Atomically dispersed Au1 catalyst towards efficient electrochemical synthesis of ammonia

Wang, Xiaoqian; Wang, Wenyu; Qiao, Man; Wu, Geng; Chen, Wenxing; Yuan, Tongwei; Xu, Qian; Chen, Min; Zhang, Yan; Wang, Jing; Ge, Jingjie; Hong, Xun; Li, Yafei; Wu, Yuen; Li, Yadong

doi:10.1016/j.scib.2018.07.005

Cited by 239 publications

(146 citation statements)

References 39 publications

Supporting

Mentioning

141

Contrasting

Order By: Relevance

“…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

View full text Add to dashboard Cite

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.

show abstract

Section: Introductionmentioning

confidence: 99%

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

et al. 2019

View full text Add to dashboard Cite

show abstract

“…Besides metal‐oxides, a variety of porous graphene‐like materials have been used as the substrates to anchor metal atoms/clusters for catalysis. For example, it has been experimentally demonstrated that single metal atoms (Pt, Pd, Ag, Ir, Au) embedded in g‐C 3 N 4 are highly active for the semihydrogenation of 1‐hexyne and electrochemical synthesis of ammonia, theoretical studies suggested that single transition metal atoms anchored on C 2 N could serve as low‐cost but highly efficient catalysts for oxygen evolution reaction, CO oxidation, nitrogen reduction reaction, HCOOH dehydrogenation, and CO 2 electrochemical reduction, and the noble metal atoms anchored on graphyne are very promising for low‐temperature CO oxidation …”

Section: Introductionmentioning

confidence: 99%

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

2019

View full text Add to dashboard Cite

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.

show abstract

“…[1,[4][5][6][7][8][9] To date, metal-based materials have been the most widelyi nvestigatede lectrocatalysts for the NRR, exhibiting acceptable NH 3 yields andf aradaic efficiencies (FEs) in aqueous electrolytes and significantly improved FEs in ionicliquid electrolytes. [10,11] Recently, severalg roupsu tilized different syntheticm ethodst of abricate noble-metal gold-based materials, such as atomically dispersed Au, [12] flower-like Au, [13] hollowA un anocages, [14] Au-containing alloys, [15] Au nanoparticles/C, [16] Au nanoclusters, [17] amorphous Au, [18] and Au nanorods with high-index faces; [19] these have been experimentally and theoretically provent ob ee lectrochemically active for the NRR. In their studies,t he size, structure, degree of crystallinity, and crystallinep lane of Au have an important influence on their NRR activity;h owever,t he influence of the substrate for loading Au on the resulting NRR has generallyb een ignored in the reported studies.I ti sk nown that the NH 3 yield from electrocatalytic N 2 fixationi na queous electrolyte by utilizing currentlyd eveloped NRR catalysts under ambient conditions is still low,f ar away from large-scale production applications.…”

Section: Introductionmentioning

confidence: 99%

Ambient Electrosynthesis of Ammonia on a Core–Shell‐Structured Au@CeO₂ Catalyst: Contribution of Oxygen Vacancies in CeO₂

Liu

Cui

Han

et al. 2019

Chemistry A European J

View full text Add to dashboard Cite

Electrosynthesis of NH3 through the N2 reduction reaction (NRR) under ambient conditions is regarded as promising technology to replace the industrial energy‐ and capital‐intensive Haber–Bosch process. Herein, a room‐temperature spontaneous redox approach to fabricate a core–shell‐structured Au@CeO2 composite, with Au nanoparticle sizes below about 10 nm and a loading amount of 3.6 wt %, is reported for the NRR. The results demonstrate that as‐synthesized Au@CeO2 possesses a surface area of 40.7 m2 g−1 and a porous structure. As an electrocatalyst, it exhibits high NRR activity, with an NH3 yield rate of 28.2 μg h−1 cm−2 (10.6 μg h−1 mg−1cat., 293.8 μg h−1 mg−1Au) and a faradaic efficiency of 9.50 % at −0.4 V versus a reversible hydrogen electrode in 0.01 m H2SO4 electrolyte. The characterization results reveal the presence of rich oxygen vacancies in the CeO2 nanoparticle shell of Au@CeO2; these are favorable for N2 adsorption and activation for the NRR. This has been further verified by theoretical calculations. The abundant oxygen vacancies in the CeO2 nanoparticle shell, combined with the Au nanoparticle core of Au@CeO2, are electrocatalytically active sites for the NRR, and thus, synergistically enhance the conversion of N2 into NH3.

show abstract

Atomically dispersed Au1 catalyst towards efficient electrochemical synthesis of ammonia

Cited by 239 publications

References 39 publications

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

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

Ambient Electrosynthesis of Ammonia on a Core–Shell‐Structured Au@CeO₂ Catalyst: Contribution of Oxygen Vacancies in CeO₂

Contact Info

Product

Resources

About

Atomically dispersed Au1 catalyst towards efficient electrochemical synthesis of ammonia

Cited by 239 publications

References 39 publications

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

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

Ambient Electrosynthesis of Ammonia on a Core–Shell‐Structured Au@CeO2 Catalyst: Contribution of Oxygen Vacancies in CeO2

Contact Info

Product

Resources

About

Ambient Electrosynthesis of Ammonia on a Core–Shell‐Structured Au@CeO₂ Catalyst: Contribution of Oxygen Vacancies in CeO₂