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Transition-Metal- and Nitrogen-Doped Carbide-Derived Carbon/Carbon Nanotube Composites as Cathode Catalysts for Anion-Exchange Membrane Fuel Cells
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-01-28 , DOI: 10.1021/acscatal.0c03511 Jaana Lilloja 1 , Elo Kibena-Põldsepp 1 , Ave Sarapuu 1 , John C Douglin 2 , Maike Käärik 1 , Jekaterina Kozlova 3 , Päärn Paiste 4, 5 , Arvo Kikas 3 , Jaan Aruväli 5 , Jaan Leis 1 , Väino Sammelselg 1, 3 , Dario R Dekel 2, 6 , Kaido Tammeveski 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-01-28 , DOI: 10.1021/acscatal.0c03511 Jaana Lilloja 1 , Elo Kibena-Põldsepp 1 , Ave Sarapuu 1 , John C Douglin 2 , Maike Käärik 1 , Jekaterina Kozlova 3 , Päärn Paiste 4, 5 , Arvo Kikas 3 , Jaan Aruväli 5 , Jaan Leis 1 , Väino Sammelselg 1, 3 , Dario R Dekel 2, 6 , Kaido Tammeveski 1
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Transition-metal- and nitrogen-codoped carbide-derived carbon/carbon nanotube composites (M-N-CDC/CNT) have been prepared, characterized, and used as cathode catalysts in anion-exchange membrane fuel cells (AEMFCs). As transition metals, cobalt, iron, and a combination of both have been investigated. Metal and nitrogen are doped through a simple high-temperature pyrolysis technique with 1,10-phenanthroline as the N precursor. The physicochemical characterization shows the success of metal and nitrogen doping as well as very similar morphologies and textural properties of all three composite materials. The initial assessment of the oxygen reduction reaction (ORR) activity, employing the rotating ring–disk electrode method, indicates that the M-N-CDC/CNT catalysts exhibit a very good electrocatalytic performance in alkaline media. We find that the formation of HO2– species in the ORR catalysts depends on the specific metal composition (Co, Fe, or CoFe). All three materials show excellent stability with a negligible decline in their performance after 10000 consecutive potential cycles. The very good performance of the M-N-CDC/CNT catalyst materials is attributed to the presence of M-Nx and pyridinic-N moieties as well as both micro- and mesoporous structures. Finally, the catalysts exhibit excellent performance in in situ tests in H2/O2 AEMFCs, with the CoFe-N-CDC/CNT reaching a current density close to 500 mA cm–2 at 0.75 V and a peak power density (Pmax) exceeding 1 W cm–2. Additional tests show that Pmax reaches 0.8 W cm–2 in an H2/CO2-free air system and that the CoFe-N-CDC/CNT material exhibits good stability under both AEMFC operating conditions.
中文翻译：
过渡金属和氮掺杂碳化物衍生的碳/碳纳米管复合材料作为阴离子交换膜燃料电池的阴极催化剂
过渡金属和氮共掺杂碳化物衍生的碳/碳纳米管复合材料（MN-CDC/CNT）已被制备、表征，并用作阴离子交换膜燃料电池（AEMFC）中的阴极催化剂。作为过渡金属，钴、铁以及两者的组合已被研究。以 1,10-菲咯啉作为氮前体，通过简单的高温热解技术掺杂金属和氮。物理化学表征显示了金属和氮掺杂的成功以及所有三种复合材料非常相似的形态和织构特性。采用旋转环盘电极法对氧还原反应（ORR）活性的初步评估表明，MN-CDC/CNT催化剂在碱性介质中表现出非常好的电催化性能。我们发现ORR催化剂中HO 2 -物质的形成取决于特定的金属成分（Co、Fe或CoFe）。所有三种材料均表现出出色的稳定性，在 10000 次连续电位循环后其性能下降可以忽略不计。 MN-CDC/CNT 催化剂材料的优异性能归因于 MN x和吡啶-N 部分以及微孔和介孔结构的存在。最后，催化剂在H 2 /O 2 AEMFCs的原位测试中表现出优异的性能，CoFe-N-CDC/CNT在0.75 V下达到接近500 mA cm –2的电流密度和峰值功率密度（ P max ) 超过 1 W cm –2 。附加测试表明P max达到 0。在不含 H 2 /CO 2的空气系统中，功率为 8 W cm –2 ，CoFe-N-CDC/CNT 材料在两种 AEMFC 操作条件下均表现出良好的稳定性。
更新日期：2021-02-19
中文翻译：
过渡金属和氮掺杂碳化物衍生的碳/碳纳米管复合材料作为阴离子交换膜燃料电池的阴极催化剂
过渡金属和氮共掺杂碳化物衍生的碳/碳纳米管复合材料（MN-CDC/CNT）已被制备、表征，并用作阴离子交换膜燃料电池（AEMFC）中的阴极催化剂。作为过渡金属，钴、铁以及两者的组合已被研究。以 1,10-菲咯啉作为氮前体，通过简单的高温热解技术掺杂金属和氮。物理化学表征显示了金属和氮掺杂的成功以及所有三种复合材料非常相似的形态和织构特性。采用旋转环盘电极法对氧还原反应（ORR）活性的初步评估表明，MN-CDC/CNT催化剂在碱性介质中表现出非常好的电催化性能。我们发现ORR催化剂中HO 2 -物质的形成取决于特定的金属成分（Co、Fe或CoFe）。所有三种材料均表现出出色的稳定性，在 10000 次连续电位循环后其性能下降可以忽略不计。 MN-CDC/CNT 催化剂材料的优异性能归因于 MN x和吡啶-N 部分以及微孔和介孔结构的存在。最后，催化剂在H 2 /O 2 AEMFCs的原位测试中表现出优异的性能，CoFe-N-CDC/CNT在0.75 V下达到接近500 mA cm –2的电流密度和峰值功率密度（ P max ) 超过 1 W cm –2 。附加测试表明P max达到 0。在不含 H 2 /CO 2的空气系统中，功率为 8 W cm –2 ，CoFe-N-CDC/CNT 材料在两种 AEMFC 操作条件下均表现出良好的稳定性。
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