Definitive Structural Identification toward Molecule-Type Sites within 1D and 2D Carbon-Based Catalysts

Jiang Hongliang; He Qun; Wang Changda; Liu Hengjie; Zhang Youkui; Lin Yunxiang; Zheng Xusheng; Chen Shuangming; Ajayan Pulickel M.; Song Li

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Definitive Structural Identification toward Molecule-Type Sites within 1D and 2D Carbon-Based Catalysts

机译：对一维和二维碳基催化剂中分子型位点的确定结构鉴定

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Developing facile preparation routes and atomic-level characterization methods for single-atom catalysts is highly desirable but still challenging. Herein, a general strategy is proposed to construct transition metal single atoms within 1D and 2D carbon supports. The carbon supports, typically graphene and carbon nanotubes, are coated with various transition metal-containing bimetal hydroxides, followed by polydopamine coating and high-temperature pyrolysis. X-ray absorption fine structure spectroscopy measurements and simulations efficiently indicate that single atoms (Co, Fe, or Cu) are captured within the applied carbon supports, distinctively forming exclusive molecule-type sites. As a proof-of-concept application, the obtained catalysts exhibit remarkable performance for electrochemical oxygen reduction reaction, even surpassing commercial Pt/C catalyst. The developed versatile route opens up new avenues for the design of carbon-based catalysts with definite molecular active sites. The atomic-level structural identifications provide significant guidance for mechanistic studies toward single-atom catalysts.

机译：为单原子催化剂开发简便的制备路线和原子级表征方法是非常可取的，但仍具有挑战性。在本文中，提出了在1D和2D碳载体中构造过渡金属单原子的一般策略。碳载体（通常为石墨烯和碳纳米管）涂有各种含过渡金属的双金属氢氧化物，然后进行聚多巴胺涂层和高温热解。 X射线吸收精细结构光谱测量和模拟有效地表明，单个原子（Co，Fe或Cu）被捕获在所施加的碳载体中，从而明显地形成了排他的分子类型位点。作为概念验证的应用，所获得的催化剂在电化学氧还原反应方面表现出卓越的性能，甚至超过了商用Pt / C催化剂。发达的通用路线为具有明确分子活性位点的碳基催化剂的设计开辟了新途径。原子级的结构鉴定为单原子催化剂的机理研究提供了重要的指导。

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来源
《Advanced energy materials》 |2018年第19期|1800436.1-1800436.6|共6页
作者
Jiang Hongliang; He Qun; Wang Changda; Liu Hengjie; Zhang Youkui; Lin Yunxiang; Zheng Xusheng; Chen Shuangming; Ajayan Pulickel M.; Song Li;
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作者单位

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

Rice Univ, Dept Sci & Technol China, Houston, TX 77005 USA;

Univ Sci & Technol China, Natl Synchrotron Radiat Lab, CAS Ctr Excellence Nanosci, Hefei 230029, Anhui, Peoples R China;

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正文语种 eng
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关键词
carbon supports; electrocatalysts; oxygen reduction reaction; single atoms; X-ray absorption spectroscopy;

机译：碳载体;电催化剂;氧还原反应;单原子;X射线吸收光谱;

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Definitive Structural Identification toward Molecule-Type Sites within 1D and 2D Carbon-Based Catalysts

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