Confined-interface-directed synthesis of Palladium single-atom catalysts on graphene/amorphous carbon

Xi, Jiangbo; Sun, Hongyu; Zhang, Zheye; Duan, Xianming; Xiao, Junwu; Xiao, Fei; Liu, Limin; Wang, Shuai

doi:10.1016/j.apcatb.2017.11.057

Cited by 164 publications

(101 citation statements)

References 42 publications

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“…[69,70] On the other hand, if NPs can also catalyze the reaction (SAs > NPs) the activity will rise more gradually with increasing dispersion until it reaches ap lateau as the metal species tend toward SAs. [71,72] In contrast, if SAs are ineffective (SA ! NPs) the activity may initially increase as the metal content is reduced because of higher dispersion, before falling sharply to close to zero when metal clusters are no longer present in the sample.…”

Section: Sacs Versus Npsmentioning

confidence: 86%

“…Most commonly this is approached by comparing the turnover frequency( tof) per mole of metal in the catalyst. [71,72] In contrast, if SAs are ineffective (SA ! If SAs exhibit am uch higher activity than NPs (SAs @ NPs), such that the contribution of the latter becomes insignificant, asharp increase in catalytic turnover will be observed at low metal content when the majority of metal centers become spatially isolated.…”

Section: Sacs Versus Npsmentioning

confidence: 99%

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The Multifaceted Reactivity of Single‐Atom Heterogeneous Catalysts

2018

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Single-atom heterogeneous catalysts (SACs) attached to carefully chosen hosts are attracting considerable interest; principally because they offer maximum utilization per metal atom and are usually readily recyclable. However, diminution of the atomic population of nanoparticles or nanoclusters to single atoms can significantly alter reactivity because of the consequent changes in the active-site structure. By examining various diverse applications, we ascertain whether the performance of SACs is enhanced or suppressed. We also note that SACs generally display unique kinds of catalytic cycles. The choice of host is crucial since it influences both the electronic and steric environment of the metal center. Moreover, it may function as a cocatalyst. All these aspects impact upon the design of new SACs, which exhibit similarities to hetero- and homogeneous predecessors. Additionally, SACs offer a viable replacement of soluble metal complexes in processes that remain difficult to heterogenize.

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Section: Sacs Versus Npsmentioning

confidence: 86%

Section: Sacs Versus Npsmentioning

confidence: 99%

The Multifaceted Reactivity of Single‐Atom Heterogeneous Catalysts

2018

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“…In some of the studies, the structure of the metal atoms in the carbon matrix is not clearly defined . For instance, Xi et al reported the synthesis of Pd SACs supported on reduced graphene oxide/amorphous carbon (rGO/AC/Pd) by stir‐mixing of K 2 PdCl 4 with rGO@AC. Whereas Pd was presumed to be intercalated between AC and rGO, the exact chemical structure was unclear.…”

Section: Sample Preparationmentioning

confidence: 99%

Carbon‐Supported Single Atom Catalysts for Electrochemical Energy Conversion and Storage

2018

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Single atoms of select transition metals supported on carbon substrates have emerged as a unique system for electrocatalysis because of maximal atom utilization (≈100%) and high efficiency for a range of reactions involved in electrochemical energy conversion and storage, such as the oxygen reduction, oxygen evolution, hydrogen evolution, and CO reduction reactions. Herein, the leading strategies for the preparation of single atom catalysts are summarized, and the electrocatalytic performance of the resulting samples for the various reactions is discussed. In general, the carbon substrate not only provides a stabilizing matrix for the metal atoms, but also impacts the electronic density of the metal atoms due to strong interfacial interactions, which may lead to the formation of additional active sites by the adjacent carbon atoms and hence enhanced electrocatalytic activity. This necessitates a detailed understanding of the material structures at the atomic level, a critical step in the construction of a relevant structural model for theoretical simulations and calculations. Finally, a perspective is included highlighting the promises and challenges for the future development of carbon-supported single atom catalysts in electrocatalysis.

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Section: Fabrication Of Atomic‐scale Active Sitesmentioning

confidence: 99%

“…As shown in Figure d, the Pt complex [Pt(NH 3 ) 4 ] 2+ is confined by 2D Ti 3 O 7 2− sheets and abundant interlayer ions, which can be converted to Pt 1 /TiO 2 by calcination. In another case, double‐shelled hollow carbon spheres were designed to localize single Pd atoms at the interface of the reduced graphene oxide (RGO) inner shell and the AC outer shell (Figure e) …”

Section: Fabrication Of Atomic‐scale Active Sitesmentioning

confidence: 99%

Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions

et al. 2019

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Ammonia is one of the most important chemicals and energy carriers. Currently, ammonia is industrially produced through the Haber–Bosch process under harsh conditions of high pressure and high temperature, which are energy consuming and environmentally unfriendly. Recently, nitrogen reduction to ammonia under ambient conditions has attracted intensive research interest, in which highly efficient catalysts are of great importance. In this review, recent theoretical and experimental progresses on novel heterogeneous catalysts with low atomicity for the nitrogen reduction reaction (NRR) under ambient conditions are highlighted. Reaction mechanisms for the NRR are first introduced. Then, advances in the synthesis and characterization of catalysts with single atom features are summarized, with a particular focus on the rational design of atomic catalysts for the NRR. Lastly, the critical challenges, possible solutions, and future perspectives in the research on NRR catalysis are presented. This review systematically presents the readers with the latest advances in this field, and more importantly, sheds light on the future development of NRR catalysis with the single atomic feature.

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Confined-interface-directed synthesis of Palladium single-atom catalysts on graphene/amorphous carbon

Cited by 164 publications

References 42 publications

The Multifaceted Reactivity of Single‐Atom Heterogeneous Catalysts

The Multifaceted Reactivity of Single‐Atom Heterogeneous Catalysts

Carbon‐Supported Single Atom Catalysts for Electrochemical Energy Conversion and Storage

Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions

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