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Non-Calcined Layer-Pillared Mn0.5Zn0.5 Bimetallic–Organic Framework as a Promising Electrocatalyst for Oxygen Evolution Reaction
Inorganic Chemistry ( IF 4.6 ) Pub Date : 2022-06-14 , DOI: 10.1021/acs.inorgchem.2c00542 Reza Abazari 1 , Ali Reza Amani-Ghadim 2 , Alexandra M Z Slawin 3 , Cameron L Carpenter-Warren 3 , Alexander M Kirillov 4
Inorganic Chemistry ( IF 4.6 ) Pub Date : 2022-06-14 , DOI: 10.1021/acs.inorgchem.2c00542 Reza Abazari 1 , Ali Reza Amani-Ghadim 2 , Alexandra M Z Slawin 3 , Cameron L Carpenter-Warren 3 , Alexander M Kirillov 4
Affiliation
Electrocatalytic generation of oxygen is of great significance for sustainable, clean, and efficient energy production. Multiple electron transfer in oxygen evolution reaction (OER) and its slow kinetics represent a serious hedge for efficient water splitting, requiring the design and development of advanced electrocatalysts with porous structures, high surface areas, abundant electroactive sites, and low overpotentials. These requisites are common for metal–organic frameworks (MOFs) and derived materials that are promising electrocatalysts for OER. The present work reports on the synthesis and full characterization of a heteroleptic 3D MOF, [Zn2(μ4-odba)2(μ-bpdh)]n·nDMF (Zn-MUM-1), assembled from 4,4′-oxydibenzoic acid and 2,5-bis(4-pyridyl)-3,4-diaza-2,4-hexadiene (bpdh). Besides, a series of heterometallic MnZn-MUM-1 frameworks (abbreviated as Mn0.5Zn0.5-MUM-1, Mn0.66Zn0.33-MUM-1, and Mn0.33Zn0.66-MUM-1) was also prepared, characterized, and used for the fabrication of working electrodes based on Ni foam (NF), followed by their exploration in OER. These noble-metal-free and robust electrocatalysts are stable and do not require pyrolysis or calcination while exhibiting better electrocatalytic performance than the parent Zn-MUM-1/NF electrode. The experimental results show that the Mn0.5Zn0.5-MUM-1/NF electrocatalyst features the best OER activity with a low overpotential (253 mV at 10 mA cm–2) and Tafel slope (73 mV dec–1) as well as significant stability after 72 h or 6000 cycles. These excellent results are explained by a synergic effect of two different metals present in the Mn–Zn MOF as well as improved charge and ion transfer, conductivity, and stability characteristics. The present study thus widens the application of heterometallic MOFs as prospective and highly efficient electrocatalysts for OER.
中文翻译:
非煅烧层柱状 Mn0.5Zn0.5 双金属-有机骨架作为一种有前途的析氧反应电催化剂
电催化制氧对于可持续、清洁、高效的能源生产具有重要意义。析氧反应 (OER) 中的多电子转移及其缓慢的动力学是有效水分解的严重障碍,需要设计和开发具有多孔结构、高表面积、丰富的电活性位点和低过电位的先进电催化剂。这些必要条件对于金属有机框架 (MOF) 和衍生材料来说很常见,这些材料有望成为 OER 的电催化剂。目前的工作报告了杂配 3D MOF [Zn 2 (μ 4 -odba) 2 (μ-bpdh)] n · n的合成和全面表征DMF (Zn-MUM-1),由 4,4'-氧二苯甲酸和 2,5-双(4-吡啶基)-3,4-二氮杂-2,4-己二烯 (bpdh) 组装而成。此外,还制备、表征了一系列异金属 MnZn-MUM-1 骨架(缩写为 Mn 0.5 Zn 0.5 -MUM-1、Mn 0.66 Zn 0.33 -MUM-1 和 Mn 0.33 Zn 0.66 -MUM-1),并用于制造基于泡沫镍 (NF) 的工作电极,随后他们在 OER 中进行了探索。这些不含贵金属且坚固耐用的电催化剂非常稳定,不需要热解或煅烧,同时表现出比母体 Zn-MUM-1/NF 电极更好的电催化性能。实验结果表明,Mn 0.5 Zn 0.5-MUM-1/NF 电催化剂具有最佳的 OER 活性,过电位低(10 mA cm –2时为 253 mV )和 Tafel 斜率(73 mV dec –1),并且在 72 小时或 6000 次循环后具有显着的稳定性。这些优异的结果可以通过 Mn-Zn MOF 中存在的两种不同金属的协同作用以及改进的电荷和离子转移、电导率和稳定性特性来解释。因此,本研究拓宽了异金属 MOF 作为前瞻性和高效 OER 电催化剂的应用。
更新日期:2022-06-14
中文翻译:
非煅烧层柱状 Mn0.5Zn0.5 双金属-有机骨架作为一种有前途的析氧反应电催化剂
电催化制氧对于可持续、清洁、高效的能源生产具有重要意义。析氧反应 (OER) 中的多电子转移及其缓慢的动力学是有效水分解的严重障碍,需要设计和开发具有多孔结构、高表面积、丰富的电活性位点和低过电位的先进电催化剂。这些必要条件对于金属有机框架 (MOF) 和衍生材料来说很常见,这些材料有望成为 OER 的电催化剂。目前的工作报告了杂配 3D MOF [Zn 2 (μ 4 -odba) 2 (μ-bpdh)] n · n的合成和全面表征DMF (Zn-MUM-1),由 4,4'-氧二苯甲酸和 2,5-双(4-吡啶基)-3,4-二氮杂-2,4-己二烯 (bpdh) 组装而成。此外,还制备、表征了一系列异金属 MnZn-MUM-1 骨架(缩写为 Mn 0.5 Zn 0.5 -MUM-1、Mn 0.66 Zn 0.33 -MUM-1 和 Mn 0.33 Zn 0.66 -MUM-1),并用于制造基于泡沫镍 (NF) 的工作电极,随后他们在 OER 中进行了探索。这些不含贵金属且坚固耐用的电催化剂非常稳定,不需要热解或煅烧,同时表现出比母体 Zn-MUM-1/NF 电极更好的电催化性能。实验结果表明,Mn 0.5 Zn 0.5-MUM-1/NF 电催化剂具有最佳的 OER 活性,过电位低(10 mA cm –2时为 253 mV )和 Tafel 斜率(73 mV dec –1),并且在 72 小时或 6000 次循环后具有显着的稳定性。这些优异的结果可以通过 Mn-Zn MOF 中存在的两种不同金属的协同作用以及改进的电荷和离子转移、电导率和稳定性特性来解释。因此,本研究拓宽了异金属 MOF 作为前瞻性和高效 OER 电催化剂的应用。