In Situ Thermal Atomization To Convert Supported Nickel Nanoparticles into Surface‐Bound Nickel Single‐Atom Catalysts

Yang, Jian; Qiu, Zongyang; Zhao, Changming; Wei, Weichen; Chen, Wenxing; Li, Zhijun; Qu, Yunteng; Dong, Juncai; Luo, Jun; Li, Zhenyu; Wu, Yuen

doi:10.1002/anie.201808049

Cited by 336 publications

(226 citation statements)

References 49 publications

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“…The strong coordination effects divided Ni atoms from Ni nanoparticles when exposed to carbon. The single Ni species were continuously lost from the Ni nanoparticles would eventually lead to the atomization of Ni nanoparticles, which is good for improving the atom utilization …”

Section: Defects‐based Single Atomic Electrocatalystmentioning

confidence: 99%

Defect‐Based Single‐Atom Electrocatalysts

et al. 2018

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Single‐atom catalysts (SACs) have attracted great attention owing to their maximum atomic utilization and high catalytic performance in electrochemical reactions. But the synthesis of SACs is not easy due to large surface energies of single atomic metal sites which often lead to their aggregation. The defects on supports can serve as anchor sites to stabilize single metal atoms and prevent them from aggregation, which has become an effective method to fabricate SACs. This review summarizes the meaningful findings about the defects on supports stabilizing single metal atoms, and their applications in electrocatalytic reaction. Various defects, including the intrinsic defects or heteroatom doping of carbon‐based materials, cation or anion vacancies of metal compound supports, and other defects (step edges, lattice defects, and caves), are comprehensively summarized, and the effects of defects on designing SACs are discussed. Although there are still many challenges to fully explore the SACs, it is believed that the newly established defect sites stabilized single atoms mechanism will be helpful for designing and fabricating highly powerful single atomic electrocatalysts for practical applications.

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Section: Defects‐based Single Atomic Electrocatalystmentioning

confidence: 99%

Defect‐Based Single‐Atom Electrocatalysts

et al. 2018

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“…Therefore, it is critical and desirable to search for durable, active, and inexpensive catalysts. Several strategies, such as reducing the precious metal loading, developing single‐atom catalysts and nonprecious metal catalysts, and fabricating metal‐free catalysts have been exploited. Among these strategies, metal‐free catalysts with controllable compositions are quite attractive because of their low‐cost, high stability, and high efficiency …”

Section: Introductionmentioning

confidence: 99%

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

et al. 2019

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Nitrogen‐doped graphdiynes recently emerged as promising metal‐free oxygen reduction reaction (ORR) electrocatalysts. However, which type of N‐dopants contributing to the enhanced catalytic performance and the catalytic performances of other heteroatom‐doped graphdiynes has not been explored systematically. Herein, ORR and oxygen evolution reaction (OER) catalytic performances of X‐doped graphdiynes are examined by means of DFT computations (X = B, N, P, and S). It is revealed that the graphitic S‐doped graphdiyne (Model S1), the sp‐N‐doped graphdiyne (Model N3) and the graphitic P‐doped graphdiyne (Model P1) exhibit comparable or even better ORR/OER activities than Pt/C or RuO2, with ORR activity trend as Model S1 > Pt/C > Model N3 and OER trend as Model P1 > RuO2 > Model N3. The carbon atoms near N‐ and S‐dopants and featuring large positive charge are the ORR active sites in Models N3 and S1, whereas the carbon atoms near N‐ and P‐dopants and possessing high spin are the OER active sites in Models N3 and P1. Overall, this study not only gains deep insights into the catalytic activity of N‐doped graphdiyne for ORR, but also guides developing of graphdiyne‐based ORR/OER catalysts beyond N‐doping.

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“…Since the first SAC, single Pt atoms on FeO x , was reported in 2011, various SACs with metal oxide supports have been successfully fabricated, such as single Au/Pt/Ir/Ni/Os atoms on FeO x , Co 3 O 4 , CeO 2 , Al 2 O 3 , and MgO surfaces. At the same time, the SACs could be accessed by thermal atomization of supported metal nanoparticles and direct atoms emitting from bulk metals . These experimental explorations also inspired many theoretical efforts.…”

Section: Introductionmentioning

confidence: 99%

1 + 1′ > 2: Heteronuclear Biatom Catalyst Outperforms Its Homonuclear Counterparts for CO Oxidation

2019

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By means of density functional theory (DFT) computations, the CO/O2 adsorption and CO oxidation pathways on the biatom catalyst, namely the heteronuclear Fe1Cu1@C2N, in comparison with its homonuclear counterparts Fe2@C2N and Cu2@C2N are systemically investigated. The reactions of O2 dissociation and CO oxidization with preadsorbed CO or O2 are comparably studied. The computations find that the heteronuclear species Fe1Cu1@C2N possesses high stabilities and is feasible to be synthesized experimentally. More importantly, the heteronuclear Fe1Cu1@C2N catalyst has even better catalytic activity toward CO oxidation than its homonuclear counterparts, especially, without suffering the CO‐poisoning problem. Considering the myriad of unexplored heteronuclear dimers that can be potentially anchored at appropriate supports, this work opens a new avenue and provides a useful guideline for further developing bimetal‐based nanocatalysts.

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In Situ Thermal Atomization To Convert Supported Nickel Nanoparticles into Surface‐Bound Nickel Single‐Atom Catalysts

Cited by 336 publications

References 49 publications

Defect‐Based Single‐Atom Electrocatalysts

Defect‐Based Single‐Atom Electrocatalysts

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

1 + 1′ > 2: Heteronuclear Biatom Catalyst Outperforms Its Homonuclear Counterparts for CO Oxidation

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