Single-Atom Catalysts for Thermal Heterogeneous Catalysis in Liquid: Recent Progress and Future Perspective

Cao, Changyan; Song, Weiguo

doi:10.1021/acsmaterialslett.0c00349

Cited by 15 publications

(12 citation statements)

References 84 publications

(133 reference statements)

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“…24−29 However, these SACs still face two key challenges (Figure S1): poor H 2 O 2 utilization efficiency (usually <10%) that makes it costly and low mass loading (generally <3 wt %) that leads to unsatisfactory mass specific activity. 30 Thus, it is urgent to develop a preeminent SAC with both high loading and H 2 O 2 utilization efficiency for one-step direct hydroxylation of the benzene reaction to phenol. Herein, we report that the synergistic interaction between individual single sites in an ultra-high-density Cu SAC of 2.4 atoms/nm 2 (corresponding to the Cu loading of 21.3 wt %) induces distinct reaction paths and overcomes the aforesaid challenges in the benzene hydroxylation reaction.…”

Section: Introductionmentioning

confidence: 99%

Understanding the Density-Dependent Activity of Cu Single-Atom Catalyst in the Benzene Hydroxylation Reaction

Cui

Cao

et al. 2023

ACS Catal.

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Regulating the density of metal single atoms and exploring the interaction among them are showing great potential to further raise the performance of single-atom catalysts (SACs). Herein, we produce a series of Cu SACs with densities ranging from 0.1 to 2.4 atoms/nm 2 and find that the catalytic activity is proportional to Cu single-atom density in the benzene hydroxylation reaction. Mechanistic studies reveal that the interactions among neighboring single-atom moieties in ultra-high-density Cu SAC alter the electronic structures of Cu single atoms, resulting in stronger • OH adsorption, which is beneficial for the benzene hydroxylation reaction by suppressing the O 2 formation side reaction. The adsorption energy of hydroxyl radicals is further proposed and verified as a key descriptor to explain the reaction differences of Cu SACs with various densities. As a result, the ultrahigh-density Cu SAC of 2.4 atoms/nm 2 (21.3 wt %) exhibits maximum mass specific activity and H 2 O 2 utilization efficiency, which are both significantly higher than the reported results in the literature and solved the key challenges of SACs in the benzene hydroxylation reaction. This study sheds light on how the SAC density affects active sites and offers a practical catalyst for phenol production by the H 2 O 2 route.

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Section: Introductionmentioning

confidence: 99%

Understanding the Density-Dependent Activity of Cu Single-Atom Catalyst in the Benzene Hydroxylation Reaction

Cui

Cao

et al. 2023

ACS Catal.

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“…Metal single-atom catalysts (SACs) have received great attention in recent years owing to their well-defined coordination structure and near-100% atomic utilization. − Moreover, SACs are generally dispersed on a heterogeneous support, inducing easy separation and relative robustness. So far, many research groups have constructed SACs for enhanced catalytic activity and selectivity. − Generally, the catalytic performance of SACs is modulated by the electronic structure of the metal centers, which is closely associated with the local atomic structure. − An efficient strategy to tailor the local atomic structure of SACs is the construction of atomic interfaces. − By introducing alien coordination atoms into the support, the newly formed atomic interface between the pristine single-atom structure and the alien atom breaks the structure and electronic symmetry of the single atoms and thus directly alters the interaction with reactants.…”

Section: Introductionmentioning

confidence: 99%

Atomically Dispersed Cu Anchored on Nitrogen and Boron Codoped Carbon Nanosheets for Enhancing Catalytic Performance

Liu

Zheng

Dong

et al. 2021

ACS Appl. Mater. Interfaces

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Development of high-performance heterogeneous catalytic materials is important for the rapid upgrade of chemicals, which remains a challenge. Here, the benzene oxidation reaction was used to demonstrate the effectiveness of the atomic interface strategy to improve catalytic performance. The developed B,N-cocoordinated Cu single atoms anchored on carbon nanosheets (Cu1/B–N) with the Cu–N2B1 atomic interface was prepared by the pyrolysis of a precoordinated Cu precursor. Benefiting from the unique atomic Cu–N2B1 interfacial structure, the designed Cu1/B–N exhibited considerable activity in the oxidation of benzene, which was much higher than Cu1/N–C, Cu NPs/N–C, and N–C catalysts. A theoretical study showed that the enhanced catalytic performance resulted from the optimized adsorption of intermediates, which originated from the manipulation of the electronic structure of Cu single atoms induced by B atom coordination in the Cu–N2B1 atomic interface. This study provides an innovative approach for the rational design of high-performance heterogeneous catalytic materials at the atomic level.

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“…During the last decade, there was an enormous interest in the synthesis and understanding of single metal atoms as the ultimate size for catalytic entities in the transformation of organic molecules [1,2] . At the nanoscale, the chemical reactivity of bulk metals changes with the size of the aggregate of atoms that compose such metal (e. g. nanoparticles, subnanometric clusters, single atoms).…”

Section: Introductionmentioning

confidence: 99%

Supported Single Atom Catalysts for C−H Activation: Selective C−H Oxidations, Dehydrogenations and Oxidative C−H/C−H Couplings

Martín

Cirujano

2021

ChemCatChem

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The activation of C−H bonds in hydrocarbons (saturated, unsaturated and aromatics) by single atom catalysts immobilized in a solid support is an active research front in catalysis. On the one hand, different examples of transition metal catalysts atomically dispersed on inorganic, organic and hybrid supports are constantly designed, synthesized and characterized using advanced microscopy and spectroscopic techniques. On the other hand, active, selective and stable single metal sites are recently developed as high performant heterogeneous catalysts for the C−H activation of organic molecules. This review covers recent examples of selective alkane and arene C−H oxidations, dehydrogenations of alkanes, as well as C−H/C−H oxidative couplings involving arenes, alkenes and alkynes, based on the use of supported single atom catalysts.

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Single-Atom Catalysts for Thermal Heterogeneous Catalysis in Liquid: Recent Progress and Future Perspective

Abstract: Single-atom catalysts have been demonstrated to be efficient catalysts bridging the gap between homogeneous and heterogeneous catalysts.

Cited by 15 publications

References 84 publications

Understanding the Density-Dependent Activity of Cu Single-Atom Catalyst in the Benzene Hydroxylation Reaction

Understanding the Density-Dependent Activity of Cu Single-Atom Catalyst in the Benzene Hydroxylation Reaction

Atomically Dispersed Cu Anchored on Nitrogen and Boron Codoped Carbon Nanosheets for Enhancing Catalytic Performance

Supported Single Atom Catalysts for C−H Activation: Selective C−H Oxidations, Dehydrogenations and Oxidative C−H/C−H Couplings

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