Electrocatalytic hydrogen evolution at carbon paste electrodes doped with a manganese(II) imidazoledicarboxylate complex

Zhengwei Wu, Tiantian Wan, Xiaoxia Kong, Qinqin Shen, Kaiyi Li, Huilu Wu
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Abstract

Abstract A mononuclear Mn(II) complex [Mn( p -MOPhH 2 IDC) 2 (H 2 O) 2 ]·2(DMF), was synthesized by the reaction of p -MOPhH 3 IDC (2-(4-methoxyphenyl)-1 H -imidazole-4,5-dicarboxylic acid) and Mn(CH 3 COO) 2 ·4H 2 O under solvothermal conditions and characterized by single-crystal X-ray diffraction, elemental analysis, IR and UV–vis spectroscopy. The structure analysis revealed that the manganese(II) center has a six-coordinated octahedral coordination geometry. The performance of a Mn(II) complex-doped carbon paste electrode (Mn-CPE) in the electrocatalytic hydrogen evolution reaction (HER) was evaluated by linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) methods. The polarization curve shows that the η 10 298K (overpotential, 10 mA cm −2 ) of the Mn-CPE was positively shifted by 341 mV compared with the bare CPE (without complex). The Tafel slope of the Mn-CPE was 161 mV dec −1 . These data indicate that the Mn-CPE was effective in the HER electrocatalytic reaction. For EIS experiments, the arc diameter of the high-frequency region of the Mn-CPE was much smaller than that of the bare CPE, which further indicates the effective catalytic capacity of the Mn(II) complex for hydrogen evolution. The information obtained from this study will help to expand the application of Mn(II) complexes in the field of electrochemistry.
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掺杂锰(II)咪唑二羧酸盐配合物的碳糊电极电催化析氢
摘要在溶剂热条件下,以p - mophh 3 IDC(2-(4-甲氧基苯基)-1 H -咪唑-4,5-二羧酸)和Mn(ch3 COO) 2·4H 2 O为原料合成了单核Mn(II)配合物[Mn(p - mophh 2 IDC) 2(H 2o) 2]·2(DMF),并用单晶x射线衍射、元素分析、红外光谱和紫外可见光谱对其进行了表征。结构分析表明,锰(II)中心具有六配位八面体配位几何。采用线性扫描伏安法(LSV)和电化学阻抗谱法(EIS)评价了Mn(II)配合物掺杂碳浆电极(Mn- cpe)在电催化析氢反应(HER)中的性能。极化曲线表明,Mn-CPE的η值为10 298K(过电位,10 mA cm−2),与裸CPE相比,正位移了341 mV。Mn-CPE的Tafel斜率为161 mV dec−1。这些数据表明Mn-CPE在HER电催化反应中是有效的。在EIS实验中,Mn-CPE的高频区弧径远小于裸CPE,进一步说明了Mn(II)配合物对析氢的有效催化能力。本研究获得的信息将有助于扩大锰(II)配合物在电化学领域的应用。
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