题目：

High-performance Photoelectrochemical Hydrogen Production Using Asymmetric Quantum Dots

作者：

Kanghong Wang^1,2,3, Chao Wang², Yi Tao¹, Zikun Tang¹, Daniele Benetti²*, François Vidal², Yu Liu⁴, Mark H. Rummeli^4,5,6,7, Haiguang Zhao⁸*, Federico Rosei²*, and Xuhui Sun¹*

单位：

¹Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, P. R. China.

²Centre Énergie, Matériaux et Télécommunications, Institut National de la Recherche Scientifique, 1650 Boul. Lionel Boulet, J3×1P7, Varennes, Québec Canada.

³Suzhou Institute for Advanced Research, University of Science and Technology of China, Suzhou 215123, P. R. China.

⁴Soochow Institute for Energy and Materials Innovation, college of Physics, Optoelectronics and Energy, Collaborative Innovation Center of Suzhou Nano Science and Technology, Key Laboratory of Advanced Carbon Materials and Wearable Energy, Technologies of Jiangsu Province, Soochow University, Suzhou 215000, P. R. China.

⁵Centre of Polymer and Carbon Materials, Polish Academy of Sciences, M. Curie-Sklodowskiej 34, Zabrze 41–819, Poland.

⁶Institute for Complex Materials, IFW Dresden, 20 Helmholtz Strasse, 01069 Dresden, Germany.

⁷Institute of Environmental Technology, VSB-Technical University of Ostrava, 17. Listopadu 15, Ostrava 708 33, Czech Republic.

⁸State Key Laboratory of Bio-Fibers and Eco-Textiles, College of Textiles & Clothing, College of Physics, Qingdao University, No. 308 Ningxia Road, Qingdao 266071, P. R. China.

摘要：

Solar-driven photoelectrochemical (PEC) reactions using colloidal quantum dots (QDs) as photoabsorbers have shown great potential for the production of clean fuels. However, the low H2 evolution rate, consistent with low values of photocurrent density, and their limited operational stability are still the main obstacles. To address these challenges, the heterostructure engineering of asymmetric capsule-shaped CdSe/CdxZn1-xSe QDs with broad absorption and efficient charge extraction compared to pure-shell QDs is reported. By engineering the shell composition from pure ZnSe shells into CdxZn1-xSe gradient shells, the electron transfer rate increased from 4.0 × 107 s⁻¹to 32.7 × 107 s⁻¹. Moreover, the capsule-shaped architecture enables more efficient spatial carrier separation, yielding a saturated current density of average of 25.4 mA cm⁻²under AM 1.5 G one sun illumination. This value is the highest ever observed for QDs-based devices and comparable to the best-known Si-based devices, perovskite-based devices, and metal oxide-based devices. Furthermore, PEC devices based on heterostructured QDs maintained 96% of the initial current density after 2 h and 82% after 10 h under continuous illumination, respectively. The results represent a breakthrough in hydrogen production using heterostructured asymmetric QDs.

影响因子：

19.924

分区情况：

一区

链接：

https://doi.org/10.1002/adfm.202400580