Ulm University, Institute of Analytical and Bioanalytical Chemistry, Albert-Einstein-Allee 11, 89081, Ulm, Germany.
Friedrich-Schiller University Jena, Institute of Organic Chemistry and Macromolecular Chemistry, Lessingstraße 8, 07743, Jena, Germany.
Angew Chem Int Ed Engl. 2023 May 22;62(22):e202217196. doi: 10.1002/anie.202217196. Epub 2023 Apr 25.
Heterogeneous light-driven catalysis is a cornerstone of sustainable energy conversion. Most catalytic studies focus on bulk analyses of the hydrogen and oxygen evolved, which impede the correlation of matrix heterogeneities, molecular features, and bulk reactivity. Here, we report studies of a heterogenized catalyst/photosensitizer system using a polyoxometalate water oxidation catalyst and a model, molecular photosensitizer that were co-immobilized within a nanoporous block copolymer membrane. Via operando scanning electrochemical microscopy (SECM), light-induced oxygen evolution was determined using sodium peroxodisulfate (Na S O ) as sacrificial electron acceptor. Ex situ element analyses provided spatially resolved information on the local concentration and distribution of the molecular components. Infrared attenuated total reflection (IR-ATR) studies of the modified membranes showed no degradation of the water oxidation catalyst under the reported light-driven conditions.
非均相光驱动催化是可持续能源转化的基石。大多数催化研究都集中在对析氢和析氧的整体分析上，这阻碍了对基质异质性、分子特征和整体反应性的关联。在这里，我们报告了使用多金属氧酸盐水氧化催化剂和模型分子光敏剂的异质化催化剂/光敏剂系统的研究，该系统被共固定在纳米多孔嵌段共聚物膜内。通过现场扫描电化学显微镜（SECM），使用过硫酸钠（Na2S2O8）作为牺牲电子受体来确定光诱导的氧气产生。对修饰膜的原位元素分析提供了关于分子成分局部浓度和分布的空间分辨信息。改性膜的红外衰减全反射（IR-ATR）研究表明，在报道的光驱动条件下，水氧化催化剂没有降解。
