In situ formation of mononuclear complexes by reaction-induced atomic dispersion of supported noble metal nanoparticles

Feng, Siquan; Song, Xinshan; Liu, Yang; Lin, Xiangsong; Li, Yan; Liu, Siyue; Dong, Wenrui; Yang, Xueming; Jiang, Zheng; Ding, Yunjie

doi:10.1038/s41467-019-12965-1

Cited by 69 publications

(50 citation statements)

References 50 publications

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“…Feng et al reported a general strategy to disperse active carbon-supported Rh nanoparticles into single-atom Rh catalyst [ 103 ]. Firstly, active carbon-supported RhCl 3 was thermally treated under nitrogen atmosphere at 300°C for 2 h. The residual was reduced with hydrogen at 300°C for 2 h to obtain the fresh 5 wt% Rh catalyst with Rh nanoparticle size of 4 nm (RhNP/AC).…”

Section: Synthetic Methods For Saecsmentioning

confidence: 99%

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

2020

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Oxygen reduction reaction (ORR) plays significant roles in electrochemical energy storage and conversion systems as well as clean synthesis of fine chemicals. However, the ORR process shows sluggish kinetics and requires platinum-group noble metal catalysts to accelerate the reaction. The high cost, rare reservation, and unsatisfied durability significantly impede large-scale commercialization of platinum-based catalysts. Single-atom electrocatalysts (SAECs) featuring with well-defined structure, high intrinsic activity, and maximum atom efficiency have emerged as a novel field in electrocatalytic science since it is promising to substitute expensive platinum-group noble metal catalysts. However, finely fabricating SAECs with uniform and highly dense active sites, fully maximizing the utilization efficiency of active sites, and maintaining the atomically isolated sites as single-atom centers under harsh electrocatalytic conditions remain urgent challenges. In this review, we summarized recent advances of SAECs in synthesis, characterization, oxygen reduction reaction (ORR) performance, and applications in ORR-related H2O2 production, metal-air batteries, and low-temperature fuel cells. Relevant progress on tailoring the coordination structure of isolated metal centers by doping other metals or ligands, enriching the concentration of single-atom sites by increasing metal loadings, and engineering the porosity and electronic structure of the support by optimizing the mass and electron transport are also reviewed. Moreover, general strategies to synthesize SAECs with high metal loadings on practical scale are highlighted, the deep learning algorithm for rational design of SAECs is introduced, and theoretical understanding of active-site structures of SAECs is discussed as well. Perspectives on future directions and remaining challenges of SAECs are presented.

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Section: Synthetic Methods For Saecsmentioning

confidence: 99%

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

2020

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“…The treatment of sintered Au catalyst with CH 3 I has been shown to be an effective method to restore the activity of an Au/C catalyst for acetylene hydrochlorination reactions [91]. Synergistic effects have been observed in the reactant-induced disintegration of metal nanoparticles [92]. After treating carbon-supported metal nanoparticles (e.g., Ru, Rh, Pd) with a CH 3 I/CO mixture, a volatile M(CO) x I y complex can be produced that can be captured and stabilized by the carbon support, resulting in the redispersion of metal nanoparticles into atomically dispersed species.…”

Section: Trends Trends In In Chemistry Chemistrymentioning

confidence: 99%

Evolution of Isolated Atoms and Clusters in Catalysis

Liu

Corma

2020

Trends in Chemistry

166

134

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Structural evolution of isolated metal atoms and metal clusters with low atomicity is commonly observed in both homogeneous and heterogeneous catalysis. This evolution is directly associated with the formation of the working active sites and deactivation mechanism of the catalyst.Understanding the evolutional behavior of subnanometric metal catalysts can help to stabilize the active sites under harsh reaction conditions. Regeneration of the deactivated metal catalyst also relies on atomic-level understanding of the dynamic structural transformation processes.

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“… 28 , 33 − 38 Atomic dispersion also has the potential to be applied to atomically dispersed materials as well as catalyst regeneration processes, and several examples have appeared. 23 − 25 , 29 − 31…”

Section: Introductionmentioning

confidence: 99%

Transformation of Bulk Pd to Pd Cations in Small-Pore CHA Zeolites Facilitated by NO

Yasumura

Ide

Ueda

et al. 2021

JACS Au

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Atomic dispersion of metal species has attracted attention as a unique phenomenon that affects adsorption properties and catalytic activities and that can be used to design so-called single atom materials. In this work, we describe atomic dispersion of bulk Pd into small pores of CHA zeolites. Under 4% NO flow at 600°C, bulk Pd metal on the outside of CHA zeolites effectively disperses, affording Pd 2+ cations on Al sites with concomitant formation of N 2 O, as revealed by microscopic and spectroscopic characterizations combined with mass spectroscopy. In the present method, even commercially available submicrosized Pd black can be used as a Pd source, and importantly, 4.1 wt % of atomic Pd 2+ cations, which is the highest loading amount reported so far, can be introduced into CHA zeolites. The structural evolution of bulk Pd metal is also investigated by in situ X-ray absorption spectroscopy (XAS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), as well as ab initio thermodynamic analysis using density functional theory (DFT) calculations.

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In situ formation of mononuclear complexes by reaction-induced atomic dispersion of supported noble metal nanoparticles

Cited by 69 publications

References 50 publications

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction

Evolution of Isolated Atoms and Clusters in Catalysis

Transformation of Bulk Pd to Pd Cations in Small-Pore CHA Zeolites Facilitated by NO

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