3D hierarchical NCNT networks and popcorn-like Co3O4 species, NAC@Co3O4/NCNTs/CNF shows a record outstanding hydrogen evolution reaction performance (HER; the overpotential at 10 mA cm(-2) is just 76 mV) and wonderful stability for the oxygen reduction reaction (ORR; 73% retention of initial ORR activity after 70 h). Density functional theory (DFT) calculations demonstrate that the chemical interaction between the popcorn-like Co3O4 species and NCNTs benefit the chemisorption of hydrogen and oxygen-containing intermediates, thus accelerating the performance of ORR, OER, and HER. Furthermore, we assembled NAC@Co3O4/NCNTs/CNF as a rechargeable Zn-air battery and an overall water splitting device, displaying a maximum power density of 267.58 mW cm(-2) and almost 100% faradaic efficiency, which provides a promising prospect for surpassing traditional trifunctional electrocatalysts. It is expected that this finding will offer a new concept for synthesizing highly efficient trifunctional materials and applications.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    Green synthesis of N-doped porous carbon/carbon dot composites as metal-free catalytic electrode materials for iodide-mediated quasi-solid flexible supercapacitors

    Wang, RuiWang, HongjuZhou, YiGao, Zhiyong...
    14页
    查看更多>>摘要：P-Nitroaniline has been adopted as a versatile precursor for the selective preparation of N-doped porous carbon (PC) and carbon dots (CDs) with rich N functionalities. Furthermore, the CDs are anchored on PC to yield PC-CDs composites with the assistance of ultrasonication. Due to the catalytic effect of the pyridinic- and pyrrolic-N sites within the CDs as well as the high specific surface area and conductivity of PC, the optimized PC-CDs-1.5% composite (containing 1.5% CDs) could substantially promote the redox reaction of the acidic KI electrolyte. Therefore, the PC-CDs-1.5%-based supercapacitor demonstrated high specific capacitance (C-s, 1783 F g(-1) at 1 A g(-1)), good rate capability (800 F g(-1) at 6 A g(-1)) and excellent cycling stability (84.7% C-s retention upon 10 000 charge-discharge cycles). Moreover, when employed as the electrode in a flexible supercapacitor, the PC-CDs-1.5% composite also exhibits good capacitive performance in the PVA-H2SO4-KI gel electrolyte, and a high energy density (E-cell) of 13.85 W h kg(-1) at a power density (P-cell) of 97.00 W kg(-1) is also delivered. In addition, the flexible device shows good electrochemical cycling stability and the C-s of the flexible device could be well maintained under bending and twisting deformations.
      原文链接:
    • NSTL
    • Royal Soc Chemistry

    A targeted and efficient CDT system with photocatalytic supplement of H2O2 and hydroxyl radical production at a neutral pH

    Da, XuwenWang, ZhanhuaJian, YaoZhang, Chao...
    13页
    查看更多>>摘要：The bottleneck problems of chemodynamic therapy (CDT) are the dependence on an acidic pH (2.0-4.0), insufficient H2O2 level in tumor tissues, and potential systematic toxicity of inorganic nanomaterials-based CDT agents. In this study, the new tricks of two old compounds, i.e. [Ru(phen)(2)(PIP-OCH3)](PF6)(2) (Ru3, phen = 1,10-phenanthroline, PIP-OCH3 = 2-(4-methoxy phenyl)-1H-imidazo[4,5-f][1,10]phenanthroline) and Fe(tpy)Cl-3 (tpy = 2,2 ':6 ',2 '-terpyridine), were harnessed to construct an ideal CDT system. Ru3 was able to efficiently photo-catalyze NADH oxidation accompanied by the production of H(2)O(2)in situ with a high yield of 73.2%, which can be converted into cytotoxic hydroxyl radicals by the biocompatible Fe(tpy)Cl-3 at a neutral pH. By loading both Ru3 and Fe(tpy)Cl-3 in tumor-targeting bovine serum albumin (BSA), the obtained BSA@Fe/Ru nanoparticles exhibited a highly efficient, selective, and photo-controlled CDT activity both in vitro and in vivo. This work may provide new sights for overcoming the issues confronted in CDT.
      原文链接:
    • NSTL
    • Royal Soc Chemistry