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源自基于双氰胺的金属有机框架的Co O @Co/NCNT纳米结构作为氧还原和析氧反应的高效双功能电催化剂

Co O @Co/NCNT Nanostructure Derived from a Dicyanamide-Based Metal-Organic Framework as an Efficient Bi-functional Electrocatalyst for Oxygen Reduction and Evolution Reactions.

作者信息

Sikdar Nivedita, Konkena Bharathi, Masa Justus, Schuhmann Wolfgang, Maji Tapas Kumar

机构信息

Chemistry and Physics of Materials Unit (CPMU), Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR), Bangalore-, 560064, Karnataka, India.

Analytical Chemistry-Center for Electrochemical Sciences (CES), Ruhr-University Bochum, 44780, Bochum, Germany.

出版信息

Chemistry. 2017 Dec 19;23(71):18049-18056. doi: 10.1002/chem.201704211. Epub 2017 Nov 23.

DOI:10.1002/chem.201704211
PMID:28914980
Abstract

There has been growing interest in the synthesis of efficient reversible oxygen electrodes for both the oxygen reduction reaction (ORR) and the oxygen evolution reactions (OER), for their potential use in a variety of renewable energy technologies, such as regenerative fuel cells and metal-air batteries. Here, a bi-functional electrocatalyst, derived from a novel dicyanamide based nitrogen rich MOF {[Co(bpe) (N(CN) )]⋅(N(CN) )⋅(5 H O)} [Co-MOF-1, bpe=1,2-bis(4-pyridyl)ethane, N(CN) =dicyanamide] under different pyrolysis conditions is reported. Pyrolysis of the Co-MOF-1 under Ar atmosphere (at 800 °C) yielded a Co nanoparticle-embedded N-doped carbon nanotube matrix (Co/NCNT-Ar) while pyrolysis under a reductive H /Ar atmosphere (at 800 °C) and further mild calcination yielded Co O @Co core-shell nanoparticle-encapsulated N-doped carbon nanotubes (Co O @Co/NCNT). Both catalysts show bi-functional activity towards ORR and OER, however, the core-shell Co O @Co/NCNT nanostructure exhibited superior electrocatalytic activity for both the ORR with a potential of 0.88 V at a current density of -1 mA cm and the OER with a potential of 1.61 V at 10 mA cm , which is competitive with the most active bi-functional catalysts reported previously.

摘要

对于氧还原反应(ORR)和析氧反应(OER)的高效可逆氧电极的合成,人们的兴趣与日俱增,因为它们在各种可再生能源技术中具有潜在应用,例如再生燃料电池和金属空气电池。在此,报道了一种双功能电催化剂,它是由一种新型的基于双氰胺的富氮金属有机框架{[Co(bpe)(N(CN)₂)]⋅(N(CN)₂)⋅(5H₂O)} [Co-MOF-1,bpe = 1,2-双(4-吡啶基)乙烷,N(CN)₂ = 双氰胺]在不同热解条件下衍生而来。Co-MOF-1在Ar气氛(800°C)下热解得到Co纳米颗粒嵌入的N掺杂碳纳米管基质(Co/NCNT-Ar),而在还原性H₂/Ar气氛(800°C)下热解并进一步温和煅烧得到Co₃O₄@Co核壳纳米颗粒封装的N掺杂碳纳米管(Co₃O₄@Co/NCNT)。两种催化剂对ORR和OER均表现出双功能活性,然而,核壳结构的Co₃O₄@Co/NCNT纳米结构在电流密度为-1 mA cm⁻²时电位为0.88 V的ORR以及在10 mA cm⁻²时电位为1.61 V的OER方面均表现出优异的电催化活性,这与先前报道的最具活性的双功能催化剂具有竞争力。

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