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一种基于三核钴的配位聚合物作为在中性 pH 条件下高效的氧气析出电催化剂。

A trinuclear cobalt-based coordination polymer as an efficient oxygen evolution electrocatalyst at neutral pH.

机构信息

Catalysis and Nanomaterials Lab 27, Department of Chemistry, Quaid-i-Azam University, Islamabad 45320, Pakistan.

Catalysis and Nanomaterials Lab 27, Department of Chemistry, Quaid-i-Azam University, Islamabad 45320, Pakistan.

出版信息

J Colloid Interface Sci. 2019 Jun 1;545:269-275. doi: 10.1016/j.jcis.2019.03.018. Epub 2019 Mar 8.

Abstract

The dearth of an efficient, robust, abundant and cost-effective water oxidation catalyst is debatably the major hurdle for the technological advancement of artificial photosynthesis devices. Herein, a three dimensional (3D) cobalt-based coordination polymer {[Co(pyz)(fa)(dmso)]·2HO}, (1) (pyz = pyrazine, fa = fumarate, dmso = dimethyl sulfoxide) has been synthesized and demonstrated to act as an efficient electrocatalyst towards water oxidation at neutral pH. Compound 1 displays a stair-like arrangement parallel to the b-axis, with the cobalt clusters arranged in a zigzag fashion, and contains small, honeycomb-like channels parallel to the c-axis. Compound 1 shows a remarkable activity for water oxidation and attains a current density of 1 mA.cm at low overpotential (η = 257 mV) with a Tafel slope value of 80.5 mV.dec. This high performance of 1 in catalysing the water oxidation reaction is attributed to its unique 3-D architecture. The results of electrochemical investigations, including long-term and controlled potential electrolysis, are anticipated to guide the forthcoming advancement in creating efficient, cheap and noble metal (Pt/Ru/Ir) free catalysts for the water oxidation reaction.

摘要

缺乏高效、稳定、丰富且经济实惠的水氧化催化剂,是人工光合作用器件技术进步的主要障碍。在此,我们合成了一种三维(3D)钴基配位聚合物{[Co(pyz)(fa)(dmso)]·2HO},(1)(pyz=吡嗪,fa=富马酸,dmso=二甲基亚砜),并证明其在中性 pH 条件下对水氧化具有高效的电催化作用。化合物 1 沿 b 轴呈现阶梯状排列,钴簇呈之字形排列,且含有沿 c 轴平行的小型、蜂窝状通道。化合物 1 在水氧化中表现出显著的活性,在低过电势(η=257 mV)下达到 1 mA.cm 的电流密度,塔菲尔斜率值为 80.5 mV.dec。1 在催化水氧化反应中具有如此高的性能,归因于其独特的 3-D 结构。电化学研究的结果,包括长期和恒电位电解,有望为开发高效、廉价且无贵金属(Pt/Ru/Ir)的水氧化反应催化剂提供指导。

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