| Understanding enhancing mechanism of Pr6O11 and Pr(OH)3 in methanol electrooxidation |
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| 作者姓名： | Yang Yang Zhenyu Li Ying Yu Xueqiong Zhang Hang Wei Haibin Chu |
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| 作者单位： | Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules |
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| 基金项目： | Project supported by the National Natural Science Foundation of China(21875125,21801140,21561023);the Natural Science Foundation of Inner Mongolia Autonomous Region of China(2017JQ03,2018BS05013);Program of Higher-level Talents of Inner Mongolia University(21300-5165155,21300-5155104)。 |
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| 摘 要： | The presence of oxygen vacancies and hydroxyl groups are both favorable for the methanol electrooxidation on Pt-based catalysts.Understanding and differentiating the enhancing mechanism between oxygen vacancies and hydroxyl groups for high activity of Pt catalysts in methanol oxidation reaction(MOR)is essential but still challenging.Herein,we developed two kinds of co-catalyst for Pt/CNTs,Pr6O11is rich in oxygen vacancies but contains substantially no hydroxyl groups,while Pr(OH)3 possesses abundant hydroxyl groups without oxygen vacancies.After a seque nce of designed experiments,it can be found that both oxygen vacancies and hydroxyl groups can improve the performance of Pt/CNTs electrocatalysts,but the enhancing mechanism and improving degree of oxygen vacancies and hydroxyl groups for the MOR are different.Since the oxygen vacancies are more conducive to increasing the intrinsic activity of the Pt catalyst,and the hydroxyl groups play a decisive role in dehydrogenation and deproto nation of methanol,the co-catalysts with both oxygen vacancies and hydroxyl groups mixed with Pt/CNTs have higher catalytic performance.Therefore,hydroxyl-rich Pr6O11·xH2O was prepared and used as MOR electrocatalyst after mixed with Pt/CNTs.Benefiting from the synergistic effect of oxygen vacancies and hydroxyl groups,the Pr6O11·xH2O/Pt/CNTs shows a high peak current density of 741 mA/mg,which is three times higher than that of Pt/CNTs.These new discoveries serve as a promising strategy for the rational design of MOR catalysts with low cost and high activity.
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| 关 键 词： | Oxygen vacancies Hydroxyl groups Pr6O11 Pr(OH)3 Methanol oxidation reaction Rare earths |
| 收稿时间： | 6 July 2020 |
Understanding enhancing mechanism of Pr6O11 and Pr(OH)3 in methanol electrooxidation |
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| Yang Yang,Zhenyu Li,Ying Yu,Xueqiong Zhang,Hang Wei,Haibin Chu.Understanding enhancing mechanism of Pr6O11 and Pr(OH)3 in methanol electrooxidation[J].Journal of Rare Earths,2022,40(1):85-92. |
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| Affiliation: | Inner Mongolia Engineering and Technology Research Center for Catalytic Conversion and Utilization of Carbon Resource Molecules, College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021, China |
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| Abstract: | The presence of oxygen vacancies and hydroxyl groups are both favorable for the methanol electrooxidation on Pt-based catalysts. Understanding and differentiating the enhancing mechanism between oxygen vacancies and hydroxyl groups for high activity of Pt catalysts in methanol oxidation reaction (MOR) is essential but still challenging. Herein, we developed two kinds of co-catalyst for Pt/CNTs, Pr6O11 is rich in oxygen vacancies but contains substantially no hydroxyl groups, while Pr(OH)3 possesses abundant hydroxyl groups without oxygen vacancies. After a sequence of designed experiments, it can be found that both oxygen vacancies and hydroxyl groups can improve the performance of Pt/CNTs electrocatalysts, but the enhancing mechanism and improving degree of oxygen vacancies and hydroxyl groups for the MOR are different. Since the oxygen vacancies are more conducive to increasing the intrinsic activity of the Pt catalyst, and the hydroxyl groups play a decisive role in dehydrogenation and deprotonation of methanol, the co-catalysts with both oxygen vacancies and hydroxyl groups mixed with Pt/CNTs have higher catalytic performance. Therefore, hydroxyl-rich Pr6O11·xH2O was prepared and used as MOR electrocatalyst after mixed with Pt/CNTs. Benefiting from the synergistic effect of oxygen vacancies and hydroxyl groups, the Pr6O11·xH2O/Pt/CNTs shows a high peak current density of 741 mA/mg, which is three times higher than that of Pt/CNTs. These new discoveries serve as a promising strategy for the rational design of MOR catalysts with low cost and high activity. |
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| Keywords: | Oxygen vacancies Hydroxyl groups Methanol oxidation reaction Rare earths |
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