基于Pt(100)的双金属催化剂在碱性环境中电催化硝酸根还原为氮气的研究

硝酸盐在水体环境中含量的持续增加严重影响了人类的健康，因此开发一种有效可行的“绿色”硝酸盐治理方案已迫在眉睫。根据硝酸根在金属表面的电催化还原路径，发展基于Pt(100)晶面的双金属催化体系有望实现硝酸根还原过程中速控步骤和选择性还原的有效结合，得到环境友好型产物--氮气。. 为此，本项目利用传统的电化学测试技术和第一性原理计算相结合的方法来研究碱性环境中硝酸根和中间产物亚硝酸根在金属表面的吸附和电催化活性，为双金属催化体系中修饰金属的选择提供理论依据。同时，研究修饰金属在Pt(100)界面上的覆盖方式和覆盖率以及溶液pH值对修饰电极电催化性能的影响，阐明硝酸根向氮气选择性转化的反应条件和路径。通过理论研究，构建具有高选择性催化性能的Pt(100)基双金属纳米催化体系来实现废水中硝酸盐治理的广泛应用。

The constantly-rising contamination of nitrate in water caused a potential health threatening consequences for human. Therefore, creating a reliable “green” approach that can achieve the denitrification efficiently is a matter of great urgency. According to the pathways of nitrate reduction electrocatalyzed by noble or tansition metals, the rate-determining step and selectivity-determing step of nitrate reduction should be promoted simultaneously on bimetallic catalysts based on Pt(100), obtaining environment-friendly nitrogen as the fianl product. . Accordingly, in this project we plan to study the adsorption and electrocatalytic activities of nitrate and nitrite (the intermediate of rate-determining step) on various metals in alkaline media using the method combined electrochemical techniques and first principle caculations, which can provide the theoretical basis for the modified metal selection. At the same time, the effect of depositon method, metal coverage and solution pH on nitrate reduction will be explored, indicating the reaction conditions and pathways for the selective conversion to dinitrogen. The research goal of this project is construction of bimetallic (nano)catalysts based on Pt(100) sites to achieve the extensive application in nitrate remediation.