Hybrid photoanodes based on surface-bound host-guest molecular assemblies

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem Pub Date : 2024-12-09 DOI:10.1016/j.chempr.2024.11.003

Jiaxuan Wang, Daokuan Li, Xiaona Li, Guoquan Liu, Yong Zhu, Licheng Sun, Fei Li

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Abstract

In artificial photosynthesis, molecule/semiconductor hybrids combine the merits of the high activity of molecular catalysts and the high stability of semiconductor light absorbers. We report here a host-guest strategy for hybrid photoanode fabrication, where phosphonate-derivatized cyclodextrins (p-CDs) as hosts were anchored on the surface of a tungsten oxide (WO₃) film, and molecular catalysts as guests were self-encapsulated into the cavities of p-CDs in either aqueous or organic media. By choosing an admantanyl cobaloxime complex (Co1) as a molecular water oxidation catalyst, the resulting WO₃|p-CD|Co1 photoanode exhibited high photoelectrochemical (PEC) activity and stability for water oxidation due to the unexpected efficient charge separation and the strong affinity between p-CD and catalyst. In addition, the WO₃|p-CD was identified to be a versatile platform for catalyst loading, when a 4-hydroxy-2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) derivative was employed as the guest molecule, the conversion yield of PEC alcohol oxidation to aldehyde was dramatically increased.

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基于表面结合主客体分子组装的杂化光阳极

在人工光合作用中，分子/半导体杂合体结合了分子催化剂的高活性和半导体光吸收剂的高稳定性的优点。我们在此报告了一种用于杂化光阳极制造的主客体策略，其中磷酸盐衍生化环糊精（p-CDs）作为宿主锚定在氧化钨（WO3）薄膜的表面，分子催化剂作为客体被自封装在水或有机介质中的p-CDs的空腔中。通过选择admantanyl cobal肟络合物（Co1）作为分子水氧化催化剂，得到的WO3|p-CD|Co1光阳极由于意想到的高效电荷分离和p-CD与催化剂之间的强亲和力，具有较高的光电化学（PEC）活性和水氧化稳定性。此外，WO3|p-CD是一种多用途的催化剂负载平台，当4-羟基-2,2,6,6-四甲基哌啶1-氧（TEMPO）衍生物作为客体分子时，PEC醇氧化制醛的转化率显著提高。

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来源期刊

Chem Environmental Science-Environmental Chemistry

CiteScore

32.40

自引率

1.30%

发文量

281

期刊介绍： Chem, affiliated with Cell as its sister journal, serves as a platform for groundbreaking research and illustrates how fundamental inquiries in chemistry and its related fields can contribute to addressing future global challenges. It was established in 2016, and is currently edited by Robert Eagling.