Catalysis on singly dispersed bimetallic sites

Zhang, Shiran; Nguyễn, Luân; Liang, Jia; Shan, Junjun; Liu, Jingyue Jimmy; Frenkel, Anatoly I.; Patlolla, Anitha; Huang, Weixin; Li, Jun; Tao, Franklin Feng

doi:10.1038/ncomms8938

Cited by 262 publications

(230 citation statements)

References 37 publications

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“…After treatment with H 2 at 200 8 8Cf or 0.5 h (line b), the binding energy shifts to 306.9 eV,s uggesting am etallic or slightly negative charged Rh state,c ompared with previous reports. Similarly,adownshift of Rh 3d photoemission peaks after 200 8 8Cr eduction (line d) is observed, indicating that Rh single atoms are in am etallic state.T he result seems to be different from previous reports, where the supported single metal atoms (such as Au, [10b,20] Pt, [7c, 21] Rh, [22] and Pd [7a,23] )a re generally positively charged. Before 200 8 8Cr eduction, Rh 3+ (309.9 eV) and Rh + (308.0 eV) are both present in the catalyst (line c).…”

Section: Angewandte Chemiecontrasting

confidence: 86%

Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh₃)₃

et al. 2016

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Homogeneous catalysts generally possess superior catalytic performance compared to heterogeneous catalysts. However, the issue of catalyst separation and recycling severely limits their use in practical applications. Single-atom catalysts have the advantages of both homogeneous catalysts, such as "isolated sites", and heterogeneous catalysts, such as stability and reusability, and thus would be a promising alternative to traditional homogeneous catalysts. In the hydroformylation of olefins, single-atom Rh catalysts supported on ZnO nanowires demonstrate similar efficiency (TON≈40000) compared to that of homogeneous Wilkinson's catalyst (TON≈19000). HAADF-STEM and infrared CO chemisorption experiments identified isolated Rh atoms on the support. XPS and XANES spectra indicate that the electronic state of Rh is almost metallic. The catalysts are about one or two orders of magnitude more active than most reported heterogeneous catalysts and can be reused four times without an obvious decline in activity.

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Section: Angewandte Chemiecontrasting

confidence: 86%

Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh₃)₃

et al. 2016

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“…Remarkably, the mass activity of the ALD50Pt/NGNs catalyst was 7.8 times greater than the ALD100Pt/NGNs catalyst (2.12 A mg −1 ) and 37.4 times greater than the Pt/C catalyst (0.27 A mg −1 ). These findings suggest that the single Pt atoms and clusters can significantly increase the Pt utilization activity in comparison to their NP counterparts1832, with the additional benefit of decreasing the cost of the catalyst for the HER.…”

Section: Resultsmentioning

confidence: 85%

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

et al. 2016

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Platinum-based catalysts have been considered the most effective electrocatalysts for the hydrogen evolution reaction in water splitting. However, platinum utilization in these electrocatalysts is extremely low, as the active sites are only located on the surface of the catalyst particles. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their efficiency by utilizing nearly all platinum atoms. Here we report on a practical synthesis method to produce isolated single platinum atoms and clusters using the atomic layer deposition technique. The single platinum atom catalysts are investigated for the hydrogen evolution reaction, where they exhibit significantly enhanced catalytic activity (up to 37 times) and high stability in comparison with the state-of-the-art commercial platinum/carbon catalysts. The X-ray absorption fine structure and density functional theory analyses indicate that the partially unoccupied density of states of the platinum atoms' 5d orbitals on the nitrogen-doped graphene are responsible for the excellent performance. S ecuring renewable and reliable sources of clean energy is one of the world's foremost challenges. Addressing this challenge is not only critical for the global economy but will also aid in the mitigation of environmental and health hazards caused by fossil fuels 1 . Hydrogen is the cleanest fuel available and is believed to be one of the most promising energy sources of the twenty-first century 2,3 . However, the majority of the hydrogen produced today is derived from steam-reformed methane, which is sourced from fossil reserves and produces a substantial amount of CO 2 (ref. 4). The production of hydrogen from water electrolysis is a promising alternative to the current CO 2 -emitting fossil fuel-based energy systems 5,6 .Platinum (Pt)-based catalysts are generally considered to be the most effective electrocatalysts for the hydrogen evolution reaction (HER) 5,7 . Unfortunately, Pt is expensive and scarce, limiting the commercial potential for such catalysts. The development of active, stable and inexpensive electrocatalysts for water splitting is a key step in the realization of a hydrogen economy, which is based on the use of molecular hydrogen for energy storage.Significant effort has been devoted to the search of non-preciousmetal-based HER catalysts, including sulfide-based materials 8-11 , and C 3 N 4 (refs 12-14). Although these candidate materials show promising activities for the HER, the activities of these catalysts in their present form are insufficient for industrial applications 15 .To overcome the challenges associated with the Pt HER catalysts and to drive the cost of H 2 production from water electrolysis down, it is very important to markedly decrease the Pt loading and increase the Pt utilization efficiency. Currently, supported Pt nanoparticles (NPs) are typically used to promote Pt activity towards the HER. Unfortunately, the geometry of the NPs limit the majority of the Pt atoms to the particle core, deeming them ineffect...

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“…As is well known, the sizes of metal nanoparticles [1][2][3][4][5][6][7][8][9][10][11][12][13][14] and oxide substrates 6,[15][16][17] are important factors in determining the activity of catalysts. However, the high costs and the finite resources of these noble metals limited their future applications as catalysts in large-scale production.…”

Section: Introductionmentioning

confidence: 99%

Theoretical investigations of non-noble metal single-atom catalysis: Ni₁/FeO_x for CO oxidation

Liang

Yang

Wang

et al. 2016

Catal. Sci. Technol.

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Significant progress has recently been made in single-atom catalysis involving noble metals. We report here a theoretical investigation on the catalytic mechanism of CO oxidation on a non-noble metal single-atom catalyst (SAC) Ni1/FeOx using density functional theory (DFT). The calculation results show that this new SAC Ni1/FeOx has high catalytic activity at room temperature for CO oxidation. The CO adsorption strength is a key factor in determining the catalytic activity for CO oxidation. Comparing with noble-metal Pt1/FeOx and Ir1/FeOx catalysts, the catalytic activity for CO oxidation on Ni1/FeOx is found to be comparable with that on Pt1/FeOx, but is considerably higher than that on Ir1/FeOx. Our theoretical prediction of this new non-noble metal Ni1/FeOx catalyst with high catalytic activity for CO oxidation at room temperature may find practical applications. The theoretical investigation provides fundamental understanding on the catalytic mechanism of singly-dispersed surface atoms and helps to stimulate further experimental study on highly active non-noble metal singleatom catalysts.

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Catalysis on singly dispersed bimetallic sites

Cited by 262 publications

References 37 publications

Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh₃)₃

Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh₃)₃

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

Theoretical investigations of non-noble metal single-atom catalysis: Ni₁/FeO_x for CO oxidation

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Catalysis on singly dispersed bimetallic sites

Cited by 262 publications

References 37 publications

Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh3)3

Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh3)3

Platinum single-atom and cluster catalysis of the hydrogen evolution reaction

Theoretical investigations of non-noble metal single-atom catalysis: Ni1/FeOx for CO oxidation

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Product

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Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh₃)₃

Hydroformylation of Olefins by a Rhodium Single‐Atom Catalyst with Activity Comparable to RhCl(PPh₃)₃

Theoretical investigations of non-noble metal single-atom catalysis: Ni₁/FeO_x for CO oxidation