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采用密度泛函理论和平面波赝势方法对含天然杂质黄铁矿的电子结构和光学性质进行了计算,并讨论了二十种天然杂质:钴、镍、砷、硒、碲、铜、金、银、钼、锌、铊、锡、钌、钯、铂、汞、镉、铋、铅和锑,对黄铁矿催化活性的影响.结果表明在过渡金属杂质中,杂质能级主要由它们的d轨道产生,而在主族金属及非金属杂质中,杂质能级主要由它们的s或p轨道产生.含铜、钼、砷、金、银或镍的黄铁矿对氧的还原的电催化能力增强.除锌、钼、钌、砷、锑、硒和碲外,其余杂质能增强黄铁矿表面俘获电子的能力,使光生电子和空穴复合的概率减小.光学性质计算表明,除镉、汞、钌、硒、碲和锌杂质对吸收带边影响不大外,其余杂质使黄铁矿的吸收带边发生了红移,特别是含金和银杂质黄铁矿的吸收系数增加了两个数量级.
The electronic structures and optical properties of pyrite with natural impurities were calculated by density functional theory and plane-wave pseudopotential method. Twenty kinds of natural impurities were discussed: cobalt, nickel, arsenic, selenium, tellurium, copper, gold, The effects of silver, molybdenum, zinc, thallium, tin, ruthenium, palladium, platinum, mercury, cadmium, bismuth, lead and antimony on the catalytic activity of pyrite were studied.The results show that the impurity levels in transition metal impurities mainly consist of their d orbital, whereas in the main group metals and non-metallic impurities, the impurity levels are mainly generated by their s or p orbitals. Pyrite containing copper, molybdenum, arsenic, gold, silver or nickel Reduced oxygen to oxygen The other impurities can enhance the ability of capturing electrons on the surface of pyrite and reduce the recombination probability of photogenerated electron and hole.Experimental results of optical properties show that, Except cadmium, mercury, ruthenium, selenium, tellurium and zinc impurities have little effect on the absorption band edge, the remaining impurities red shift the absorption edge of pyrite, especially the absorption coefficient of gold and silver impurities pyrite Increased by two orders of magnitude.