In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation

Hülsey, Max J.; Zhang, Bin; Ma, Zhirui; Asakura, Hiroyuki; Adekoya, David; Chen, Wei; Tanaka, Tsunehiro; Zhang, Peng; Wu, Zili; Yan, Ning

doi:10.1038/s41467-019-09188-9

Cited by 208 publications

(204 citation statements)

References 71 publications

(55 reference statements)

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“…In addition to CeO2, other transition metal oxides like TiO2 [69], MnO2 [99,100], Co3O4 [101], and heteropoly acid [102] have also been regarded as promising supporting materials for SACs for CO oxidation by SACs. Since single atoms are highly mobile and tend to form aggregates during synthesis and catalysis, gentle routes allowing stabilization of single atomic metal sites have been considered, including defect engineering strategy on the surface of support materials developed by our group (Fig.…”

Section: Catalytic Oxidation Of Comentioning

confidence: 99%

“…PGMs-based SACs showed high activities towards CO elimination at low-temperature since Pt-SACs could form a distinctive interface with the support (i.e. reduction of Ce ions at Pt-CeO2 interface in Pt1/CeO2) and proceed according to MvK mechanism [21,50,51,56,86,93,95,98,102,106,107]. Although Al2O3 is non-reducible and inert, Al2O3 supported PGM-based SACs catalysts are also attractive because Al2O3 could be used as common support material in composite TWCs and DOCs to expand the surface area.…”

Section: Catalytic Oxidation Of Comentioning

confidence: 99%

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Single-atom site catalysts for environmental catalysis

et al. 2020

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In recent decades, the environmental protection and long-term sustainability have become the focus of attention due to the increasing pollution generated by the intense industrialization. To overcome these issues, environmental catalysis has increasingly been used to solve the negative impact of pollutants emission on the global environment and human health. Supported platinum-metal-group (PGM) materials are commonly utilized as the state-of-the-art catalysts to eliminate gaseous pollutants but large quantities of PGMs are required. By comparison, single-atom site catalysts (SACs) have attracted much attention in catalysis owing to their 100% atom efficiency and unique catalytic performances towards various reactions. Over the past decade, we have witnessed burgeoning interests of SACs in heterogeneous catalysis. However, to the best of our knowledge, the systematic summary and analysis of SACs in catalytic elimination of environmental pollutants has not yet been reported. In this paper, we summarize and discuss the environmental catalysis applications of SACs. Particular focus was paid to automotive and stationary emission control, including model reaction (CO oxidation, NO reduction and hydrocarbon oxidation), overall reaction (three-way catalytic and diesel oxidation reaction), elimination of volatile organic compounds (formaldehyde, benzene, and toluene), and removal/decomposition of other pollutants (Hg 0 and SO 3). Perspectives related to further challenges, directions and design strategies of single-atom site catalysts in environmental catalysis were also provided.

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Section: Catalytic Oxidation Of Comentioning

confidence: 99%

Section: Catalytic Oxidation Of Comentioning

confidence: 99%

Single-atom site catalysts for environmental catalysis

et al. 2020

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“…Compared with other methods (such as Hatree‐Fock method), the most important advantage of DFT is that it considers the electronic correlation. It also has high computational efficiency and can determine the relative reliability of the calculated simulation results . DFT calculation in nonprecious metal single‐atom catalysis is mainly divided into three aspects: simulating the catalytic mechanism, calculating the catalytic activity, and designing the optimal catalyst.…”

Section: Theoretical Calculations For Nonprecious Metal Single Atomicmentioning

confidence: 99%

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

et al. 2019

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Nonprecious metal single‐atom materials have attracted extensive attention in the field of electrocatalysis due to their low cost, high reactivity, high selectivity, and high atomic utilization. However, the high surface energy of a single atom causes agglomeration during preparation and catalytic measurement, resulting in damage to the catalytic sites. The strong interaction between substrate and monoatoms is the key factor to prevent the aggregation of individual metal atoms, and the geometry and electronic structure of the catalysts can be adjusted to optimize the catalytic activity. Due to the hierarchically pores, high specific surface area, and defect effect, nitrogen‐doped porous carbon (NPC) has been widely studied as an ideal nonprecious metal single‐atom support, which synergistically enhance the electrocatalytic performance toward oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction with non‐noble metal single atoms. This review summarizes the controllable synthesis, characterization, theoretical calculation, and application of M (M = Co, Fe, Ni, Cu, Zn, Mo, etc.) single atoms on nitrogen‐doped porous carbon. Finally, the future development and challenges of nitrogen‐doped porous carbon supported nonprecious metal single‐atom electrocatalysts for practical commercialization are concluded.

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“…Charge and spin can be carefully tuned in surface-confined metal-organic networks, at least in UHV, and we tackle here the issue whether this fundamental bottom-up approach can be extended beyond the surface science UHV environmental constraints. Recently, the reactivity of tetrapyrrole monolayers at surfaces has been investigated in situ at the solid/liquid interface under electrochemical conditions, mainly by STM methods [20,[132][133][134][135][136][137][138][139][140][141][142]. Very recently, instead, surface science spectroscopic approaches combining SFG and NAP-XPS methods allowed extension of the investigations of the ligand-macrocycle interaction up to the mbar pressure regime at room temperature, thus close to applicative relevant conditions [14,37,99,105,108].…”

Section: A Fundamental Approach Beyond Uhvmentioning

confidence: 99%

Tetrapyrroles at near-ambient pressure: porphyrins and phthalocyanines beyond the pressure gap

Vesselli

2020

J. Phys. Mater.

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Many complex mechanisms underlying the fascinating functionalities provided by tetrapyrrolic macrocycles in biochemistry have been already unraveled. Light harvesting, molecular transport, and catalytic conversion are some of the processes performed by tetrapyrrole-based centers embedded in protein pockets. The main function is determined by the single atom species that is caged in the macrocycle, while a finer tuning (band gap, chemical selectivity etc) is granted by the geometric and electronic structure of the tetrapyrrole, including its residues, and by the proximal and distal structures of the protein surroundings that exploit the molecular trans-effect and direct weak interactions, respectively. Hence, a scientific and technological challenge consists in the artificial replication of both structure and functionality of natural reaction centers in 2D ordered arrays at surfaces. Nano-architected 2D metalorganic frameworks can be indeed self-assembled under controlled conditions at supporting surfaces and, in the specific, porphyrin-and phthalocyaninebased systems have been widely investigated in ultra-high vacuum conditions by means of surface science approaches. Deep insight into the geometry, electronic structure, magnetic properties, ligand adsorption mechanisms, and light absorption has been obtained, with the strong experimental constraint of vacuum. Especially in the case of the interaction of tetrapyrroles with ligands, this limit represents a relevant gap with respect to both comparison with natural counterparts from the liquid environment and potential applicative views at both solid-liquid and solid-gas interfaces. Thus, a step forward in the direction of near-ambient pressure is strongly necessary, while maintaining the atomiclevel detail characterization accuracy. Nowadays this becomes feasible by exploiting state-of-the-art experimental techniques, in combination with computational simulations. This review focusses on the latest advances in this direction.

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In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation

Cited by 208 publications

References 71 publications

Single-atom site catalysts for environmental catalysis

Single-atom site catalysts for environmental catalysis

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

Tetrapyrroles at near-ambient pressure: porphyrins and phthalocyanines beyond the pressure gap

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