Chemistry Department, The City College and the Graduate School of the City University of New York, 160 Convent Avenue, New York, NY 10031, USA.
Chemphyschem. 2010 Dec 3;11(17):3678-84. doi: 10.1002/cphc.201000689.
Composites of a copper-based metal-organic framework (MOF) and graphite oxide (GO) were tested for hydrogen sulfide removal at ambient conditions. In order to understand the mechanisms of adsorption, the initial and exhausted samples were analyzed by various techniques including X-ray diffraction, Fourier transform infrared spectroscopy, thermogravimetric analyses, and sorption of nitrogen. Compared to the parent materials, an enhancement in hydrogen sulfide adsorption was found. It was the result of physical adsorption of water and H(2)S in the pore space formed at the interface between the MOF units and the graphene layers where the dispersive forces are the strongest. Besides physisorption, reactive adsorption was found as the main mechanism of retention. H(2)S molecules bind to the copper centers of the MOF. They progressively react with the MOF units resulting in the formation of copper sulfide. This leads to the collapse of the MOF structure. Water enhances adsorption in the composites as it allows the dissolution of hydrogen sulfide.
采用铜基金属-有机骨架（MOF）和氧化石墨（GO）复合材料，在常温常压下进行硫化氢去除测试。为了理解吸附机理，通过 X 射线衍射、傅里叶变换红外光谱、热重分析和氮气吸附等多种技术对初始和耗尽的样品进行了分析。与母体材料相比，发现复合材料对硫化氢的吸附增强。这是由于 MOF 单元和石墨烯层之间界面处形成的孔隙空间中物理吸附的水和 H(2)S 所致，在该界面处，分散力最强。除了物理吸附外，还发现反应性吸附是主要的保留机制。H(2)S 分子与 MOF 的铜中心结合。它们与 MOF 单元逐步反应，导致形成硫化铜。这导致 MOF 结构的坍塌。由于水允许硫化氢溶解，因此它增强了复合材料中的吸附。
