Conductive One-Dimensional Coordination Polymers with Tunable Selectivity for the Oxygen Reduction Reaction.
Conductive One-Dimensional Coordination Polymers with Tunable Selectivity for the Oxygen Reduction Reaction.
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DOI：
10.1021/acsami.1c16121
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发表时间：
2021-10
影响因子：
9.5
通讯作者：
Qian Zhao;Di Zhu;Xun Zhou;Sheng-Hua Li;Xu-Ran Sun;Jing Cui;Zhiwu Fan;M. Guo;Jin Zhao
中科院分区：
文献类型：
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作者：
Qian Zhao;Di Zhu;Xun Zhou;Sheng-Hua Li;Xu-Ran Sun;Jing Cui;Zhiwu Fan;M. Guo;Jin Zhao
近年来，非贵金属配合物导电材料作为氧还原反应（ORR）的电催化剂受到越来越多的关注。在此，我们报道了有效的ORR电催化剂含有M-S2 N2网站与可调的选择性的基础上简单的一维（1D）的配位聚合物（CP）。采用溶剂热法，以M（OAc）2和2，5-二氨基-1，4-苯二硫醇（DABDT）为原料，合成了1D CPs。由于其良好的电导率（10-6-10-2 S cm-1），1D CP可以在不添加碳材料的情况下以低催化量用作ORR催化剂。在碱性介质中，钴基CP呈现出有序的纳米片结构，Co-S2 N2位点暴露，并表现出显著的电催化氧化还原活性（Eonset = 0.93 V vs可逆氢电极（RHE），E1/2 = 0.82 V，n = 3.85，JL = 5.22 mA cm-2，Tafel斜率为63 mV dec-1）。然而，镍基CP有利于2 e-ORR过程，具有约87%的H2 O2选择性和0.78 V的Eonset。这项工作为基于导电非贵金属CP的ORR催化剂的构建提供了新的机会。
Conductive materials involving nonprecious metal coordination complexes as electrocatalysts for the oxygen reduction reaction (ORR) have received increasing attention in recent years. Herein, we reported efficient ORR electrocatalysts containing M-S2N2 sites with tunable selectivity based on simple one-dimensional (1D) coordination polymers (CPs). The 1D CPs were synthesized from M(OAc)2 and 2,5-diamino-1,4-benzenedithiol (DABDT) by a solvent thermal method. Due to their good electrical conductivities (10-6-10-2 S cm-1), the 1D CPs could be used as ORR catalysts in low catalytic amounts without the addition of carbon materials. Cobalt-based CPs showed a well-organized structure of nanosheets with Co-S2N2 sites exposed and exhibited remarkable electrocatalytic ORR activity (Eonset = 0.93 V vs reversible hydrogen electrode (RHE), E1/2 = 0.82 V, n = 3.85, JL = 5.22 mA cm-2, Tafel slope of 63 mV dec-1) in alkaline media. However, nickel-based CPs favored a 2e- ORR process with ∼87% H2O2 selectivity and an Eonset of 0.78 V. This work provides new opportunities for the construction of ORR catalysts based on conductive nonprecious metal CPs.