Liu Yongpeng, Bouri Maria, Yao Liang, Xia Meng, Mensi Mounir, Grätzel Michael, Sivula Kevin, Aschauer Ulrich, Guijarro Néstor
Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Station 6, Lausanne, 1015, Switzerland.
Department of Chemistry and Biochemistry, University of Bern, Freiestrasse 3, CH-3012, Bern, Switzerland.
Angew Chem Int Ed Engl. 2021 Oct 25;60(44):23651-23655. doi: 10.1002/anie.202108994. Epub 2021 Oct 1.
Gathering information on the atomic nature of reactive sites and trap states is key to fine tuning catalysis and suppressing deleterious surface voltage losses in photoelectrochemical technologies. Here, spectroelectrochemical and computational methods were combined to investigate a model photocathode from the promising chalcopyrite family: CuIn Ga S . We found that voltage losses are linked to traps induced by surface Ga and In vacancies, whereas operando Raman spectroscopy revealed that catalysis occurred at Ga, In, and S sites. This study allows establishing a bridge between the chalcopyrite's performance and its surface's chemistry, where avoiding formation of Ga and In vacancies is crucial for achieving high activity.
获取有关反应位点和陷阱态原子性质的信息是微调催化作用并抑制光电化学技术中有害表面电压损失的关键。在此，将光谱电化学和计算方法相结合，研究了来自前景广阔的黄铜矿族的一种模型光电阴极：CuInGaS 。我们发现电压损失与由表面Ga和In空位诱导的陷阱有关，而原位拉曼光谱表明催化作用发生在Ga、In和S位点。这项研究有助于在黄铜矿的性能与其表面化学之间架起一座桥梁，其中避免形成Ga和In空位对于实现高活性至关重要。
