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Chromophore Dipole Directs Morphology and Photocatalytic Hydrogen Generation
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-04-06 , DOI: 10.1021/jacs.7b12641 Adam S Weingarten 1 , Adam J Dannenhoffer 2 , Roman V Kazantsev 1 , Hiroaki Sai 3 , Dongxu Huang 2 , Samuel I Stupp 1, 2, 3, 4, 5
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-04-06 , DOI: 10.1021/jacs.7b12641 Adam S Weingarten 1 , Adam J Dannenhoffer 2 , Roman V Kazantsev 1 , Hiroaki Sai 3 , Dongxu Huang 2 , Samuel I Stupp 1, 2, 3, 4, 5
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The spontaneous self-assembly of chromophores into light-harvesting antennae provides a potentially low-cost approach to building solar-to-fuel conversion materials. However, designing such supramolecular architectures requires a better understanding of the balance between noncovalent forces among the molecular components. We investigated here the aqueous assembly of perylene monoimide chromophore amphiphiles synthesized with different substituents in the 9-position. The molecular dipole strength decreases as the nature of the substituent is altered from electron donating to electron withdrawing. Compounds with stronger molecular dipoles, in which dipolar interactions stabilize assemblies by 10-15 kJ·mol-1, were found to form crystalline nanoribbons in solution. In contrast, when the molecular dipole moment is small, nanofibers were obtained. Highly blue-shifted absorption maxima were observed in assemblies with large dipoles, indicating strong electronic coupling is present. However, only the moderate dipole compound had the appropriate molecular packing to access charge-transfer excitons leading to enhanced photocatalytic H2 production.
中文翻译：
发色团偶极子指导形态和光催化产氢
发色团自发自组装成光捕获天线为构建太阳能到燃料转换材料提供了一种潜在的低成本方法。然而，设计这种超分子结构需要更好地理解分子组分之间的非共价力之间的平衡。我们在这里研究了在 9 位具有不同取代基合成的苝单酰亚胺发色团两亲物的水性组装。随着取代基的性质从给电子变为吸电子，分子偶极强度降低。具有更强分子偶极子的化合物，其中偶极相互作用使组装体稳定10-15 kJ·mol-1，被发现在溶液中形成结晶纳米带。相反，当分子偶极矩小时，得到纳米纤维。在具有大偶极子的组件中观察到高度蓝移的吸收最大值，表明存在强电子耦合。然而，只有中等偶极子化合物具有适当的分子堆积来获取电荷转移激子，从而增强光催化氢气的产生。
更新日期：2018-04-06
中文翻译：
发色团偶极子指导形态和光催化产氢
发色团自发自组装成光捕获天线为构建太阳能到燃料转换材料提供了一种潜在的低成本方法。然而，设计这种超分子结构需要更好地理解分子组分之间的非共价力之间的平衡。我们在这里研究了在 9 位具有不同取代基合成的苝单酰亚胺发色团两亲物的水性组装。随着取代基的性质从给电子变为吸电子，分子偶极强度降低。具有更强分子偶极子的化合物，其中偶极相互作用使组装体稳定10-15 kJ·mol-1，被发现在溶液中形成结晶纳米带。相反，当分子偶极矩小时，得到纳米纤维。在具有大偶极子的组件中观察到高度蓝移的吸收最大值，表明存在强电子耦合。然而，只有中等偶极子化合物具有适当的分子堆积来获取电荷转移激子，从而增强光催化氢气的产生。
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