Per‐6‐Thiol‐Cyclodextrin Engineered [FeFe]‐Hydrogenase Mimic/CdSe Quantum Dot Assembly for Photocatalytic Hydrogen Production,Solar RRL

当前位置： X-MOL 学术 › Solar RRL › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Per‐6‐Thiol‐Cyclodextrin Engineered [FeFe]‐Hydrogenase Mimic/CdSe Quantum Dot Assembly for Photocatalytic Hydrogen Production
Solar RRL ( IF 6.0 ) Pub Date : 2020-09-24 , DOI: 10.1002/solr.202000474
Xu-Bing Li ₁ , Jing-Xin Jian ₁ , Xu-Zhe Wang ₁ , Yang Wang ₁ , Shu-Guang Xia _{1,

2} , Chen-Ho Tung _{1,

2} , Li-Zhu Wu _{1,

2}

Affiliation

[FeFe]‐hydrogenase ([FeFe]‐H₂ase) mimics, inspired by hydrogenases in nature, have emerged as an important class of molecular catalysts toward hydrogen (H₂) evolution. Herein, a per‐6‐thiol‐cyclodextrin (CDSH) engineered [FeFe]‐H₂ase mimic/CdSe quantum dot (QD) assembly is established for effective photocatalytic H₂ evolution. In the assembly, CDSH is first anchored on CdSe QDs via the strong multidentate Cd‐thiol coordination. Then, [FeFe]‐H₂ase mimic is assembled on the QD surface via the host–guest supramolecular interaction between the hydrophobic cavity of cyclodextrin (CD) and the adamantyl (AD) group of [FeFe]‐H₂ase mimic. In neutral aqueous solution of isopropanol, the Fe₂S₂‐AD/CDSH/CdSe assembly exhibits a turnover number (TON) of 1.12 × 10⁵ (based on Fe₂S₂‐AD) under visible light, which is about 12‐fold to the corresponding system without CDSH. Mechanistic insights indicate that the CDSH can not only prevent the aggregation of QDs in acidic conditions, but also balance the interfacial charge (electron and hole) transfer to avoid the photocorrosion of QDs, thereby giving the highest TON of H₂ photogeneration based on [FeFe]‐H₂ase mimics up to date.

中文翻译：

Per-6-巯基-环糊精设计的[FeFe]-氢化酶模拟物/ CdSe量子点组件，用于光催化制氢

受自然界中的加氢酶启发，[FeFe]-加氢酶（[FeFe] -H ₂酶）模拟物已成为促进氢（H ₂）进化的一类重要的分子催化剂。在此，建立了一个由6-硫醇-环糊精（CDSH）设计的[FeFe] -H ₂酶模拟物/ CdSe量子点（QD）组件，以有效地光催化H ₂释放。在组装中，首先通过强大的多齿Cd-硫醇配位将CDSH固定在CdSe QD上。然后，[FeFe] -H ₂酶模拟物通过环糊精（CD）的疏水腔与[FeFe] -H ₂酶模拟物的金刚烷基（AD）基团之间的宿主-客体超分子相互作用组装在QD表面上。在中性异丙醇水溶液中，铁₂ S ₂ -AD / CDSH / CdSe组件在可见光下的周转率（TON）为1.12×10 ⁵（基于Fe ₂ S ₂ -AD），约为没有CDSH的相应系统的12倍。机理研究表明，CDSH不仅可以防止酸性条件下量子点的聚集，而且可以平衡界面电荷（电子和空穴）的转移，从而避免量子点的光腐蚀，从而使基于[FeFe的] H ₂光生化具有最高的TON。] ‐H ₂酶是最新的。

更新日期：2020-09-24

点击分享查看原文

点击收藏

阅读更多本刊最新论文