A heterogeneous single-atom palladium catalyst surpassing homogeneous systems for Suzuki coupling

Chen, Zupeng; Vorobyeva, Evgeniya; Mitchell, Sharon; Fako, Edvin; Ortuño, Manuel Á.; López, Núria; Collins, Sean M.; Midgley, Paul A.; Richard, Sylvia; Vilé, Gianvito; Pérez‐Ramírez, Javier

doi:10.1038/s41565-018-0167-2

Cited by 542 publications

(464 citation statements)

References 39 publications

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“…The remaining material was re‐dispersed in deionized water and freeze‐dried to obtain GO. ECN was synthesized as previously described . Briefly, dicyandiamide (10 g) was heated to 823 K (2.3 K min −1 ) in a N 2 atmosphere for 4 h. ECN was obtained by thermal exfoliation of the resulting material at 773 K (5 K min −1 ) for 5 h in static air.…”

Section: Methodsmentioning

confidence: 99%

Tailoring Nitrogen‐Doped Carbons as Hosts for Single‐Atom Catalysts

et al. 2019

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The application of nitrogen‐doped carbons (NDCs) as host materials for single‐atom catalysts (SACs) is increasing because of the strong binding affinity of the heteroatom with transition metals. Establishment of the relation between the properties of NDCs, their interaction with metals, and the performance of the resulting catalysts is crucial to guide the design of more effective SACs but has not been critically addressed. Here, a series of NDCs is prepared and studied as hosts for palladium atoms. The amount of nitrogen incorporated primarily depends on the choice of carbon followed by the doping temperature and nitrogen source. Pyridinic and pyrrolic species predominate in all cases, especially at lower doping temperatures. The stabilization of palladium atoms is successful above a critical nitrogen content that depends on the carbon type. Evaluation in the catalytic semi‐hydrogenation of 2‐methyl‐3‐butyn‐2‐ol readily distinguishes the reactivity of single atoms and nanoparticles, which correlates with the electronic properties of palladium described by the average oxidation state. Comparison with SACs based on compositionally‐related carbon nitride hosts shows that similarly high stability and tunability of the metal is achievable over NDCs, despite their lower nitrogen contents and greater heterogeneity of coordination sites.

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Section: Methodsmentioning

confidence: 99%

Tailoring Nitrogen‐Doped Carbons as Hosts for Single‐Atom Catalysts

et al. 2019

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“…The suitable selection of precursor, appropriate anchoring material/capping cage, and precise defective sites are, however, very critical for all the above mentioned methods to develop SACs successfully . For further details in this regard, recent articles are suggested to the readers …”

Section: Synthesis Of Mncsmentioning

confidence: 99%

Metal Nanoclusters: New Paradigm in Catalysis for Water Splitting, Solar and Chemical Energy Conversion

et al. 2019

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A sustainable future demands innovative breakthroughs in science and technology today, especially in the energy sector. Earth‐abundant resources can be explored and used to develop renewable and sustainable resources of energy to meet the ever‐increasing global energy demand. Efficient solar‐powered conversion systems exploiting inexpensive and robust catalytic materials for the photo‐ and photo‐electro‐catalytic water splitting, photovoltaic cells, fuel cells, and usage of waste products (such as CO2) as chemical fuels are appealing solutions. Many electrocatalysts and nanomaterials have been extensively studied in this regard. Low overpotentials, catalytic stability, and accessibility remain major challenges. Metal nanoclusters (NCs, ≤3 nm) with dimensions between molecule and nanoparticles (NPs) are innovative materials in catalysis. They behave like a “superatom” with exciting size‐ and facet‐dependent properties and dynamic intrinsic characteristics. Being an emerging field in recent scientific endeavors, metal NCs are believed to replace the natural photosystem II for the generation of green electrons in a viable way to facilitate the challenging catalytic processes in energy‐conversion schemes. This Review aims to discuss metal NCs in terms of their unique physicochemical properties, possible synthetic approaches by wet chemistry, and various applications (mostly recent advances in the electrochemical and photo‐electrochemical water splitting cycle and the oxygen reduction reaction in fuel cells). Moreover, the significant role that MNCs play in dye‐sensitized solar cells and nanoarrays as a light‐harvesting antenna, the electrochemical reduction of CO2 into fuels, and concluding remarks about the present and future perspectives of MNCs in the frontiers of surface science are also critically reviewed.

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“…For further understanding of the processing–structural–property relationship as well as the evolution of the active sites in the actual catalytic process, in situ and operando techniques are favorable to providing a versatile investigation platform for the rational design of the catalysts. For example, single Pd atoms on exfoliated g‐C 3 N 4 have shown excellent performance in crosscoupling reactions, and DFT studies suggest that the Pd atoms adopt continuously variable coordination within the carbon nitride lattice, although the experimental verification of this computational simulation remains challenging. Consequently, further development and application of in situ characterization techniques are critical for gaining deeper insight into the fundamental catalytic processes, which is essential for the rational design of novel catalysts. c)Further effort is also required to design efficient NRR catalysts by combining theoretical simulations and experimental studies.…”

Section: Discussionmentioning

confidence: 99%

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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A heterogeneous single-atom palladium catalyst surpassing homogeneous systems for Suzuki coupling

Cited by 542 publications

References 39 publications

Tailoring Nitrogen‐Doped Carbons as Hosts for Single‐Atom Catalysts

Tailoring Nitrogen‐Doped Carbons as Hosts for Single‐Atom Catalysts

Metal Nanoclusters: New Paradigm in Catalysis for Water Splitting, Solar and Chemical Energy Conversion

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

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