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DEMS study of hydrogen evolution reaction at Ni/reduced graphene oxides/Mo2C composites
Electrochimica Acta ( IF 5.5 ) Pub Date : 2025-01-26 , DOI: 10.1016/j.electacta.2025.145748
Sthephanie J. Martínez, Yapci Remedios-Díaz, Stefan Delgado, José Luis Rodríguez, Elena Pastor
Electrochimica Acta ( IF 5.5 ) Pub Date : 2025-01-26 , DOI: 10.1016/j.electacta.2025.145748
Sthephanie J. Martínez, Yapci Remedios-Díaz, Stefan Delgado, José Luis Rodríguez, Elena Pastor
In the present paper, Ni nanoparticles on graphene-based materials (Ni-GMs) and Mo2C composites (Ni-Mo2C) were tested as electrocatalysts towards the hydrogen evolution reaction (HER) using differential electrochemical mass spectrometry (DEMS) in alkaline medium. Precise determination of the Tafel slope and rate-determining step (RDS), along with the reaction mechanism, was achieved. The findings show that Ni deposition and the addition of Mo2C particles significantly enhance the catalytic activity, leading to low overpotentials towards the HER. Among the tested composites, Ni/rGO/Mo2C demonstrated the best onset potential (-54 mVRHE), followed by Ni/N-rGO/Mo2C (-63 mVRHE) and Ni/SNrGO/Mo2C (-100 mVRHE), with ionic current measurements (m/z = 2) confirming a Volmer-Heyrovsky pathway as the RDS. The addition of Mo2C, while not altering the reaction mechanism, significantly enhanced onset potentials and kinetics, with Tafel slopes for Ni-GMs ranging from 54 to 70 mV·dec−1, underscoring improved HER efficiency. Furthermore, the stability of these composites, particularly Ni/N-rGO/Mo2C, was tested overextended HER operation, showing sustained current densities and reduced degradation. Electrochemical impedance spectroscopy (EIS) revealed that Ni/N-rGO/Mo2C exhibited the lowest charge-transfer resistance, facilitating efficient electron transfer, which likely contributes to its superior durability. The incorporation of heteroatoms such as N and S further enhanced performance by preventing the adverse conductivity effects associated with Mo2C, thereby maintaining high catalytic activity. Collectively, these results indicate that Ni-Mo2C composites could be considered as promising catalysts to be used as cathodes in electrolysers.
中文翻译:
Ni/还原氧化石墨烯/Mo2C复合材料析氢反应的DEMS研究
在本文中,使用差分电化学质谱 (DEMS) 在碱性介质中测试石墨烯基材料 (Ni-GMs) 和 Mo2C 复合材料 (Ni-Mo2C) 上的 Ni 纳米颗粒作为电催化剂进行析氢反应 (HER)。实现了 Tafel 斜率和速率确定步骤 (RDS) 以及反应机制的精确测定。研究结果表明,Ni 沉积和 Mo2C 颗粒的添加显着增强了催化活性,导致对 HER 的过电位较低。在测试的复合材料中,Ni/rGO/Mo2C 表现出最佳的起始电位 (-54 mVRHE),其次是 Ni/N-rGO/Mo2C (-63 mVRHE) 和 Ni/SNrGO/Mo2C (-100 mVRHE),离子电流测量 (m/z = 2) 证实 Volmer-Heyrovsky 途径为 RDS。Mo2C 的添加在不改变反应机理的情况下,显著提高了起始电位和动力学,Ni-GM 的塔菲尔斜率范围为 54 至 70 mV·dec−1,强调了 HER 效率的提高。此外,这些复合材料的稳定性,特别是 Ni/N-rGO/Mo2C,在超长 HER 操作下进行了测试,显示出持续的电流密度和减少的降解。电化学阻抗谱 (EIS) 显示 Ni/N-rGO/Mo2C 表现出最低的电荷转移电阻,有利于高效的电子转移,这可能有助于其卓越的耐久性。 N 和 S 等杂原子的掺入通过防止与 Mo2C 相关的不良导电效应,从而进一步提高性能,从而保持高催化活性。总的来说,这些结果表明 Ni-Mo2C 复合材料可以被认为是有前途的催化剂,可用作电解槽中的阴极。
更新日期:2025-01-30
中文翻译:
Ni/还原氧化石墨烯/Mo2C复合材料析氢反应的DEMS研究
在本文中,使用差分电化学质谱 (DEMS) 在碱性介质中测试石墨烯基材料 (Ni-GMs) 和 Mo2C 复合材料 (Ni-Mo2C) 上的 Ni 纳米颗粒作为电催化剂进行析氢反应 (HER)。实现了 Tafel 斜率和速率确定步骤 (RDS) 以及反应机制的精确测定。研究结果表明,Ni 沉积和 Mo2C 颗粒的添加显着增强了催化活性,导致对 HER 的过电位较低。在测试的复合材料中,Ni/rGO/Mo2C 表现出最佳的起始电位 (-54 mVRHE),其次是 Ni/N-rGO/Mo2C (-63 mVRHE) 和 Ni/SNrGO/Mo2C (-100 mVRHE),离子电流测量 (m/z = 2) 证实 Volmer-Heyrovsky 途径为 RDS。Mo2C 的添加在不改变反应机理的情况下,显著提高了起始电位和动力学,Ni-GM 的塔菲尔斜率范围为 54 至 70 mV·dec−1,强调了 HER 效率的提高。此外,这些复合材料的稳定性,特别是 Ni/N-rGO/Mo2C,在超长 HER 操作下进行了测试,显示出持续的电流密度和减少的降解。电化学阻抗谱 (EIS) 显示 Ni/N-rGO/Mo2C 表现出最低的电荷转移电阻,有利于高效的电子转移,这可能有助于其卓越的耐久性。 N 和 S 等杂原子的掺入通过防止与 Mo2C 相关的不良导电效应,从而进一步提高性能,从而保持高催化活性。总的来说,这些结果表明 Ni-Mo2C 复合材料可以被认为是有前途的催化剂,可用作电解槽中的阴极。