Department of Chemistry and Geochemistry, Colorado School of Mines , Golden, Colorado 80401, United States.
Department of Chemical and Biological Engineering, Colorado School of Mines , Golden, Colorado 80401, United States.
J Am Chem Soc. 2016 Jan 13;138(1):116-25. doi: 10.1021/jacs.5b06392. Epub 2015 Oct 22.
Low-temperature direct methane fuel cells (DMEFCs) offer the opportunity to substantially improve the efficiency of energy production from natural gas. This study focuses on the development of well-defined platinum organometallic complexes covalently anchored to ordered mesoporous carbon (OMC) for electrochemical oxidation of methane in a proton exchange membrane fuel cell at 80 °C. A maximum normalized power of 403 μW/mg Pt was obtained, which was 5 times higher than the power obtained from a modern commercial catalyst and 2 orders of magnitude greater than that from a Pt black catalyst. The observed differences in catalytic activities for oxidation of methane are linked to the chemistry of the tethered catalysts, determined by X-ray photoelectron spectroscopy. The chemistry/activity relationships demonstrate a tangible path for the design of electrocatalytic systems for C-H bond activation that afford superior performance in DMEFC for potential commercial applications.
低温直接甲烷燃料电池（DMEFC）为提高天然气能源生产效率提供了新的契机。本研究致力于开发结构明确的铂金属有机配合物，将其共价固定在有序介孔碳（OMC）上，在 80°C 的质子交换膜燃料电池中用于甲烷的电化学氧化。在 80°C 的条件下，获得了 403 μW/mgPt 的最大归一化功率，是现代商业催化剂获得功率的 5 倍，是 Pt 黑催化剂的 2 个数量级。甲烷氧化的催化活性差异与连接催化剂的化学性质有关，这可以通过 X 射线光电子能谱来确定。化学/活性关系为设计用于 C-H 键活化的电催化体系提供了明确的方向，在直接甲烷燃料电池中具有潜在的商业应用前景。
