CO‐Tolerant PEMFC Anodes Enabled by Synergistic Catalysis between Iridium Single‐Atom Sites and Nanoparticles

Yang, Xiaolong; Wang, Ying; Xian, Wang; Mei, Bingbao; Luo, Ergui; Yang, Li; Meng, Qinglei; Zhao, Jianmin; Jiang, Zheng; Liu, Changpeng; Ge, Junjie; Wang, Xing

doi:10.1002/ange.202110900

Cited by 9 publications

(4 citation statements)

References 45 publications

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“…The cooperativity between Ir NPs and Ir SAs conferred the catalyst with superior H 2 oxidation activity (1.19 W cm −2 ) and excellent CO electro-oxidation activity (85 mW cm −2 ) in PEMFCs. [13] In SA-CoCu@Cu/CoNP-mediated ORR reaction, the interaction between Co-N 4 site and nearby Cu-N x site/CuCo-NP increased the ORR activity both towards H 2 O and H 2 O 2 . However, it was demonstrated that the H 2 O 2 molecule can be reduced to H 2 O at Cu-N x sites without any barrier, thus endowing the CoCu@Cu/CoNP with prolonged stability.…”

Section: Selectivity and Stabilitymentioning

confidence: 96%

The Optimized Catalytic Performance of Single‐Atom Catalysts by Incorporating Atomic Clusters or Nanoparticles: In‐Depth Understanding on Their Synergisms

Zhou

Xue

et al. 2023

Advanced Energy Materials

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The performance optimization of single‐atom catalysts (SACs) is important but remains challenging. Taking advantage of accompanying in situ formation of atomic clusters (ACs)/nanoparticles (NPs) during the preparation of SACs can be a promising solution. The coupled ACs/NPs and single atoms (SAs) can be highly efficient in catalyzing various reactions (e.g., oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), CO2 reduction reaction (CO2RR), N2 oxidation reaction (NOR), etc), showing superior activity, selectivity, and stability. The mechanisms can be mainly categorized as ACs/NPs intensified SAs, SAs intensified ACs/NPs, and reactions proceeding on both ACs/NPs and SAs. The proposed mechanisms may be applicable to rationalize the excellent catalysts consisting of ACs/NPs and SAs. In the end, the existing issues and further development directions are put forward. This review is expected to simultaneously contribute to the development and application of highly efficient SACs and the in‐depth understanding of the single‐atom catalysis (SAC).

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Section: Selectivity and Stabilitymentioning

confidence: 96%

The Optimized Catalytic Performance of Single‐Atom Catalysts by Incorporating Atomic Clusters or Nanoparticles: In‐Depth Understanding on Their Synergisms

Zhou

Xue

et al. 2023

Advanced Energy Materials

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“…In addition, most supported metal catalysts likely contain a mixture of metal single atoms, metal clusters, or metal nanoparticles, which also show improved catalytic performance due to the electron synergistic effect of the metal single atoms and clusters or nanoparticles. [49][50][51][52][53] Unfortunately, these hybrid structures of single metal species (i.e., the mixtures of single atoms and nano-islands of the same metal element) do not belong to the as-proposed third category of "island-sea synergism" SANIs catalyst (because the surfaces of these metal or metal oxide nano-islands do not have the single-atom structure of the second metal). We propose to introduce a second metal single atom to selectively load on to these metal or metal oxide nano-islands and investigate the synergistic effect of the single atoms on nano-islands and carrier (sea), which is likely to further improve catalytic performance or lead to new reaction mechanisms.…”

Section: The Challenges and Proposals Of Sanismentioning

confidence: 99%

Single‐Atom Nano‐Islands (SANIs): A Robust Atomic–Nano System for Versatile Heterogeneous Catalysis Applications

2023

Advanced Materials

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and conventional transition metals SACs supported on metal or non-metal carriers) have been developed and upgraded greatly. [3][4][5] Theoretically speaking, the dispersion limit of supported metal catalysts is the uniform distribution of the metal in the form of single atoms on the support: this is not only the ideal state of supported metal catalysts, but also brings the science of catalysis from the "nano age" into the "atomic age". [6][7][8] SACs usually refer to the active sites where isolated metal atoms are loaded onto the surface of the carriers to reach the maximum atomic utilization. These active sites are anchored by adjacent coordination atoms on the carrier (generally through covalent metal-nonmetal bonding) to prevent the thermodynamic diffusion and irreversible aggregation of single metal atoms. However, SACs all along face an unavoidable physicochemical problem: when the metal particles are reduced to the level of single atomic dispersions, the specific surface area increases sharply (reaching the maximum theoretical value), also leading to the maximum value of the metal surface free energy. [9] Therefore, in the actual application environment and catalytic reaction conditions, especially at high temperature or in a reducing atmosphere, the single atomic metal active sites are extremely prone to agglomeration and coupling to form large atomic clusters (even nanoparticles), resulting in the degradation of catalyst performance or even complete inactivation. [10] Recently, however, scientists have found that fully exposed cluster catalysts with low coordination metal bonds (the coordination number of the metal bond is ≈4.4) [11] and local single-atomic agglomeration [12] show more satisfactory performances in specific complex catalytic systems. These works provide a basic understanding of the dynamic stability of SACs under working conditions and call for a reassessment of the reported stability of SACs by considering realistic reaction conditions.Admittedly, it is quite necessary to reevaluate the realistic catalytic stability and dynamic catalysis mechanism of SACs; nevertheless, we hold the opinion that it is more important to design fundamentally a kind of efficient SACs with high activity and high stability at the same time (such as the "moving but not aggregating" design philosophy for metal active sites). On October 26, 2022, in collaboration with Yong Wang's group at Washington State University, Bruce C. Gates's group at the University of California, and Jingyue Liu's group at Arizona Academician Tao Zhang from China and co-workers designed the first Pt 1 / FeO x single-atom catalysts (SACs) in 2011, and they proposed the concept of "single-atom catalysis" in the field of heterogeneous catalysis. Generally, it is easy for active metal single-atom sites on a carrier to migrate and aggregate, which results in poor performance; or the chemical bond between the metal atom and carrier is too strong (immovable), which results in passivation of the active site. Recently, "nano-island" type SACs were...

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“…Generally, synergic catalysis of multiple active sites can significantly lower the kinetic barriers for a multistep reaction to accelerate the reaction process . Consequently, coupling multifunctional active sites into one catalyst for complex multistep reactions is an effective strategy to improve the performance of the catalyst. − Recently, the coexistence of nanoparticles and single-atom sites, a common phenomenon during synthesis, has been demonstrated to achieve better electrocatalytic activity than separate nanoparticles and separate single atoms. − For example, Chong et al proposed that close proximity between platinum–cobalt core–shell nanoparticles and single-atom Co sites could promote the synergistic catalysis of oxygen reduction reaction (ORR) . Zhang et al designed a supported Rh catalyst with both isolated Rh atoms and Rh ensemble sites for cyclohexanol dehydrogenation, in which isolated Rh species is extremely active for the first step of dehydrogenation, and Rh ensemble sites are mainly responsible for the successive reaction step .…”

Section: Introductionmentioning

confidence: 99%

Ensemble Effect of Ruthenium Single-Atom and Nanoparticle Catalysts for Efficient Hydrogen Evolution in Neutral Media

Liu

Zhang

et al. 2023

ACS Appl. Mater. Interfaces

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Hydrogen evolution reaction (HER) plays a key role in electrochemical water splitting, which is a sustainable way for hydrogen production. The kinetics of HER is sluggish in neutral media that requires noble metal catalysts to alleviate energy consumption during the HER process. Here, we present a catalyst comprising a ruthenium single atom (Ru1) and nanoparticle (Run) loaded on the nitrogen-doped carbon substrate (Ru1-Run/CN), which exhibits excellent activity and superior durability for neutral HER. Benefiting from the synergistic effect between single atoms and nanoparticles in the Ru1-Run/CN, the catalyst exhibits a very low overpotential down to 32 mV at a current density of 10 mA cm–2 while maintaining excellent stability up to 700 h at a current density of 20 mA cm–2 during the long-term test. Computational calculations reveal that, in the Ru1-Run/CN catalyst, the existence of Ru nanoparticles affects the interactions between Ru single-atom sites and reactants and thus improves the catalytic activity of HER. This work highlights the ensemble effect of electrocatalysts for HER and could shed light on the rational design of efficient catalysts for other multistep electrochemical reactions.

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CO‐Tolerant PEMFC Anodes Enabled by Synergistic Catalysis between Iridium Single‐Atom Sites and Nanoparticles

Cited by 9 publications

References 45 publications

The Optimized Catalytic Performance of Single‐Atom Catalysts by Incorporating Atomic Clusters or Nanoparticles: In‐Depth Understanding on Their Synergisms

The Optimized Catalytic Performance of Single‐Atom Catalysts by Incorporating Atomic Clusters or Nanoparticles: In‐Depth Understanding on Their Synergisms

Single‐Atom Nano‐Islands (SANIs): A Robust Atomic–Nano System for Versatile Heterogeneous Catalysis Applications

Ensemble Effect of Ruthenium Single-Atom and Nanoparticle Catalysts for Efficient Hydrogen Evolution in Neutral Media

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