Fernández-Climent Roser, Redondo Jesús, García-Tecedor Miguel, Spadaro Maria Chiara, Li Junnan, Chartrand Daniel, Schiller Frederik, Pazos Jhon, Hurtado Mikel F, de la Peña O'Shea Victor, Kornienko Nikolay, Arbiol Jordi, Barja Sara, Mesa Camilo A, Giménez Sixto
Institute of Advanced Materials (INAM), Universitat Jaume I, Av. de Vicente Sos Baynat, s/n, 12006 Castelló, Spain.
Department of Polymers and Advanced Materials, Centro de Física de Materiales, University of the Basque Country UPV/EHU, 20018 San Sebastián, Spain.
ACS Catal. 2023 Jul 26;13(15):10457-10467. doi: 10.1021/acscatal.3c01673. eCollection 2023 Aug 4.
Copper-based hydrogen evolution electrocatalysts are promising materials to scale-up hydrogen production due to their reported high current densities; however, electrode durability remains a challenge. Here, we report a facile, cost-effective, and scalable synthetic route to produce CuS electrocatalysts, exhibiting hydrogen evolution rates that increase for ∼1 month of operation. Our CuS electrodes reach a state-of-the-art performance of ∼400 mA cm at -1 V vs RHE under mild conditions (pH 8.6), with almost 100% Faradaic efficiency for hydrogen evolution. The rise in current density was found to scale with the electrode electrochemically active surface area. The increased performance of our CuS electrodes correlates with a decrease in the Tafel slope, while analyses by X-ray photoemission spectroscopy, X-ray diffraction, and spectroelectrochemistry cooperatively revealed the Cu-centered nature of the catalytically active species. These results allowed us to increase fundamental understanding of heterogeneous electrocatalyst transformation and consequent structure-activity relationship. This facile synthesis of highly durable and efficient CuS electrocatalysts enables the development of competitive electrodes for hydrogen evolution under mild pH conditions.
基于铜的析氢电催化剂因其报道的高电流密度而成为有望扩大制氢规模的材料；然而，电极耐久性仍然是一个挑战。在此，我们报告了一种简便、经济高效且可扩展的合成路线来制备硫化铜（CuS）电催化剂，其析氢速率在运行约1个月后有所增加。我们的硫化铜电极在温和条件（pH 8.6）下相对于可逆氢电极（RHE）在-1 V时达到了约400 mA/cm²的先进性能，析氢的法拉第效率几乎达到100%。发现电流密度的增加与电极的电化学活性表面积成比例。我们的硫化铜电极性能的提高与塔菲尔斜率的降低相关，同时通过X射线光电子能谱、X射线衍射和光谱电化学分析共同揭示了催化活性物种以铜为中心的性质。这些结果使我们能够加深对非均相电催化剂转变以及随之而来的结构-活性关系的基本理解。这种简便合成高耐久性和高效硫化铜电催化剂的方法能够开发出在温和pH条件下用于析氢的有竞争力的电极。
