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制备具有优异氧还原反应活性的过渡金属单原子锚定碳的通用方法

Universal Method to Fabricate Transition Metal Single-Atom-Anchored Carbon with Excellent Oxygen Reduction Reaction Activity.

作者信息

Yu Lin-Qian, Xia Wen-Jing, Ma Wen-Jie, Wen Te-Er, Chen Shu-La, Jin Feng, Huang Bao-Cheng, Jin Ren-Cun

机构信息

Laboratory of Water Pollution Remediation, School of Life and Environmental Sciences, Hangzhou Normal University, Hangzhou 311121, China.

出版信息

ACS Appl Mater Interfaces. 2021 Mar 24;13(11):13534-13540. doi: 10.1021/acsami.0c21641. Epub 2021 Mar 11.

DOI:10.1021/acsami.0c21641
PMID:33705092
Abstract

Single-atom catalysts (SACs) have attracted great attention due to their high atom-utilization and catalytic efficiency. However, a universal synthetic route is still lacking, which restricts the SAC-related investigation and application. Here, we report a simple and cost-effective method to fabricate transition metal SACs through ion exchange and annealing procedures. Benefiting from the "egg-box" structure property of alginate, the metal ion can be effectively anchored into the organic center. Using CuCl as a representative transition metal ion, the Cu SAC structure was synthesized and identified by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy. Through optimizing CuCl concentration, the obtained Cu SAC exhibited a good oxygen reduction reaction activity, whose onset potential, half wave potential, and limiting current density are all comparable to those of 20 wt % Pt/C. Cu-N was identified as the responsible catalytic site. More importantly, other transition metal SACs can be easily synthesized altering metallic solution, which proves the universality of our proposed method. This work may be valuable for the cost-effective and universal SAC synthetic method development.

摘要

单原子催化剂(SACs)因其高原子利用率和催化效率而备受关注。然而,目前仍缺乏通用的合成路线,这限制了与SAC相关的研究和应用。在此,我们报道了一种通过离子交换和退火程序制备过渡金属SACs的简单且经济高效的方法。受益于藻酸盐的“蛋盒”结构特性,金属离子可有效锚定在有机中心。以CuCl作为代表性过渡金属离子,合成了Cu SAC结构,并通过像差校正高角度环形暗场扫描透射电子显微镜和X射线吸收精细结构光谱进行了鉴定。通过优化CuCl浓度,所获得的Cu SAC表现出良好的氧还原反应活性,其起始电位、半波电位和极限电流密度均与20 wt% Pt/C相当。Cu-N被确定为活性催化位点。更重要的是,通过改变金属溶液可以轻松合成其他过渡金属SACs,这证明了我们所提出方法的通用性。这项工作对于开发具有成本效益的通用SAC合成方法可能具有重要价值。

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引用本文的文献

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Chemical Kinetics of Metal Single Atom and Nanocluster Formation on Surfaces: An Example of Pt on Hexagonal Boron Nitride.表面上金属单原子和纳米团簇形成的化学动力学:以六方氮化硼上的铂为例。
Nano Lett. 2023 Sep 13;23(17):8006-8012. doi: 10.1021/acs.nanolett.3c01968. Epub 2023 Aug 18.
2
Electrochemical Crosslinking of Alginate-Towards Doped Carbons for Oxygen Reduction.用于氧还原的藻酸盐掺杂碳的电化学交联
Polymers (Basel). 2023 Jul 26;15(15):3169. doi: 10.3390/polym15153169.
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A minireview on the synthesis of single atom catalysts.
关于单原子催化剂合成的一篇综述短文。
RSC Adv. 2022 Mar 24;12(15):9373-9394. doi: 10.1039/d2ra00657j. eCollection 2022 Mar 21.