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Activated ZrC Promotes the Methanol Electro‐oxidation Activity and Enhances Poison Tolerance of Pt Nanoparticles in Acidic Medium
ChemistrySelect ( IF 1.9 ) Pub Date : 2020-06-26 , DOI: 10.1002/slct.202001581 Malaya K. Sahoo 1 , Ramasamy Shanmugam 1 , Ediga Umeshbabu 1 , G. Ranga Rao 1
ChemistrySelect ( IF 1.9 ) Pub Date : 2020-06-26 , DOI: 10.1002/slct.202001581 Malaya K. Sahoo 1 , Ramasamy Shanmugam 1 , Ediga Umeshbabu 1 , G. Ranga Rao 1
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Metal carbides which mimic Pt metal are good promoters for electrocatalytic reactions. Here we report the promoting activity of activated ZrC (a ‐ZrC) towards methanol electrooxidation reaction. The a ‐ZrC samples are prepared from commercial ZrC by chemical activation at two different temperatures (600 and 800 °C) using Na2CO3 as an activating reagent. The BET surface area of the commercial ZrC sample is 1 m2 g−1 which has been increased to 82 m2 g−1 and 134 m2 g−1 by chemical activation at 600 and 800 °C, respectively. In order to study the promoting activity of the activated ZrC samples in direct methanol fuel cell (DMFC), a ‐ZrC supported Pt/Vulcan carbon (XC) is synthesized through conventional polyol reflux method. The electrocatalytic activities of Pt/a ‐ZrC800‐XC, Pt/a ‐ZrC600‐XC, Pt/ZrC‐XC and Pt/XC electrocatalysts have been studied towards methanol electrooxidation reaction in an acidic media. The triple interface between Pt, activated ZrC and Vulcan carbon (Vulcan XC‐72R) reduces the adsorption energies, facilitating fast transport and short diffusion paths for electroactive species, which makes the Pt/a ‐ZrC800‐XC catalyst promising for DMFC applications. The decrease in adsorption energies is confirmed by the first principle calculations which show that the relative energy values of methanol adsorption, conversion of methanol to CO and further to CO2 on Pt/ZrC‐XC are much more negative than Pt/XC and bare Pt, indicating the thermodynamic feasibility of the reaction. The electrochemical analysis shows that, Pt/a ‐ZrC800‐XC electrocatalyst provides higher mass activity, higher antipoisioning activity, and required stability towards methanol electrooxidation reaction.
中文翻译：
活化的ZrC促进了甲醇在酸性介质中的电氧化活性并增强了Pt纳米颗粒的抗毒性
模仿Pt金属的金属碳化物是电催化反应的良好促进剂。在这里，我们报告活化的ZrC（a - ZrC ）对甲醇电氧化反应的促进活性。在一个-ZrC样品从商业的ZrC通过化学活化使用Na制备在两个不同温度（600和800℃）2 CO 3作为活化试剂。商业ZrC样品的BET表面积为1 m 2 g -1，已增加到82 m 2 g -1和134 m 2 g -1分别在600和800°C下进行化学活化。为了研究活化的ZrC样品在直接甲醇燃料电池（DMFC）中的促进活性，通过常规的多元醇回流法合成了‐ZrC负载的Pt / Vulcan碳（XC）。PT的电催化活性/一个-ZrC 800 -XC，铂/一个-ZrC 600 -XC，铂/的ZrC-XC和Pt / XC电催化剂进行了研究，对在酸性介质甲醇电氧化反应。Pt，活性ZrC和Vulcan碳（Vulcan XC-72R）之间的三重界面降低了吸附能，促进了电活性物质的快速运输和短扩散路径，这使得Pt / a- ZrC 800‐XC催化剂有望用于DMFC应用。吸附能的降低已通过第一原理计算得到证实，第一原理计算表明，Pt / ZrC-XC上甲醇吸附，甲醇转化为CO以及进一步转化为CO 2的相对能值比Pt / XC和裸露的Pt负得多。 ，表明该反应的热力学可行性。电化学分析表明，Pt / a- ZrC 800- XC电催化剂可提供更高的质量活性，更高的反渗透活性以及对甲醇电氧化反应所需的稳定性。
更新日期：2020-06-26
中文翻译：
活化的ZrC促进了甲醇在酸性介质中的电氧化活性并增强了Pt纳米颗粒的抗毒性
模仿Pt金属的金属碳化物是电催化反应的良好促进剂。在这里，我们报告活化的ZrC（a - ZrC ）对甲醇电氧化反应的促进活性。在一个-ZrC样品从商业的ZrC通过化学活化使用Na制备在两个不同温度（600和800℃）2 CO 3作为活化试剂。商业ZrC样品的BET表面积为1 m 2 g -1，已增加到82 m 2 g -1和134 m 2 g -1分别在600和800°C下进行化学活化。为了研究活化的ZrC样品在直接甲醇燃料电池（DMFC）中的促进活性，通过常规的多元醇回流法合成了‐ZrC负载的Pt / Vulcan碳（XC）。PT的电催化活性/一个-ZrC 800 -XC，铂/一个-ZrC 600 -XC，铂/的ZrC-XC和Pt / XC电催化剂进行了研究，对在酸性介质甲醇电氧化反应。Pt，活性ZrC和Vulcan碳（Vulcan XC-72R）之间的三重界面降低了吸附能，促进了电活性物质的快速运输和短扩散路径，这使得Pt / a- ZrC 800‐XC催化剂有望用于DMFC应用。吸附能的降低已通过第一原理计算得到证实，第一原理计算表明，Pt / ZrC-XC上甲醇吸附，甲醇转化为CO以及进一步转化为CO 2的相对能值比Pt / XC和裸露的Pt负得多。 ，表明该反应的热力学可行性。电化学分析表明，Pt / a- ZrC 800- XC电催化剂可提供更高的质量活性，更高的反渗透活性以及对甲醇电氧化反应所需的稳定性。
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