Hillers-Bendtsen Andreas Erbs, Kjeldal Frederik Ørsted, Høyer Nicolai Machholdt, Mikkelsen Kurt V
Department of Chemistry, H. C. Ørsted Institute, University of Copenhagen, Universitetsparken 5, 2100 Copenhagen, Denmark.
Phys Chem Chem Phys. 2022 Mar 2;24(9):5506-5521. doi: 10.1039/d2cp00226d.
In this paper, we present an investigation concerning the prospects of using nanoparticles to improve solar energy storage properties of three different norbornadiene/quadricyclane derivatives. Computationally, we study how different nanoparticles influence the properties of the systems that relate to the storage of solar energy, namely, the storage energy and the back reaction barrier. Our approach employs hybrid quantum mechanical/molecular mechanical calculations in which the molecular systems are described using density functional theory while the nanoparticles are described using molecular mechanics. The interactions between the two subsystems are determined using polarization dynamics. The results show that the influence of the nanoparticles on the thermochemical properties largely depends on the type of nanoparticle used, the relative orientation with respect to the nanoparticle, and the distance between the the nanoparticle and the molecular system. Additionally, we find indications that copper and/or titanium dioxide nanoparticles can lower the energy barrier of the back reaction for all of the studied systems without significantly lowering the storage capability of the systems. Consequently, the study shows that nanoparticles can potentially be employed in the optimization of molecular photoswitches towards solar energy storage.
在本文中，我们对使用纳米颗粒改善三种不同降冰片二烯/四环烷衍生物的太阳能存储特性的前景进行了研究。通过计算，我们研究了不同的纳米颗粒如何影响与太阳能存储相关的系统特性，即存储能量和逆反应势垒。我们的方法采用了混合量子力学/分子力学计算，其中分子系统使用密度泛函理论进行描述，而纳米颗粒使用分子力学进行描述。两个子系统之间的相互作用通过极化动力学来确定。结果表明，纳米颗粒对热化学性质的影响在很大程度上取决于所使用的纳米颗粒类型、相对于纳米颗粒的相对取向以及纳米颗粒与分子系统之间的距离。此外，我们发现有迹象表明，对于所有研究的系统，铜和/或二氧化钛纳米颗粒可以降低逆反应的能垒，而不会显著降低系统的存储能力。因此，该研究表明，纳米颗粒有可能用于优化分子光开关以实现太阳能存储。
