2D pyrene-based metal–organic framework nanobelts as efficient photocatalysts for the coupling of thiols into disulfides,Inorganic Chemistry Frontiers

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2D pyrene-based metal–organic framework nanobelts as efficient photocatalysts for the coupling of thiols into disulfides
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2024-07-15 , DOI: 10.1039/d4qi01273a
Xin Zhao ₁ , Yajun Zhao ₁ , Tao He ₂ , Jing-Tong Deng ₂ , Zong-Wen Mo ₁ , Jiewei Liu _{1,

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Affiliation

Photocatalytic coupling of thiols is a promising green approach to obtain disulfides. In this work, we report a stable pyrene-based MOF (Ni-PTTB) and its exfoliated two-dimensional (2D) nanobelts (Ni-PTTB-NB), which were prepared through the self-assembly of 1,3,6,8-tetrakis(3-carboxyphenyl) pyrene (H₄PTTB) and Ni(NO₃)₂·6H₂O. Taking advantages of the uniformly dispersed π-conjugated pyrene units, the obtained pyrene-based MOFs displayed visible-light absorption as well as intriguing optoelectronic properties. Interestingly, the 2D Ni-PTTB-NB showed obviously improved charge separation and migration compared to the pristine bulk Ni-PTTB, as revealed by a range of photoelectrochemical tests as well as Kelvin probe force microscopy (KPFM) measurements. Importantly, the Ni-PTTB-NB exhibited exceptional catalytic performance in the photocatalytic coupling of thiols in the air, giving rise to a 99% conversion of thiols and 99% selectivity of the disulfide products. Mechanism studies disclosed that the thiyl radicals are important intermediate in the catalytic process, which are obtained through the oxidation of thiols by the photogenerated holes. This work provides insights into the future design and development of 2D MOFs for the photocatalytic synthesis of high-value organic compounds.

中文翻译：

二维芘基金属有机骨架纳米带作为硫醇偶联成二硫化物的有效光催化剂

硫醇的光催化偶联是一种有前途的获得二硫化物的绿色方法。在这项工作中，我们报告了一种稳定的基于芘的MOF（Ni-PTTB）及其剥离的二维（2D）纳米带（Ni-PTTB-NB），它们是通过1,3,6的自组装制备的， 8-四(3-羧基苯基)芘 (H ₄ PTTB) 和 Ni(NO ₃ ) ₂ ·6H ₂ O。利用均匀分散的π-共轭芘单元，所获得的芘基MOF表现出可见光吸收以及有趣的光电特性。有趣的是，一系列光电化学测试以及开尔文探针力显微镜 (KPFM) 测量表明，与原始块状 Ni-PTTB 相比，2D Ni-PTTB-NB 显示出明显改善的电荷分离和迁移。重要的是，Ni-PTTB-NB在空气中硫醇的光催化偶联中表现出优异的催化性能，硫醇的转化率为99%，二硫化物产物的选择性为99%。机理研究表明，硫基自由基是催化过程中重要的中间体，它是通过光生空穴氧化硫醇而获得的。这项工作为未来用于光催化合成高价值有机化合物的 2D MOF 的设计和开发提供了见解。

更新日期：2024-07-15

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