Decatungstate

  • 文章类型: Journal Article
    在此,我们描述了一种可持续且有效的光催化方法,用于手性亚磺酰基亚胺的立体选择性自由基烷基化。通过使用容易获得的非预官能化自由基前体和低负载的TBADT作为直接HAT光催化剂,我们成功地获得了不同的手性胺,在温和的条件下,高产率和优异的非对映选择性。这种方法提供了一种有效的方法来获取不同的药物相关化合物,包括天然和合成的α-氨基酸,芳基乙基胺,以及批准的药物和天然产品中常见的其他结构图案。
    Herein we describe a sustainable and efficient photocatalytic method for the stereoselective radical alkylation of chiral sulfinyl imines. By employing readily available non-prefunctionalized radical precursors and the cost-effective TBADT as a direct HAT photocatalyst, we successfully obtain diverse chiral amines with high yields and excellent diastereoselectivity under mild conditions. This method provides an efficient approach for accessing a diverse array of medicinally relevant compounds, including both natural and synthetic α-amino acids, aryl ethyl amines, and other structural motifs commonly found in approved pharmaceuticals and natural product.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    过渡金属二硫属化合物(TMD)是有前途的二维纳米材料,可用于多种应用,但是它们内在的化学惰性阻碍了它们的修饰。在这里,提出了一种用于2H-MoS2和2H-MoSe2的光催化酰化的新方法,利用四丁基十一钨酸铵((nBu4N)4W10O32)多金属氧酸盐配合物作为催化剂,并利用常规卤素灯作为辐射源。通过利用TMD的半导体特性,这些材料的功能化出现了新的途径。这种新颖的光催化方案构成了基于催化方案的2D纳米材料化学修饰的第一份报告,适用于脂肪族和芳香族基材。通过使用烷基和芳香醛来探索TMD的去钨酸盐光催化酰化反应的范围,并且通过多种光谱学证实了该方法的成功,热,显微成像,和氧化还原技术。这种用于修饰2D纳米材料的催化方法在TMD的功能化协议中引入了原子经济原理。它标志着在TMD修饰和纳米材料化学领域向更可持续和有效的方法转变。
    Transition metal dichalcogenides (TMDs) are promising 2D nanomaterials for diverse applications, but their intrinsic chemical inertness hinders their modification. Herein, a novel approach is presented for the photocatalytic acylation of 2H-MoS2 and 2H-MoSe2, utilizing tetrabutyl ammonium decatungstate ((nBu4N)4W10O32) polyoxometalate complex as a catalyst and a conventional halogen lamp as a source of irradiation. By harnessing the semiconducting properties of TMDs, new avenues emerge for the functionalization of these materials. This novel photocatalytic protocol constitutes the first report on the chemical modification of 2D nanomaterials based on a catalytic protocol and applies to both aliphatic and aromatic substrates. The scope of the decatungstate-photocatalyzed acylation reaction of TMDs is explored by employing an alkyl and an aromatic aldehyde and the success of the methodology is confirmed by diverse spectroscopic, thermal, microscopy imaging, and redox techniques. This catalytic approach on modifying 2D nanomaterials introduces the principles of atom economy in a functionalization protocol for TMDs. It marks a transformative shift toward more sustainable and efficient methodologies in the realm of TMD modification and nanomaterial chemistry.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    我们在本文中报告了吲哚的方便且可扩展的脱芳烃加氢酰化反应。采用容易获得的醛作为酰基源,TBADT作为廉价的直接HAT光催化剂,在温和条件下,各种吲哚衍生物以良好至优异的产率以及极大的非对映选择性转化为合成上感兴趣的2-酰基吲哚。成功开发了反应的不对称形式,并进行了实验机理研究,以进一步了解假定的反应途径。
    We report herein a convenient and scalable dearomative hydroacylation reaction of indoles. Employing readily available aldehydes as the acyl source and TBADT as an inexpensive direct HAT photocatalyst, a variety of indoles derivatives were converted into synthetically interesting 2-acylindolines in good to excellent yields as well as great diastereoselectivity under mild conditions. An asymmetric version of the reaction was successfully developed and an experimental mechanistic investigation was carried out in order to gain further insights on the assumed reaction pathway.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    化合物[Ag44(W10O32)(StBu)24(CF3COO)8](CF3COO)6·6H2O(1)通过一锅法合成。这是分离包含[W10O32]6-模板的新硫醇化银簇的第一种情况,该模板通过自组装过程从WO42-聚氧阴离子转变。还原的[W10O32]6-模板的阴离子性质和有效的银-氧相互作用有助于1中Ag44纳米轮的形成。发光,1的光催化活性和电化学性能进行了研究。
    Compound [Ag44 (W10 O32 )(St Bu)24 (CF3 COO)8 ](CF3 COO)6  ⋅ 6H2 O (1) was synthesized through a one-pot method. This is the first case of isolating a new silver thiolate cluster containing a [W10 O32 ]6- template which transforms from WO4 2- polyoxoanion through a self-assembly process. The anionic nature of the reduced [W10 O32 ]6- template and the effective silver-oxygen interaction contribute to the formation of the Ag44 nanowheel in 1. The luminescence, photocatalytic activity and electrochemistry properties of 1 were studied.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    The development of photocatalysts making full use of natural light sources is highly desired for the remediation of marine oil spill pollution, which is full of challenges. Herein, we demonstrate a well-defined visible-near-infrared-responsive g-C3N4Hx+ reduced decatungstate charge-transfer salt (RCD-CTS), which possess efficient light-absorption ability ranging from visible light to the near infrared region. The RCD-CTS photocatalyst exhibits excellent performance for photocatalytic removal of petroleum hydrocarbon. The structural characterization and theoretical calculation confirmed strong chemical interaction between components and partly reduction of decatungstate results in the plasmonic properties and the absorption of near infrared light. As a results, it is proposed that\"hot electrons\"transfer process generated by plasmon effect promotes the efficient separation of charge-carriers. Ultimately, this work sheds light on the discovery and application of visible-near-infrared-responsive optical materials that may be exploited further in artificial photosynthesis, solar energy conversion, and phototherapy.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

       PDF(Sci-hub)

  • 文章类型: Journal Article
    已开发出一种通过脱钨酸盐光催化实现的温和且选择性的C(sp3)-H好氧氧化。该反应可以在微流反应器中得到显著改善,从而能够安全使用氧气并增强反应混合物的辐照。我们的方法允许活化和未活化的C-H键的氧化(30个实施例)。选择性氧化天然支架的能力,如(-)-氨溴化物,醋酸孕烯醇酮,(+)-sclareolide,还有青蒿素,举例说明了这种新方法的实用性。
    A mild and selective C(sp3 )-H aerobic oxidation enabled by decatungstate photocatalysis has been developed. The reaction can be significantly improved in a microflow reactor enabling the safe use of oxygen and enhanced irradiation of the reaction mixture. Our method allows for the oxidation of both activated and unactivated C-H bonds (30 examples). The ability to selectively oxidize natural scaffolds, such as (-)-ambroxide, pregnenolone acetate, (+)-sclareolide, and artemisinin, exemplifies the utility of this new method.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

       PDF(Pubmed)

  • 文章类型: Journal Article
    Synergistic control over the SH 2 transition states of hydrogen abstraction exploiting polar and steric effects provides a promising cooperative strategy for site-selective C(sp3 )-H functionalization using decatungstate anion photocatalysis. By using this photocatalytic approach, the C-H bonds of substituted lactones and cyclic ketones were functionalized selectively. In the remarkable case of 2-isoamyl 4-tert-butyl cyclohexanone (1 t) bearing five methyl, five methylene, and three methine C-H bonds, one methine C-H bond in the isoamyl tether was selectively functionalized.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

       PDF(Sci-hub)

公众号