Department of Chemistry, The University of Alabama , Tuscaloosa, Alabama 35487-0336, United States.
Center for Materials for Information Technology, The University of Alabama , Tuscaloosa, Alabama 35487-0209, United States.
J Am Chem Soc. 2015 Sep 23;137(37):11996-2005. doi: 10.1021/jacs.5b05367. Epub 2015 Sep 15.
Developing high-efficiency, durable, and low-cost catalysts based on earth-abundant elements for the oxygen evolution reaction (OER) is essential for renewable energy conversion and energy storage devices. In this study, we report a highly active nanostructured electrode, NanoCOT, which contains carbon, oxygen, and titanium, for efficient OER in alkaline solution. The NanoCOT electrode is synthesized from carbon transformation of TiO2 in an atmosphere of methane, hydrogen, and nitrogen at a high temperature. The NanoCOT exhibits enhanced OER catalytic activity in alkaline solution, providing a current density of 1.33 mA/cm(2) at an overpotential of 0.42 V. This OER current density of a NanoCOT electrode is about 4 times higher than an oxidized Ir electrode and 15 times higher than a Pt electrode because of its nanostructured high surface area and favorable OER kinetics. The enhanced catalytic activity of NanoCOT is attributed to the presence of a continuous energy band of the titanium oxide electrode with predominantly reduced defect states of Ti (e.g., Ti(1+), Ti(2+), and Ti(3+)) formed by chemical reduction with hydrogen and carbon. The OER performance of NanoCOT can also be further enhanced by decreasing its overpotential by 150 mV at a current density of 1.0 mA/cm(2) after coating its surface electrophoretically with 2.0 nm IrOx nanoparticles.
开发基于丰富元素的高效、持久和低成本催化剂对于可再生能源转换和储能设备至关重要。在这项研究中,我们报告了一种高效的纳米结构电极 NanoCOT,它包含碳、氧和钛,可在碱性溶液中实现高效的析氧反应(OER)。NanoCOT 电极是通过在高温下将 TiO2 在甲烷、氢气和氮气的气氛中进行碳转化合成的。NanoCOT 在碱性溶液中表现出增强的 OER 催化活性,在 0.42 V 的过电势下提供 1.33 mA/cm2 的电流密度。由于其纳米结构的高表面积和有利的 OER 动力学,NanoCOT 电极的 OER 电流密度大约是氧化铱电极的 4 倍,铂电极的 15 倍。NanoCOT 的增强催化活性归因于钛氧化物电极的连续能带的存在,以及通过氢和碳的化学还原形成的主要还原缺陷态 Ti(例如 Ti(1+)、Ti(2+)和 Ti(3+))。通过在其表面电泳涂覆 2.0nm 的 IrOx 纳米粒子,可以将 NanoCOT 的过电势降低 150mV,在 1.0mA/cm2 的电流密度下进一步提高其 OER 性能。