The global trend toward automatization and miniaturization of smart devices has triggered the development of reliable off‐grid power sources with low economic and environmental impact. Such autonomy can be provided when a photovoltaic cell is integrated with an electrochemical double‐layer capacitor in one monolithic power pack. This work demonstrates a reliable and straightforward approach to monolithically integrate high‐performance organic solar cells with mesoporous nitrogen‐doped carbon nanosphere‐based supercapacitors in a single device with a three‐electrode configuration. To assess the efficiency of the device, a novel approach is presented that relies on the direct monitoring of both integrating parts during illuminated and dark phases and accounts for possible losses. The evaluation with the standard literature approach shows an outstanding performance of the integrated photosupercapacitor with a peak photoelectrochemical energy conversion efficiency of 17%. However, this type of efficiency does not properly represent the real overall efficiency of the device. Based on the newly developed efficiency calculation, a more modest overall cycle efficiency of 2% is obtained, which represents the overall performance of the integrated device in a better way. This versatile evaluation approach is applicable for all kinds of integrated multifunctional photoconversion–storage systems.
The increasing energy demand for diverse applications requires new types of devices and materials. Multifunctional materials that can fulfill different roles are of high interest as they can allow fabricating devices that can both convert and store energy. Herein, organic donor–acceptor redox polymers that can function as charge storage materials in batteries and as donor materials in bulk heterojunction (BHJ) photovoltaic devices are investigated. Based on its reversible redox chemistry, phenothiazine is used as the main building block in the conjugated copolymer design and combined with diketopyrrolopyrrol and benzothiadiazole as electron‐poor comonomers to shift the optical absorption into the visible region. The resulting polymers show excellent cycling stability as positive electrode materials in lithium–organic batteries at discharge potentials of 3.6–3.7 V versus Li/Li+ as well as good performances in BHJ solar cells with up to 1.9% power conversion efficiency. This study shows that the design of such multifunctional materials is possible, however, that it also faces challenges, as essential properties for good device function can lead to diametrically opposite requirements in materials design.
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