Wang Xinyu, Yu Xu, Wu Shuang, He Pinyi, Qin Fu, Yao Yongkang, Bai Jianliang, Yuan Guojun, Ren Lili
School of Chemistry & Chemical Engineering, Southeast University, Nanjing 211189, China.
School of Environment and Chemical Engineering, Anhui Vocational and Technical College, Hefei 230011, China.
ACS Appl Mater Interfaces. 2023 Mar 29;15(12):15533-15544. doi: 10.1021/acsami.3c00547. Epub 2023 Mar 15.
The rational design of highly efficient and stable electrocatalysts for the oxygen evolution reaction (OER) is an urgent need but remains challenging for various sustainable energy systems. How to adjust the atomic structure and electronic structure of the active center is a key bottleneck problem. Accelerating the electron transfer process and the deep self-reconstruction of active sites could be a cost-effective strategy toward electrocatalytic OER catalyst development. Here, a crystalline-amorphous (c-a) coupled NiS/NiP electrocatalyst self-supported on nickel foam with an intimate interface was developed via a feasible solvothermal-electrochemistry method. The coupling interface of the crystalline structure with high conductivity and amorphous structure with numerous potential active sites could regulate the electronic structure and optimize the adsorption/desorption of O-containing species, ultimately resulting in high OER catalytic performance. The obtained NiS/NiP/NF presents a low OER overpotential of 265 mV to obtain 10 mA·cm and a small Tafel slope of 51.6 mV·dec. Also, the catalyst with the coupled interface exhibited significantly enhanced long-term stability compared to the other two catalysts, with <5% decay in OER activity over 20 h of continuous operation, while that of NiS/NF and NiP/NF decreased by about 30 and 50%, respectively. This study provides inspiration for other energy conversion reactions in optimizing the performance of catalysts by coupling crystalline-amorphous structures.
为析氧反应（OER）合理设计高效稳定的电催化剂是各种可持续能源系统的迫切需求，但仍具有挑战性。如何调整活性中心的原子结构和电子结构是一个关键的瓶颈问题。加速电子转移过程和活性位点的深度自我重构可能是开发电催化OER催化剂的一种经济有效的策略。在此，通过一种可行的溶剂热-电化学方法，制备了一种自支撑在泡沫镍上、具有紧密界面的晶态-非晶态（c-a）耦合NiS/NiP电催化剂。具有高导电性的晶体结构与具有众多潜在活性位点的非晶态结构的耦合界面可以调节电子结构，优化含O物种的吸附/解吸，最终实现高OER催化性能。所制备的NiS/NiP/NF在电流密度为10 mA·cm时具有265 mV的低OER过电位和51.6 mV·dec的小塔菲尔斜率。此外，与其他两种催化剂相比，具有耦合界面的催化剂表现出显著增强的长期稳定性，在连续运行20 h后OER活性衰减<5%，而NiS/NF和NiP/NF的活性分别下降约30%和50%。本研究为通过耦合晶态-非晶态结构优化催化剂性能的其他能量转换反应提供了启示。
