Brändlin Mathis, Pfund Björn, Wenger Oliver S
Department of Chemistry, University of Basel, Basel, Switzerland.
Department of Chemistry, Michigan State University, East Lansing, MI, USA.
Nat Chem. 2025 Aug 25. doi: 10.1038/s41557-025-01912-x.
Photochemistry involves elementary steps in which single electrons are transferred, but artificial photosynthesis requires multi-electron reactions. This discrepancy necessitates light-driven charge accumulation, which has so far proved very difficult to achieve without sacrificial redox reagents. Here we report a molecular donor-photosensitizer-acceptor compound in which light absorption leads to the reversible accumulation of two positive and two negative charges. The resulting photoproduct forms with an overall quantum yield of 37%, has a lifetime of more than 100 ns and stores 3.0 eV of energy. The use of a structurally well-defined molecular compound provides fundamental insights into how light-driven multi-electron transfer can generally be performed efficiently and sustainably, at irradiance levels orders of magnitude below those required in comparable systems. This represents a step towards more application-oriented research on solar fuels from fundamental studies of photoinduced (single) electron transfer.
光化学涉及单电子转移的基元步骤，但人工光合作用需要多电子反应。这种差异使得光驱动电荷积累成为必要，而到目前为止，在没有牺牲性氧化还原试剂的情况下，这已证明很难实现。在此，我们报道了一种分子供体 - 光敏剂 - 受体化合物，其中光吸收导致两个正电荷和两个负电荷的可逆积累。所产生的光产物形成时的总量子产率为37%，寿命超过100纳秒，并储存3.0电子伏特的能量。使用结构明确的分子化合物为光驱动多电子转移通常如何在比同类系统所需辐照度低几个数量级的水平上高效且可持续地进行提供了基本见解。这代表着从光致（单）电子转移的基础研究迈向对太阳能燃料更具应用导向性研究的一步。
