CCS Chemistry 2022年第12期上线

以下文章来源于CCSChemistry ，作者CCS Chemistry

CCSChemistry.

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CCS Chemistry 2022年第12期上线！本期包括6篇Communication和14篇Research Article，涵盖了氟化学、精准合成、金催化、单分子磁体、功能π-体系、聚集诱导发光、共价有机框架材料（COFs）、配位自适应网络（CoAN）和蛋白降解等方面的最新研究进展。

本期封面文章来自中国科学技术大学吴宇恩教授团队，该团队报道了一种通过N-甲基-2-吡咯烷酮作为向导分子构建多层、具有弯曲基底平面的硫化钼结构的新方法。弯曲平面应力可激活惰性基面，从而提供更丰富的配位位点以锚定单原子金属铂。在弯曲硫化钼载体表面，应力辅助的单原子金属铂位点具有优秀的H2S检测能力。该研究为单原子催化剂用于高灵敏气体传感器的构建和应用提供了新方法和新思路。

了解更多信息，欢迎访问：https://www.chinesechemsoc.org/toc/ccschem/4/12 。

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2022年第12期

Author Spotlight

本期Author Spotlight邀请了天津大学马军安教授、杭州师范大学卢华教授、中国科学院理化技术研究所丛欢研究员和中国科学技术大学吴宇恩教授，分享自己科研经历中独特的心得和感悟。

Link：https://doi.org/10.31635/ccschem.022.202201124ed2

以下是本期每篇文章的导读和阅读链接：

- Diradical Materials. The unique electronic and magnetic properties of air-stable diradicaloid polycyclic aromatic hydrocarbon materials make them good candidate materials for different applications. Qinqin Shi, Hui Huang, and coworkers report a new kind of furan-fused rubicene and investigate the chalcogen effect on the diradical characteristics of rubicenes. Some key take aways include kinetic stabilization of diradicals under the influence of non-planarity/bulky substitution, topology, and chalcogen incorporation. Their work provides a simple strategy of constructing diradical materials.

Cite this: CCS Chem.2022, 4, 3669–3676

Link：https://doi.org/10.31635/ccschem.022.202201954

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-Stereoselective Glycosylation. Liming Zhang and coworkers develop an effective method for the synthesis of 1,2-cis-furanosides based on a gold(I)-catalyzed glycosylation reaction with ortho-alkynylbenzoates as donors and using the directing-group-on-leaving-group strategy. They achieved good to excellent stereoselectivities in the high-yielding furanosylation reactions which can be completed in two hours. Given the difficulty of 1,2-cis-furanosides synthesis using conventional methods, the ease of the approach could open up new opportunities to explore the use of 1,2-cis-furanosides in medicine and materials.

Cite this: CCS Chem.2022, 4, 3677–3685

Link：https://doi.org/10.31635/ccschem.022.202202175

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-Chiral AIEgens. Wallach’s rule states that racemic crystals tend to have a higher density than their enantiomeric counterparts. Kai Li, Shuang Quan Zang, and coworkers report an interesting photophysical phenomenon, which they attribute to the influence of Wallach’s rule, where a series of racemic aggregation-induced emission (AIE) luminogens and their homochiral analogues exhibit different luminescence properties in the aggregated state. Furthermore, a novel cryptographic information storage system is constructed based on the racemism-enhanced emission.

Cite this: CCS Chem.2022, 4, 3686–3692

Link：https://doi.org/10.31635/ccschem.022.202201998

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-Disubstituted Pyrazole Synthesis. Fa-Guang Zhang, Jun-An Ma, and coworkers disclose two classes of previously elusive trifluoromethyl- and cyano-functionalized pyrazoles that can be readily constructed via a silver-catalyzed direct [3 + 2] cycloaddition reaction of dicyanoalkenes with trifluorodiazoethane in a one-pot approach. Furthermore, the application potential of the reaction is demonstrated in the efficient synthesis of cyano-analogues of CF3-containing drugs (Celecoxib) and agrochemicals.

Cite this: CCS Chem.2022, 4, 3693–3704

Link：https://doi.org/10.31635/ccschem.022.202201923

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-Porous Metal–Organic Frameworks. Hierarchically porous (HP) materials that facilitate mass transfer in heterogeneous catalysis are highly sought. Hai-Long Jiang and coworkers develop a facile “rigid modular assisted defect formation” strategy to fabricate stable HP metal–organic frameworks (MOFs) from microporous MOFs. The obtained HP UiO-66-NH2, decorated with trifluoromethanesulfonate groups to enhance Lewis acidity, exhibits excellent catalytic activity and selectivity.

Cite this: CCS Chem.2022, 4, 3705–3714

Link：https://doi.org/10.31635/ccschem.022.202201974

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-Fluorescent Probes for Bioimaging. Xianfeng Gu, Chunchang Zhao, and coworkers design a dual parameter-activated probe for cancer imaging through successive activation by alkaline phosphatase (ALP) and H2S. The ALP-mediated dephosphorylation leads to a charge reversal of probe aggregates, activating aggregation-enhanced responsiveness to H2S with light-up near-infrared fluorescence. Such an activatable probe can be employed in cancer imaging with high specificity and accuracy.

Cite this: CCS Chem.2022, 4, 3715–3723

Link：https://doi.org/10.31635/ccschem.022.202201971

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-Supramolecular Elastomer. Except for fluorocarbons and silicones, few artificial materials display both water and organic solvent resistance. Bin Zhang, Yun Yan, and coworkers fabricate a supramolecular elastomer through complexation of folic acid and branched poly(ethylene imine) in water under suitable pH conditions. The recyclable supramolecular elastomer displays not only self-healing properties but also good stability in water and some organic solvents.

Cite this: CCS Chem.2022, 4, 3724–3734

Link：https://doi.org/10.31635/ccschem.022.202201775

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-AIE Biomedical Probes. Accurate and dynamic visualization of vascular diseases can contribute to the timely prevention of further deterioration. Xiaoxing Xiong, Xianli Meng, Xuechuan Hong, and coworkers have designed a new type of benzobis(1,2,5-thiadiazole)-based fluorophores with remarkable AIE characteristics, which show high quantum yields in NIR-II window (>1000 nm, 14.45%) and NIR-IIb window (>1500 nm, 0.27%). High resolution in vivo NIR-IIb imaging of revascularization, thrombolysis, and real-time feedback of therapeutic efficacy of ischemic stroke by a Chinese medicine Dengzhan Xixin injection are achieved for the first time.

Cite this: CCS Chem.2022, 4, 3735–3750

Link：https://doi.org/10.31635/ccschem.022.202101547

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-Covalent Organic Frameworks. Zhikun Zheng and coworkers present a liquid-crystal-directed synthesis method for the production of highly crystalline COFs. Syntheses of 17 donor–acceptor two-dimensional COFs with a yield of up to 94% have been demonstrated, showing good generality of the method. Furthermore, one of the donor–acceptor COFs exhibits a production rate of 4300 μmol h−1 gcat−1 in photocatalytic H2O2 production, much higher than g-C3N4.

Cite this: CCS Chem.2022, 4, 3751–3761

Link：https://doi.org/10.31635/ccschem.022.202101578

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Single-Molecule Magnets. Magnetoelectric multiferroic materials have unique advantages in low-power and high-density information storage because they simultaneously display ferroelectricity and ferromagnetism. Akseli Mansikkamäki, Jinkui Tang, and coworkers report the design, synthesis, structures, and magnetic properties of three pairs of enantiomers of Dy(III)-macrocycles. The proportion of polar space groups in chiral space groups is very large, bringing great potential to the synthesis of complexes with polar space groups. A similar strategy may be extended to the design of single-molecule magnets with tailor-made properties.

Cite this: CCS Chem.2022, 4, 3762–3771

Link：https://doi.org/10.31635/ccschem.022.202101604

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-Molecular Nanotubes. The construction of large molecules with precise and complex architectures and topology remains a challenge. Huan Cong and coworkers report the synthesis of a series of discrete and monodispersed nanotubes by connecting three to five rigid macrocycles with reversible imine and Pt(II)–pyridine bonds. Furthermore, they demonstrate that the anisotropic molecular nanotubes can be deposited onto chemically modified surfaces with an upright orientation in a predictable fashion.

Cite this: CCS Chem.2022, 4, 3772–3780

Link：https://doi.org/10.31635/ccschem.022.202101728

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-Coordination Adaptable Network. Cheng-Hui Li and coworkers design and prepare a coordination adaptable network (CoAN) by crosslinking low-molecular-weight flexible molecules with dynamic coordination bonds between thiol/thiolate and Zn2+. The as-prepared CoAN materials exhibit high mechanical strength yet can be reprocessed rapidly and recycled at mild conditions. Additionally, the materials do not show performance reduction in mechanical properties after being repeatedly reprocessed.

Cite this: CCS Chem.2022, 4, 3781–3797

Link：https://doi.org/10.31635/ccschem.022.202101672

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-Germanium π-Conjugated Materials. Zujin Zhao, Hua Lu, and coworkers report a simple and effective method for the construction of Ge-containing π-conjugated molecules, including benzogermoles. The photophysical properties of these molecules can be tuned by introducing different substituents, and intense solid-state luminescence ranging from deep-blue to red regions has been observed. Notably, Ge-bridged ladder-type derivatives are synthesized for the first time, which display efficient deep-blue electroluminescence with good color purity.

Cite this: CCS Chem.2022, 4, 3798–3808

Link：https://doi.org/10.31635/ccschem.022.202101625

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-Cell-Selective Protein Degradation. Proteolysis targeting chimera (PROTAC) technology is a chemical protein knockdown approach that degrades protein by hijacking the cellular ubiquitin-proteasome system to impede tumor growth. Ming Wang and coworkers report a clever strategy to generate PROTAC prodrugs using a responsive chemical modification. The PROTAC molecules are chemically conjugated with several small molecule moieties which can be cleaved in the appropriate environment. The in vitro results clearly show the degradation of targeted proteins using the pro-PROTAC strategy.

Cite this: CCS Chem.2022, 4, 3809–3819

Link：https://doi.org/10.31635/ccschem.022.202101529

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-Difluoromethyl Ether Synthesis. Qiuling Song and coworkers disclose a novel difluorocarbene-mediated C–O bond cleavage of cyclic ethers for the construction of difluoromethyl ethers. This protocol features mild conditions, high efficiency, and a broad substrate scope, which can tolerate sensitive functional groups, such as hydroxyl groups, olefins, and C–C triple bonds. A wide range of possible reaction substrates and good compatibility give this approach unique advantages in late-stage modification of drug molecules and natural products.

Cite this: CCS Chem.2022, 4, 3820–3831

Link：https://doi.org/10.31635/ccschem.022.202101576

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-Heteronuclear Complex for Photochromism. Photochromic compounds have wide-ranging applications in optical information storage, anticounterfeiting, and protection. Liang-Jin Xu, Zhong-Ning Chen, and coworkers present a novel photochromic system with a CuPt2 complex. Upon UV light irradiation, a biradical is generated, giving rise to a drastic change in UV–vis absorption spectrum. When UV light irradiation is ceased, decoloration occurs through thermal cycloreversion, showing that the photochromic CuPt2 complexes have self-recovery characteristics..

Cite this: CCS Chem.2022, 4, 3832–3841

Link：https://doi.org/10.31635/ccschem.022.202101675

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-Single-Atom Site Catalysts. Yuen Wu and coworkers report a valuable method to construct a multilayer MoS2 structure with bent basal planes by using N-methyl-2-pyrrolidone as guiding molecules. The bending-induced strain can activate the inert basal plane and provide abundant sites to anchor Pt monomers. The strain assisted single Pt sites on the curved MoS2 surface exhibit superior H2S-sensing performance over reference catalysts.

Cite this: CCS Chem.2022, 4, 3842–3851

Link：https://doi.org/10.31635/ccschem.022.202101628

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-Visible-to-Ultraviolet Upconversion. Visible-to-UV triplet–triplet annihilation upconversion (TTA-UC) systems are all reported to have energy gains less than 0.92 eV, thus restricting the excitation wavelength to the blue region. By pairing multiple-resonance thermally activated delayed fluorescence sensitizers with appropriate acceptors, Xiaosong Cao, Chuluo Yang, and coworkers develop green-to-UV TTA-UC systems with an anti-Stokes shift up to 1.05 eV, which can be used for photochemical reactions under excitation of low-power-density green light.

Cite this: CCS Chem.2022, 4, 3852–3863

Link：https://doi.org/10.31635/ccschem.022.202101507

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-Precise Synthesis of Polypeptides. Jinming Hu, Shiyong Liu, and coworkers present facile syntheses of well-defined polypeptides with complex chain topologies via polymerization of moisture-insensitive and air tolerant α-amino acid precursors and using primary amine hydrochloride as the initiator. Their work provides a reliable tool for the precise synthesis of polypeptides with different topologies (e.g., block, star, star-block, brush, and multiblock).

Cite this: CCS Chem.2022, 4, 3864–3877

Link：https://doi.org/10.31635/ccschem.022.202101704

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-Prodrug Delivery System. Efficacy of prodrugs in cancer therapy requires selective and efficient drug activation in cancer cells. Youyong Yuan and coworkers report a novel dual-prodrug delivery system with tumor-selective cascade-amplified prodrug activation for synergistic oxidation-chemotherapy, providing a new prodrug strategy for precise regulation in cancer therapy.

Cite this: CCS Chem.2022, 4, 3878–3888

Link：https://doi.org/10.31635/ccschem.022.202101564

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中国化学会

Chemsoc

原标题：《CCS Chemistry 2022年第12期上线》

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