Templated 2D Polymer Heterojunctions for Improved Photocatalytic Hydrogen Production.
Templated 2D Polymer Heterojunctions for Improved Photocatalytic Hydrogen Production.
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用于改进光催化制氢的模板化二维聚合物异质结。
DOI：
10.1002/adma.202300037
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发表时间：
2023
期刊：
影响因子：
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通讯作者：
Aitchison CM
中科院分区：
文献类型：
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作者：
Aitchison CM
2D聚合物由于其可调谐性、电荷传输特性和鲁棒性而成为太阳能燃料生产中最有前途的有机光催化剂之一。然而，它们难以加工，因此对结合这些组分的异质结材料的形成的研究有限。在这项工作中，使用一种新的模板方法来结合基于亚胺的供体聚合物和通过Knoevenagel缩合形成的受体聚合物联合收割机。异质结的形成被证明是高度依赖于拓扑匹配的供体和受体聚合物与最活跃的模板材料被发现之间的三至九倍更活跃的crosslinking比其组成成分。瞬态吸收光谱表明，这种改善是由于更快的电荷分离和更有效的电荷提取的模板异质结。该模板材料显示出非常高的析氢速率，在抗坏血酸空穴清除剂的情况下>20 mmol h−1m− 2，但在仅存在水和钴基氧化还原介体的情况下也产生氢。这表明通过这种方法获得的改进的电荷分离界面和减少的捕获可能适合于Z方案形成。
2D polymers have emerged as one of the most promising classes of organic photocatalysts for solar fuel production due to their tunability, charge‐transport properties, and robustness. They are however difficult to process and so there are limited studies into the formation of heterojunction materials incorporating these components. In this work, a novel templating approach is used to combine an imine‐based donor polymer and an acceptor polymer formed through Knoevenagel condensation. Heterojunction formation is shown to be highly dependent on the topological match of the donor and acceptor polymers with the most active templated material found to be between three and nine times more active for photocatalysis than its constituent components. Transient absorption spectroscopy reveals that this improvement is due to faster charge separation and more efficient charge extraction in the templated heterojunction. The templated material shows a very high hydrogen evolution rate of >20 mmol h−1m−2with an ascorbic acid hole scavenger but also produces hydrogen in the presence of only water and a cobalt‐based redox mediator. This suggests the improved charge‐separation interface and reduced trapping accessed through this approach could be suitable for Z‐scheme formation.