Pristine S,N-containing Mn-based metal organic framework nanorods enable efficient oxygen reduction electrocatalysis,Dalton Transactions

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Pristine S,N-containing Mn-based metal organic framework nanorods enable efficient oxygen reduction electrocatalysis
Dalton Transactions ( IF 3.5 ) Pub Date : 2020/02/25 , DOI: 10.1039/c9dt04852a
Shujun Chao _{1,

2,

3,

4,

5} , Qingyun Xia _{1,

2,

3,

4,

5} , Yingling Wang _{1,

2,

3,

4,

5} , Wenge Li _{3,

4,

5,

6} , Wenge Chen _{3,

4,

5,

6}

Affiliation

Owing to their unique physicochemical properties, metal–organic frameworks (MOFs) are a kind of promising material for electrocatalysis. However, many reports focus on the use of MOFs as precursors to produce efficient electrocatalysts by pyrolysis. The use of pristine MOFs with well-defined structures as efficient electrocatalysts directly is still a challenging problem. Herein, S,N-containing Mn^II[(Tdc)(4,4′-Bpy)]_n with different morphologies have been obtained by using Mn^II, thiophene-2,5-dicarboxylate (Tdc) and 4,4′-bipyridine (4,4′-Bpy) as raw materials via hydrothermal synthesis. Furthermore, the influences of different hydrothermal reaction times (0, 2 and 4 h) and anions (SO₄²⁻, Cl⁻, NO₃⁻ and CH₃COO⁻) on the morphologies, compositions and ORR activity of the resultant Mn-MOFs are also investigated at length. The results indicate that only the reaction of MnSO₄ with Tdc and 4,4′-Bpy for 4 h can form relatively uniform one-dimensional (1D) MOF nanorods. The 1D nanorods combine the favorable features towards the oxygen reduction reaction (ORR), such as a high surface area and efficient 1D electron/mass transport capability. Therefore, the Mn^II[(Tdc)(4,4′-Bpy)]_n nanorods display the highest ORR activity with an onset potential of 0.98 V and a half-wave potential of 0.78 V vs. RHE (reversible hydrogen electrode), which is even comparable to that of Pt/C. In addition, the Mn^II[(Tdc)(4,4′-Bpy)]_n nanorods exhibit higher stability, methanol resistance and ORR selectivity than Pt/C. The present study illustrates an efficient fabrication strategy for highly efficient 1D MOF nanorods for energy storage and conversion applications.

中文翻译：

原始的S，N含Mn基金属有机骨架纳米棒可实现高效的氧还原电催化

由于其独特的理化特性，金属有机骨架（MOF）是一种有前途的电催化材料。然而，许多报道集中于使用MOF作为前体通过热解产生有效的电催化剂。直接使用结构明确的原始MOF作为有效的电催化剂仍然是一个难题。在此，通过使用Mn ^II，噻吩-2,5-二羧酸（Tdc）和4,4'-获得了具有不同形态的含S，N的Mn ^II [（Tdc）（4,4'-Bpy）] _n联吡啶（4,4'-BPY）为原料通过水热合成。此外，水热反应时间（0、2和4 h）和阴离子（SO ₄^2-，Cl^-，NO₃^-和CH₃ COO^-）上的形态，组合物和所得到的锰的MOFs的ORR活性的也研究在长度。结果表明，只有MnSO₄与Tdc和4,4'-Bpy反应4 h才能形成相对均匀的一维（1D）MOF纳米棒。一维纳米棒结合了氧还原反应（ORR）的有利功能，例如高表面积和高效的一维电子/质量传输能力。因此，Mn^II [（Tdc）（4,4'-Bpy）]_n纳米棒显示最高的ORR活性，起始电势为0.98 V，半波电势为0.78 V vs.RHE（可逆氢电极），甚至与Pt / C相当。此外，Mn ^II [（Tdc）（4,4'-Bpy）] _n纳米棒比Pt / C具有更高的稳定性，耐甲醇性和ORR选择性。本研究说明了用于能量存储和转换应用的高效一维MOF纳米棒的有效制造策略。

更新日期：2020-04-08

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