Simple-Cubic Carbon Frameworks with Atomically Dispersed Iron Dopants toward High-Efficiency Oxygen Reduction

Wang, Biwei; Wang, Xinxia; Zou, Jialin; Yan, Yancui; Xie, Songhai; Hu, Guangzhi; Li, Yanguang; Dong, Angang

doi:10.1021/acs.nanolett.7b00004

Cited by 174 publications

(112 citation statements)

References 42 publications

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“…It is well known that cyanate and thiocyanate anions coordinate strongly to metals, and consequently can passivates active sites. Thus, it has been shown that the introduction of CN − ions on Fe 1 /N‐doped C or Co 1 /N‐doped C catalysts is detrimental to their performances in ORR, demonstrating the activity of these SAC ,. Theoretical calculations have confirmed that FeN 4 sites present in nitrogen‐doped carbon materials can act as very efficient catalytic sites for oxygen adsorption and O=O bond cleavage, with performances reaching the ones of platinum ,.…”

Section: Catalysis With Single Atom Catalysts On Carbon‐based Materialsmentioning

confidence: 97%

Single Atom Catalysts on Carbon‐Based Materials

2018

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Metal particle size is an important parameter to consider when looking at supported catalyst performances. As for other properties, surface reactivity of metallic nanoparticles is thus highly size‐dependent. The smallest size that can be reached for this type of object is of course the isolated atom deposited on a support. The preparation of single‐atom catalysts (SAC) is not trivial, since to avoid clustering, the mean adsorption energy of the metal on the support should be higher than its cohesive energy. The choice of a support that allows a strongly interacting environment with the metal is therefore a key step in the preparation of such catalysts. The spectrum of carbon (nano)materials is very broad, and their structure as well as their surface chemistry, although sometime complex, can be tuned and exploited for the stabilization of SAC. This Review summarizes in a comprehensive manner experimental and computational studies aiming at: i) preparing SAC on carbon materials, ii) understanding the metal‐support interactions in SAC, and iii) studying how this relates to catalytic performances. The use of SAC follows well the needs dictated by society (energy and environment issues), and many studies have already been published in various fields, such as thermal catalysis, photocatalysis and electrocatalysis.

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Section: Catalysis With Single Atom Catalysts On Carbon‐based Materialsmentioning

confidence: 97%

Single Atom Catalysts on Carbon‐Based Materials

2018

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“…Nowadays, one of the most promising candidates to replace PMs as ORR catalyst is single‐atom Fe embedded nitrogen‐doped carbon (Fe–N–C), where FeNx moieties formed by coordination of single‐atom Fe with nitrogen embedded in carbon matrix are regarded as active sites for ORR . However, due to the thermodynamical instability, single‐atom Fe is prone to migration and agglomeration into nanoparticles during pyrolysis, resulting in lower utilization of metal species, decrement of FeN x active site, and thereby poor catalyst performance .…”

Section: Introductionmentioning

confidence: 99%

ZIF‐8 with Ferrocene Encapsulated: A Promising Precursor to Single‐Atom Fe Embedded Nitrogen‐Doped Carbon as Highly Efficient Catalyst for Oxygen Electroreduction

Wang

Han

Wang

et al. 2018

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The oxygen reduction reaction (ORR) plays an important role in the fields of energy storage and conversion technologies, including metal-air batteries and fuel cells. The development of nonprecious metal electrocatalysts with both high ORR activity and durability to replace the currently used costly Pt-based catalyst is critical and still a major challenge. Herein, a facile and scalable method is reported to prepare ZIF-8 with single ferrocene molecules trapped within its cavities (Fc@ZIF-8), which is utilized as precursor to porous single-atom Fe embedded nitrogen-doped carbon (Fe-N-C) during high temperature pyrolysis. The catalyst shows a half-wave potential (E ) of 0.904 V, 67 mV higher than commercial Pt/C catalyst (0.837 V), which is among the best compared with reported results for ORR. Significant electrochemical properties are attributed to the special configuration of Fc@ZIF-8 transforming into a highly dispersed iron-nitrogen coordination moieties embedded carbon matrix.

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“…In order to increase the loading of single atoms, many research groups have improved the pyrolysis process by the substitution of precursors . For instance, atomically dispersed Fe‐N‐C was prepared by using the Fe‐decorated 3D simple‐cubic carbon frameworks as the precursor . As another example, the pyrolysis of Zn/Co bimetallic metal–organic frameworks (MOF) led to the formation of single‐atom Co‐N‐C species .…”

Section: Introductionmentioning

confidence: 99%

Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy

Lei

Liu

Yin

et al. 2020

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Increasing the mass loading of transition metal single atoms coordinated with nitrogen in carbon‐based materials (M‐N‐C) is still challenging. Herein, inspired by the bioconcentration effect in the living body, a biochemistry strategy for the synthesis of Fe‐N‐C single atoms is demonstrated. Through introducing ferrous glycinate into the growth of fungus, the Fe atoms are bioconcentrated in hyphae. The highly dispersed Fe‐N‐C single atoms in hyphae‐derived carbon fibers (labeled as Fe‐N‐C SA/HCF) are prepared by the pyrolysis of Fe‐riched hyphae. In the bioconcentration process, the uptake of Fe ions by hyphae promotes the secretion of glutathione and ferritin, which provides additional coordination sites for Fe ions. Accordingly, the mass content of Fe in bioconcentrated Fe‐N‐C SA/HCF reaches 4.8%, which is 5.3 times larger than that of the sample prepared by the conventional pyrolysis process. The present bioconcentration strategy is further extended to the preparation of Co, Ni, and Mn single atoms. Owing to the high content of Fe‐N‐C single atoms, Fe‐N‐C SA/HCF shows the onset potential (Eonset) of 0.931 V versus reversible hydrogen electrode (RHE) and half‐wave potential (E1/2) of 0.802 V versus RHE in oxygen reduction reaction measurements, which is comparable to the commercial Pt/C catalysts.

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Simple-Cubic Carbon Frameworks with Atomically Dispersed Iron Dopants toward High-Efficiency Oxygen Reduction

Cited by 174 publications

References 42 publications

Single Atom Catalysts on Carbon‐Based Materials

Single Atom Catalysts on Carbon‐Based Materials

ZIF‐8 with Ferrocene Encapsulated: A Promising Precursor to Single‐Atom Fe Embedded Nitrogen‐Doped Carbon as Highly Efficient Catalyst for Oxygen Electroreduction

Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy

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