采用热解法制备了硫、氮共掺杂铜单原子催化阴极。以Ti/IrO₂-RuO₂为阳极、Cu-CNS@NF和NF电极为阴极,考察了阴极材质对生成无机氯副产物的影响。在相同实验条件下,Cu-CNS@NF阴极体系中氯酸盐的生成速率仅为NF的79%。通过分槽分步还原实验、·H淬灭实验结合XPS、XAS、电化学行为等表征发现,阴极通过还原中间产物 \mathrm{C} \mathrm{l} {\mathrm{O}}_2^{-}和ClO^-间接减少了氯酸盐的生成,这可能是电解稀氯溶液过程中阴极抑制氯酸盐副产物生成的机理。Cu-CNS@NF阴极经S、N掺杂具有更多的活性位点,降低电荷转移电阻,吸附·H能力更强,促进中间产物的还原,从而表现出更优异的抑制效果。进一步研究了电流密度、初始Cl^-浓度、初始pH对氯酸盐生成的影响。

Cu-CNS@NF,an atomically dispersed Cu atoms on S-N co-doped carbon cathode,is prepared via pyrolysis method.The influences of cathode material on the formation of inorganic chlorates byproducts are evaluated through using Ti/IrO₂-RuO₂ as the anode,with Cu-CNS@NF and NF electrodes respectively as the cathode.Under identical experimental conditions,the formation rate of chlorates in the Cu-CNS@NF cathode system is only 79% that in the NF cathode system.Characterization techniques including separate compartment stepwise reduction experiment,·H quenching experiment,XPS,XAS,and electrochemical behavior are utilized to understand the mechanism behind the cathodic suppression of chlorates byproducts during electrolysis of dilute chloride solution.It is found that the cathode indirectly reduces the formation of chlorates by reducing intermediate products such as \mathrm{C} \mathrm{l} {\mathrm{O}}_2^{-} and ClO^-,potentially contributing to the inhibition mechanism of chlorates byproduct formation during the electrolysis process.Cu-CNS@NF cathode doped with sulfur and nitrogen exhibits more active sites,reduces charge transfer resistance,enhances ·H adsorption capacity,and facilitates the reduction of intermediate products,leading to superior suppression effect.Further study is also carried out to analyze the influences of current density,initial Cl^- concentration,and initial pH on chlorates formation.