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Electrical Stimulation of Catalytic Activity of Platinum Nanocoatings in CO oxidation
Russian Journal of Physical Chemistry B ( IF 1.4 ) Pub Date : 2020-07-31 , DOI: 10.1134/s1990793120030033
M. V. Grishin , A. K. Gatin , V. G. Slutskii , A. S. Fedotov , V. A. Kharitonov , B. R. Shub

Abstract—

An increase in the rate of catalytic CO oxidation for platinum nanocoatings was measured when the electrical stress of various polarity and value was applied to a coating from an external source. Under conditions of the experiment at 250°C, atmospheric pressure and the starting composition mixture of 4.8% CO + 10.2% O2 + Ar, applying the positive stress of +10 or +30 V on a coating leads to increase in the rate of CO oxidation by 18 or 54%, respectively. Applying the negative stress of –10 or –30 V leads to small acceleration in oxidation by 4 or 8%. It is shown that the effect of applied stress does not depend on particle size in a coating and grows linearly with stress. Quantum-chemical calculations of heats of association of CO and O2 with electrically neutral or electrically charged platinum cluster were performed. It was found that the creation of the positive charge on Pt2 leads to decrease in the heat of CO association by 6.4 kcal/mol and increase in the heat of O2 association by 4.7 kcal/mol, while the creation of the negative charge on Pt2 leads to a small effect of decrease in the heat of CO association by 3.0 kcal/mol and increase in the heat of O2 association by 4.2 kcal/mol. From the results, it is proposed to explain increase in the rate of catalytic CO oxidation on platinum electrically charged with the help of the external stress source.


中文翻译:

电刺激铂纳米涂层在CO氧化中的催化活性

摘要-

当从外部来源向涂层施加各种极性和值的电应力时,测量了铂纳米涂层的催化CO氧化速率的增加。在250°C,大气压和4.8%CO + 10.2%O 2 + Ar的起始成分混合物的实验条件下,在涂层上施加+10或+30 V的正应力会导致涂层速率的增加。 CO氧化分别增加18%或54%。施加–10或–30 V的负应力会导致4或8%的小氧化加速。结果表明,施加应力的效果不取决于涂层中的粒径,而是随应力线性增长。CO和O 2缔合热的量子化学计算用电中性或带电的铂簇进行。发现在Pt 2上产生正电荷会导致CO缔合热降低6.4 kcal / mol,而在O 2缔合热方面增加4.7 kcal / mol,而在Pt 2上产生负电荷Pt 2导致CO缔合热降低3.0 kcal / mol以及O 2缔合热增加4.2 kcal / mol的影响很小。从结果可以提出,借助于外部应力源可以解释带电的铂上的催化CO氧化速率的增加。
更新日期:2020-07-31
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