Strong metal-support interaction promoted scalable production of thermally stable single-atom catalysts

Liu, Kaipeng; Zhao, Xupeng; Ren, Guoqing; Yang, Tao; Ren, Yujing; Lee, Adam F.; Su, Yang; Pan, Xiaoli; Zhang, Jingcai; Chen, Zhiqiang; Yang, Jingguo; Liu, Xiaoyan; Zhou, Tong; Xi, Wei; Luo, Jun; Zeng, Chaobin; Matsumoto, Hiroaki; Liu, Wei; Jiang, Qike; Wilson, Karen; Wang, Aiqin; Qiao, Botao; Li, Weizhen; Zhang, Tao

doi:10.1038/s41467-020-14984-9

Cited by 213 publications

(163 citation statements)

References 74 publications

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“…Thus, the strong interaction between Ru and Fe stabilizes the SACs and proves the stabilization effect of EMSI. [122] Furthermore, despite the typical support of metal oxides, graphene also has a strong interaction with single metal atoms. Yao et al synthesized the single Ni atoms anchored on defected graphene.…”

Section: Stabilization Effectmentioning

confidence: 99%

Electronic Metal–Support Interaction of Single‐Atom Catalysts and Applications in Electrocatalysis

et al. 2020

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between the electronic structure and catalytic efficiency of heterogenous catalysts. Dating back to 1930s, the concept of "electronic factor" was proposed by G. M. Schwab to describe the influence of electronic interaction on catalytic behavior of supported catalyst and divided the interaction into two parts, structural and synergetic ones. [4] Electrons transferring between the metal and the support was first under consideration when it came to the catalysis. After that, S. J. Tauster used the term of "strong metal-support interaction" (SMSI) to describe the chemisorption properties of group VIII elements supported by a metal oxide (e.g. SiO 2 , MgO) in 1978. [5] Later the concept was broadened to interaction between any metallic species and support, based on the experimental phenomena. [6] Till that time, based on the early characterization of surface science, researchers had realized that the active site might change during the process from metallic to an SMSI state, which was indicated to be covered or encapsulated by the support. [7] Among many hypotheses concerning the mechanism of SMSI, electron transfer between the metal and the support has been adapted by many researchers, and was confirmed by Rodriguez based on X-ray crystallography and UV photoemission spectroscopy in 1990s. [8] Then almost at the same time that the term of SACs was formally put forward, C. T. Campbell proposed the concept of "electronic metal-support interaction" (EMSI). As Campbell described, the chemical and catalytic properties might be affected by the electronic perturbations (i.e., shifts in the energy of d-band center) due to the EMSI. [9] In other words, the EMSI gave a much more detailed explanation of the enhanced properties of supported catalysts than SMSI, indicating that the study on catalysis was finally pushed to the electronic scale after so many years. [9b,c,10] Unfortunately, for metal particles or clusters, the accurate identification of electronic state is often difficult or even impossible. [11] The most reliable way to overcome the barrier above is to develop the catalyst based on single-atom metal that avoids intrinsic metal effects, including the electronic quantum size effect as well as structure-sensitivity geometrical effect. [12] Therefore, the rise of SACs provides a nearly perfect model to study the EMSI. As the supported metal species downsize to the single atom, the interaction between active site and support is always uniform, which can be much easier to be characterized by both experiment and theoretical calculation. [13] With the help of advanced techniques, for instance, X-ray absorption spectroscopy (XAS), the information about electronic The electronic metal-support interaction (EMSI), which acts as a bridge between theoretical electronic study and the design of heterogenous catalysts, has attracted much attention. Utilizing the interaction between the metal and the support is one of the most essential strategies to enhance electrocatalytic efficiency due to structural and synergetic promotion. To ...

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Section: Stabilization Effectmentioning

confidence: 99%

Electronic Metal–Support Interaction of Single‐Atom Catalysts and Applications in Electrocatalysis

et al. 2020

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“…Recent advances in synthetic strategies for SACs are generally dominated by wet-chemistry approaches including defect engineering, spatial confinement, and coordination design strategies 14 , 15 . Mechanochemistry scenarios, which have attracted more interest because of their quick, quantitative, and solvent-free properties compared with wet-chemistry approaches, however, have always been a great challenge for fabricating atomically dispersed metal sites 16 – 18 . In addition, the successful assembly of metal single atoms on conventional carriers often requires a very careful control of synthesis conditions, such as low temperature 19 , 20 , low metal loading 21 , 22 , grafting of N-rich organic linkers 23 , 24 , etc.…”

Section: Introductionmentioning

confidence: 99%

Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

et al. 2020

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Single-atom catalysts (SACs) have attracted considerable attention in the catalysis community. However, fabricating intrinsically stable SACs on traditional supports (N-doped carbon, metal oxides, etc.) remains a formidable challenge, especially under hightemperature conditions. Here, we report a novel entropy-driven strategy to stabilize Pd single-atom on the high-entropy fluorite oxides (CeZrHfTiLa)O x (HEFO) as the support by a combination of mechanical milling with calcination at 900°C. Characterization results reveal that single Pd atoms are incorporated into HEFO (Pd 1 @HEFO) sublattice by forming stable Pd-O-M bonds (M = Ce/Zr/La). Compared to the traditional support stabilized catalysts such as Pd@CeO 2 , Pd 1 @HEFO affords the improved reducibility of lattice oxygen and the existence of stable Pd-O-M species, thus exhibiting not only higher low-temperature CO oxidation activity but also outstanding resistance to thermal and hydrothermal degradation. This work therefore exemplifies the superiority of high-entropy materials for the preparation of SACs.

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“…This result keeps a good agreement with the temperature-programmed SXRD data. The in situ environmental TEM results evidence that the interaction between Ag NPs and O 2 is the driving force to enhance the mobility of Ag atoms 22 , which move from the NPs to the support and are finally hosted in the matrix 23 – 25 . As showed in Supplementary Fig.…”

Section: Resultsmentioning

confidence: 95%

“…During the redispersion process, a stronger adherence of Ag NP to α-MnO 2 was observed, leading to the collapse of the Ag NP. It looks like that the process is surface-mediated, in which atomic species after being emitted from a metal NP diffuse on the surface of the support until being trapped by a strong metal-support interaction 23 – 25 (Supplementary discussion).…”

Section: Resultsmentioning

confidence: 99%

Stable single atomic silver wires assembling into a circuitry-connectable nanoarray

et al. 2021

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Atomic metal wires have great promise for practical applications in devices due to their unique electronic properties. Unfortunately, such atomic wires are extremely unstable. Here we fabricate stable atomic silver wires (ASWs) with appreciably unoccupied states inside the parallel tunnels of α-MnO2 nanorods. These unoccupied Ag 4d orbitals strengthen the Ag–Ag bonds, greatly enhancing the stability of ASWs while the presence of delocalized 5s electrons makes the ASWs conducting. These stable ASWs form a coherently oriented three-dimensional wire array of over 10 nm in width and up to 1 μm in length allowing us to connect it to nano-electrodes. Current-voltage characteristics of ASWs show a temperature-dependent insulator-to-metal transition, suggesting that the atomic wires could be used as thermal electrical devices.

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Strong metal-support interaction promoted scalable production of thermally stable single-atom catalysts

Cited by 213 publications

References 74 publications

Electronic Metal–Support Interaction of Single‐Atom Catalysts and Applications in Electrocatalysis

Electronic Metal–Support Interaction of Single‐Atom Catalysts and Applications in Electrocatalysis

Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

Stable single atomic silver wires assembling into a circuitry-connectable nanoarray

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