Zhao Dandan, Pi Yecan, Shao Qi, Feng Yonggang, Zhang Ying, Huang Xiaoqing
College of Chemistry, Chemical Engineering and Materials Science , Soochow University , Suzhou , Jiangsu 215123 , China.
ACS Nano. 2018 Jun 26;12(6):6245-6251. doi: 10.1021/acsnano.8b03141. Epub 2018 May 17.
The development of electrocatalysts with high activity and stability for oxygen evolution reaction (OER) is critically important, the one being regarded as the bottleneck process of overall water splitting. Herein, we fulfill significant OER improvement in both activity and stability by constructing a class of Ni(OH)-CeO supported on carbon paper (Ni Ce @CP) with an intimate hydroxide (Ni(OH))-oxide (CeO) interface. Such interface largely promotes the OER activity with a low overpotential of 220 mV at 10 mA cm and a small Tafel slope of 81.9 mV dec in 1 M KOH. X-ray photoelectron spectroscopy analysis shows that the intimate interface induced by the strong electronic interactions between Ni(OH) and CeO involves the modulation of binding strength between intermediates and catalysts, making a great contribution to the OER enhancement. Importantly, such intimate interface structures can be largely maintained even after a long-time stability test. We have further demonstrated that, when pairing the NiCe@CP after phosphorization (P-NiCe@CP), the NiCe@CP and P-NiCe@CP assembly is highly active and stable for overall water splitting with a low voltage of 1.68 V at 25 mA cm and negligible stability delay over 30 h of continuous operation, which are much better than the commercial Ir/C and Pt/C.
开发具有高活性和稳定性的析氧反应(OER)电催化剂至关重要,该反应被视为全水解的瓶颈过程。在此,我们通过构建一类负载在碳纸上的Ni(OH)-CeO(Ni Ce @CP),其具有紧密的氢氧化物(Ni(OH))-氧化物(CeO)界面,在活性和稳定性方面实现了显著的OER性能提升。这种界面在1 M KOH中,在10 mA cm时具有220 mV的低过电位和81.9 mV dec的小塔菲尔斜率,极大地促进了OER活性。X射线光电子能谱分析表明,Ni(OH)和CeO之间强电子相互作用诱导的紧密界面涉及中间体与催化剂之间结合强度的调节,对OER增强有很大贡献。重要的是,即使经过长时间稳定性测试,这种紧密界面结构仍能在很大程度上得以保持。我们进一步证明,将磷化后的NiCe@CP(P-NiCe@CP)配对时,NiCe@CP和P-NiCe@CP组件对于全水解具有高活性和稳定性,在25 mA cm时低电压为1.68 V,连续运行30 h的稳定性延迟可忽略不计,这比商业Ir/C和Pt/C要好得多。