【最新中稿作品】金属–多酚组装材料、超细钌团簇、纳米疫苗等

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标题

Metal Ion-Directed Functional Metal–Phenolic Materials

作者

Huimin Geng ,Qi-Zhi Zhong, Jianhua Li, Zhixing Lin, Jiwei Cui*, Frank Caruso*, and Jingcheng Hao*

引用

Chem. Rev. 2022, 122, 13, 11432–11473

Publication Date:May 10, 2022

DOI

https://doi.org/10.1021/acs.chemrev.1c01042

研究介绍

近年来，金属–多酚胶体组装材料发展迅速，已广泛应用于化学、材料科学、生物医学等领域。

近日，山东大学胶体与界面化学教育部重点实验室郝京诚教授团队受邀在化学领域Chem.Rev(2022,DOI:10.1021/acs.chemrev.1c01042,IF = 60.622，封面文章)发表了题为“Metal Ion-Directed Functional Metal–Phenolic Materials”的综述性论文。

该文章阐述了碱金属、碱土金属、过渡金属、贵金属离子、类金属与多酚类化合物之间的阳离子–π作用、配位作用、氧化还原作用和动态共价键四种相互作用力（图1）；

讨论了相互作用力的协同机制、影响因素、表征技术，构建新颖功能组装材料特点，以及在生物、催化、环境领域的应用，展望了金属–多酚组装材料领域的发展前景和面临的挑战。

团队利用高频超声技术结合芬顿反应，实现了一步法介导含芳香衍生物的羟基化组装，构筑了金属-多酚超分子功能涂层（Angew. Chem. Int. Ed.2021, 60, 21529）。

图1. 阳离子–π作用、配位作用、氧化还原作用和动态共价键相互作用示意图和元素周期表中可用于金属-多酚组装材料的元素

中稿封面·一周精选

01

Volume 134, Issue 33 04 July 2022

Titel

Anion-Guided Stepwise Assembly of High-Nuclearity Lanthanide Hydroxide Clusters

DOI

https://doi.org/10.1002/ange.202209210

Abstract（上下滑动查看）

Die rationale Synthese von Lanthanoidclustern mit hohem Kerngehalt bleibt eine Herausforderung. In ihrem Forschungsartikel (e202205385) entwickelten Min Feng, Zhiping Zheng et al. eine anionengeleitete, schrittweise Synthese eines hochnuklearen Sodalith-ähnlichen Clusters Er60. Die sukzessive Einführung von I−, CO32− und NO3− führte zur Isolierung von drei Zwischenclustern, nämlich dem radartigen Er12, dem schiffsartigen Er34 und dem schalenartigen Er48. Die Ergebnisse öffneten die “Black Box” des schwer fassbaren Selbstorganisationsprozesses und lieferten wichtige mechanistische Erkenntnisse.

02

Volume 144, Issue 32 July 22, 2022

Titel

Growth Kinetics of Single Polymer Particles in Solution via Active-Feedback 3D Tracking

DOI

https://pubs.acs.org/doi/10.1021/jacs.2c04990

Abstract（上下滑动查看）

The ability to directly observe chemical reactions at the single-molecule and single-particle level has enabled the discovery of behaviors otherwise obscured by ensemble averaging in bulk measurements. However powerful, a common restriction of these studies to date has been the absolute requirement to surface tether or otherwise immobilize the chemical reagent/reaction of interest. This constraint arose from a fundamental limitation of conventional microscopy techniques, which could not track molecules or particles rapidly diffusing in three dimensions, as occurs in solution. However, many chemical processes occur entirely in the solution phase, leaving single-particle/-molecule analysis of this critical area of science beyond the scope of available technology. Here, we report the first kinetics studies of freely diffusing and actively growing single polymer–particles at the single-particle level freely diffusing in solution. Active-feedback single-particle tracking was used to capture three-dimensional (3D) trajectories and real-time volumetric images of freely diffusing polymer particles (D ≈ 10–12 m2/s) and extract the growth rates of individual particles in the solution phase. The observed growth rates show that the average growth rate is a poor representation of the true underlying variability in polymer–particle growth behavior. These data revealed statistically significant populations of faster- and slower-growing particles at different depths in the sample, showing emergent heterogeneity while particles are still freely diffusing in solution. These results go against the prevailing premise that chemical processes in freely diffusing solution will exhibit uniform kinetics. We anticipate that these studies will launch new directions of solution-phase, nonensemble-averaged measurements of chemical processes.

03

Volume 18, Issue 32 11 August 2022

Titel

Elastic Nanovaccine Enhances Dendritic Cell-Mediated Tumor Immunotherapy (Small 32/2022)

DOI

https://doi.org/10.1002/smll.202270173

Abstract（上下滑动查看）

Nanovaccine-based immunotherapy (NBI) has the ability to initiate dendritic cell (DC)-mediated tumor-specific immune responses and maintain long-term antitumor immune memory. To date, the mechanism by which the mechanical properties of nanoparticles alter the functions of DCs in NBI remains largely unclear. Here, a soft mesoporous organosilica-based nanovaccine (SMONV) is prepared and the elasticity-dependent effect of the nanovaccine on the underlying DC-mediated immune responses is studied. It is found that the elasticity results in greater internalization of SMONV by DCs, followed by the induction of substantial cytosolic delivery of antigens via endosomal escape, leading to effective DC maturation and antigen cross-presentation. Impressively, elasticity enables SMONV to enhance lymphatic drainage of antigens in vivo, thus stimulating robust humoral and cellular immunity. The results from therapeutic tumor vaccination further reveal that subcutaneously administered SMONV effectively suppresses tumor growth in tumor-bearing mice by evoking antigen-specific CD8+ T-cell immune responses, mitigating regulatory T-cell-mediated immunosuppression, and increasing central memory and effector memory T-cell populations. Furthermore, combinatorial immunization with SMONV and anti-PD-L1 blocking antibodies results in an amplified therapeutic effect on tumor-bearing mice. These findings reveal the elastic effect of the nanovaccine on DC-mediated immune responses, and the prepared SMONV represents a facile and powerful strategy for antitumor immunotherapy.

04

Volume9, Issue23 11 August 2022

Titel

LSPR-Enhanced Pyro-Phototronic Effect for UV Detection with an Ag–ZnO Schottky Junction Device

DOI

https://doi.org/10.1002/admi.202200327

Abstract（上下滑动查看）

Sensitive and rapid detection of low-power density ultraviolet (UV) light is of great significance for various applications such as space exploration, biological analysis, environmental sensors, communications, and imaging. However, the persistent photoconductivity (PPC) of photodetectors, which are based on ZnO, will cause a long decay time and make it difficult to capture weak light signals. In this work, the pyro-phototronic effect of ZnO is integrated with the localized surface plasmon resonance (LSPR) of Ag nanoparticles (NPs) to enhance the performance of ZnO-based photodetectors. The self-powered photodetector is consisted of the ZnO nanowires (ZnO NWs) and Ag NPs, which can detect 325 nm UV light with a power density of 340 nW cm−2 quickly and sensitively. Compared with the photodetector without Ag NPs, the performance is significantly improved. Under the 325 nm UV light with the same power density, the best responsivity, and detectivity are 8.82 × 10−5 A W−1 and 4.9 × 1010 Jones, respectively. And the fast response time is remarkably reduced to 8.72 ms. These results help to understand the performance of LSPR enhanced photodetectors deeply and expand the methods for preparing high-performance photodetectors.

05

Volume 108, 10 May 2022

Titel

Hierarchical red phosphorus incorporated TiO2 hollow sphere heterojunctions toward superior photocatalytic hydrogen production

DOI

https://doi.org/10.1016/j.jmst.2021.09.026

Abstract（上下滑动查看）

Solar-to-hydrogen conversion through photocatalysis is a sustainable and promising strategy for storing solar energy. Recently, elemental red phosphorus (RP) with broad light absorption has been recognized as a potential candidate for photocatalytic hydrogen evolution, while challenges remain due to the rapid recombination of photogenerated carriers. In this work, RP modified TiO2 hollow spheres were designed and fabricated through the chemical vapor deposition method. The optimal hydrogen production rate reaching 215.5 μmol/(g h) over TiO2@RP heterostructure was obtained under simulated solar light irradiation. Experimental results evidenced that the hollow sphere structure and RP light absorber extended light absorption ability, and the heterostructure induced interfacial charge migration facilitated photoinduced charge separation, which benefited the photocatalytic hydrogen production performance.

06

Issue 16,21 August 2022

Titel

Visible-light-driven regioselective carbocarboxylation of 1,3-dienes with organic halides and CO2†

DOI

https://doi.org/10.1039/D2GC01256A

Abstract

Harnessing light to convert carbon dioxide (CO2) into value-added fine chemicals is an attractive synthesis strategy. Herein, we report an unprecedented visible-light-driven regioselective carbocarboxylation of 1,3-dienes with CO2 using aryl and alkyl halides under mild conditions with low-cost potassium formate (HCOOK) to produce carbon dioxide radical anions as the potent reducing agent for the challenging organic halide reduction. Highly 3,4-regioselective carbocarboxylation was achieved with 1,1-diaryl-substituted 1,3-dienes, while major 1,4-carbocarboxylation products were obtained with less hindered mono-aryl substituted 1,3-dienes. This protocol renders a rapid method for producing complex β,γ-unsaturated carboxylic acids from easily available 1,3-dienes and organic halides with CO2.

01

Volume 65, Issue 15 August 1, 2022

Titel

Design, Synthesis, and Biological Evaluation of Pyrrole-2-carboxamide Derivatives as Mycobacterial Membrane Protein Large 3 Inhibitors for Treating Drug-Resistant Tuberculosis

DOI

https://doi.org/10.1021/acs.jmedchem.2c00718

Abstract（上下滑动查看）

In this work, pyrrole-2-carboxamides were designed with a structure-guided strategy based on the crystal structure of MmpL3 and a pharmacophore model. The structure–activity relationship studies revealed that attaching phenyl and pyridyl groups with electron-withdrawing substituents to the pyrrole ring and attaching bulky substituents to the carboxamide greatly improved anti-TB activity. Most compounds showed potent anti-TB activity (MIC < 0.016 μg/mL) and low cytotoxicity (IC50 > 64 μg/mL). Compound 32 displayed excellent activity against drug-resistant tuberculosis, good microsomal stability, almost no inhibition of the hERG K+ channel, and good in vivo efficacy. Furthermore, the target of the pyrrole-2-carboxamides was identified by measuring their potency against M. smegmatis expressing wild-type and mutated variants of the mmpL3 gene from M. tuberculosis (mmpL3tb) and determining their effect on mycolic acid biosynthesis using a [14C] acetate metabolic labeling assay. The present study provides new MmpL3 inhibitors that are promising anti-TB agents.

01

Volume 11, Issue 20

Titel

Injectable electrospun fiber-hydrogel composite sequentially releasing clonidine and ropivacaine for prolonged and walking regional analgesia

DOI

https://doi.org/10.7150/thno.74845

Abstract（上下滑动查看）

Rationale:Peripheral nerve block is a traditional perioperative analgesic method for its precise pain control and low systemic toxicity. However, a single low dose of local anesthetic merely provides a few hours of analgesia, and high dose results in irreversible toxicity, whereas continuous infusion of anesthetics is expensive and complicated. Therefore, it is necessary to develop a long-acting and sensory-selective local anesthetic for safe perioperative analgesia.

Methods:An injectable composite comprising ropivacaine-loaded poly (ε-caprolactone) electrospun fiber and clonidine-loaded F127 hydrogel (Fiber-Rop/Gel-Clo composite) was developed for long-acting and walking regional analgesia with barely one dose. The peripheral nerve blockade effect of the composite was evaluated in a rat sciatic nerve block model. Also, the biodegradability and biosafety of the composite was evaluated.

Results:The preferentially released Clo from the hydrogel rapidly constricted the peripheral arterial vessels, reducing the blood absorption of Rop and thus enhancing the local Rop accumulation at the injection site. The subsequently sustainable release of Rop from the fiber, significantly prolonged the sciatic nerve block of rats. Remarkably, an amazing sensorimotor segregation effect was achieved, as the sensory blockade (32.0 ± 1.4 h) lasted significantly longer than the motor blockade (20.3 ± 0.9 h). Additionally, the Fiber-Rop/Gel-Clo composite presented good biodegradability and biosafety in vivo.

Conclusions: Our designed Fiber-Rop/Gel-Clo composite with minimal invasion, prolonged synergistic analgesia, and strikingly sensorimotor segregation effect, posted a promising prospect for regional long-term walking analgesia in clinical treatment.

Keywords:ropivacaine, clonidine, electrospun fiber, injectable hydrogel, long-acting regional analgesia, sensorimotor separation

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