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Influence of electrode assembly on catalytic activation and deactivation of a Pt film immobilized H+ conducting solid electrolyte in electrocatalytic reduction reactions

机译:电极组件对固定化Pt膜的H +导电固体电解质在电催化还原反应中的催化活化和失活的影响

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Symmetric (Cu-Pt vertical bar Nafion vertical bar Pt-Cu) and asymmetric (Pt vertical bar Nafion vertical bar Pt-Cu) assemblies were fabricated to study the nitrate reduction processes at the cathode. The electrocatalytic nitrate reduction reactions were performed in these assemblies in order to investigate the prerequisite for the enhanced catalytic activity, electrochemical cell durability as well as preferable product selectivity resulting from the reduction of nitrate at the cathode. It has been observed for the symmetric assembly that Cu particles were oxidized on the anode surface under an applied potential and the resulting copper ions migrated to the cathode surface through the Nafion membrane, which deposited as copper oxide on the cathode surface. The formation of this copper oxide covering layer on the Pt-Cu cathode surface is attributed as the reason for the deactivation of the cathode that governed the reduced nitrate reduction along with increasing nitrite selectivity. These problems were addressed and resolved with the asymmetric design of the electrocatalytic reactor, where enhanced hydrogen evolution activates the surface by eroding the CuO over layer as well as speeding up the slow rate determining hydrogenation reactions.
机译:制造对称(Cu-Pt垂直棒Nafion垂直棒Pt-Cu)和非对称(Pt垂直棒Nafion垂直棒Pt-Cu)组件以研究阴极处的硝酸盐还原过程。在这些组件中进行电催化硝酸盐还原反应,以研究提高催化活性,电化学电池的耐久性以及阴极还原硝酸盐所产生的优选产品选择性的前提条件。对于对称组件,已经观察到,在施加的电势下,Cu颗粒在阳极表面上被氧化,并且所得的铜离子通过Nafion膜迁移至阴极表面,该Nafion膜以氧化铜的形式沉积在阴极表面上。在Pt-Cu阴极表面上形成该氧化铜覆盖层的原因是阴极失活的原因,该失活决定了硝酸盐还原的减少以及亚硝酸盐选择性的增加。这些问题已通过电催化反应器的非对称设计得到解决并得以解决,在电催化反应器中,增强的析氢作用通过腐蚀覆盖层上的CuO并加快确定氢化反应的慢速速率来活化表面。

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