N-Coordinated Ir single atoms anchored on carbon octahedrons for catalytic oxidation of formaldehyde under ambient conditions

Peng, Shiqi; Rao, Yongfang; Huang, Yu; Li, Tan; Li, Rong; Cao, Junji; Lee, Shuncheng

doi:10.1039/d2cy00743f

Cited by 7 publications

(4 citation statements)

References 47 publications

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“…15b Meanwhile, no agglomeration of Ir nanoparticles was observed, 15c which is consistent with the TEM characterization results (Figure 5). Noteworthily, it is documented that higher pyrolysis temperature facilitates the formation of metallic iridium rather than Ir-N X species, 16 which well rationalizes the better catalytic performance of Ir-N@HPmeso ZrO 2 -350 than those catalysts pyrolyzed at 500 and 800 °C (Figure 2). The poisoning experiment by treating the model reaction with KSCN led to no product formation, which further proves that the Ir-N X species serve as the catalytically active sites (Table S2).…”

Section: ■ Results and Discussionmentioning

confidence: 71%

Direct Construction of Julolidines via Reductive Annulation of Quinolines and Conjugated Enones by a MOF-Derived Hierarchically Porous Iridium Catalyst

Jia

Xie

et al. 2022

ACS Catal.

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Here, we describe the development of a MOF-derived hierarchically porous ZrO2-supported iridium catalyst (Ir-N@HP-mesoZrO2), featuring sufficient accessible catalytic sites even with ultralow iridium loading. Such a catalyst was successfully applied to selective and direct construction of julolidines via catalytic reductive annulation of readily available quinolines and conjugated enones, proceeding with good substrate and functional group compatibility, reusable catalyst, high step and atom efficiency, and easy applicability for the fabrication of functional molecules. The present work opens a door to further develop useful transformations by merging hydrogen transfer-mediated substrate activation with in situ incorporation of a coupling sequence under heterogeneous reductive catalysis.

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Section: ■ Results and Discussionmentioning

confidence: 71%

Direct Construction of Julolidines via Reductive Annulation of Quinolines and Conjugated Enones by a MOF-Derived Hierarchically Porous Iridium Catalyst

Jia

Xie

et al. 2022

ACS Catal.

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“… 12 , 16 , 45 − 47 However, the relevance of our results is not limited to metal-TCNQ and can be broadly applied to all supported systems, including models for the highly promising single-atom catalysts based on N-doped graphene. 48 − 50 We propose that graphene-supported metal-TCNQ systems can serve as perfect models for such catalysts, as they feature the same local environment of the metal (coordinated to four nitrogen atoms, metal-N 4 ), they utilize a similar supporting material (graphene), and they can be studied with atomic-scale precision using on-surface approaches. Moreover, the performance of single-atom catalysts is undoubtedly affected by local doping or charge-transfer effects, and the dopable graphene support offers a unique opportunity to experimentally model such effects.…”

Section: Resultsmentioning

confidence: 99%

How the Support Defines Properties of 2D Metal–Organic Frameworks: Fe-TCNQ on Graphene versus Au(111)

Jakub,

Shahsavar,

Planer

et al. 2024

J. Am. Chem. Soc.

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The functionality of 2D metal−organic frameworks (MOFs) is crucially dependent on the local environment of the embedded metal atoms. These atomic-scale details are best ascertained on MOFs supported on well-defined surfaces, but the interaction with the support often changes the MOF properties. We elucidate the extent of this effect by comparing the Fe-TCNQ 2D MOF on two weakly interacting supports: graphene and Au(111). We show that the Fe-TCNQ on graphene is nonplanar with iron in quasi-tetrahedral sites, but on Au(111) it is planarized by stronger van der Waals interaction. The differences in physical and electronic structures result in distinct properties of the supported 2D MOFs. The d z 2 center position is shifted by 1.4 eV between Fe sites on the two supports, and dramatic differences in chemical reactivity are experimentally identified using a TCNQ probe molecule. These results outline the limitations of common onsurface approaches using metal supports and show that the intrinsic MOF properties can be partially retained on graphene.

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“…Formaldehyde (HCHO) is the most prevalent indoor gaseous pollutant, which is released from construction and decoration materials ( Yu and Crump, 1998 ; Salthammer et al, 2010 ). SACs for HCHO abatement consist of metal-oxide supported SACs ( Hu et al, 2015 ; Chen et al, 2017b ; Chen J. et al, 2018 ; Chen et al, 2019 ; Chen J. et al, 2020 )and carbon supported SACs( Peng et al, 2022 ; Tang et al, 2022 ) according to the variety of supports.…”

Section: Applications Of Single-atom Catalysts For Air Pollutant Removalmentioning

confidence: 99%

“…For HCHO oxidation over carbon supported SACs, Langmuir–Hinshelwood (L-H) mechanism is appropriate and molecular oxygen activation is pivotal. N-doped carbon stabilized iridium single atoms (Ir 1 -N-C) could deliver high HCHO removal efficiency (>95%) under high/low concentrations at 20°C ( Peng et al, 2022 ). Ir single atoms, coordinating with four N atoms, serve as the active sites to adsorb and dissociate O 2 by the strong electron coupling between Ir 5d orbital and O 2 2p orbital.…”

Section: Applications Of Single-atom Catalysts For Air Pollutant Removalmentioning

confidence: 99%

Recent progresses on single-atom catalysts for the removal of air pollutants

Wang

Wang²

2022

Front. Chem.

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The booming industrialization has aggravated emission of air pollutants, inflicting serious harm on environment and human health. Supported noble-metals are one of the most popular catalysts for the oxidation removal of air pollutants. Unfortunately, the high price and large consumption restrict their development and practical application. Single-atom catalysts (SACs) emerge and offer an optimizing approach to address this issue. Due to maximal atom utilization, tunable coordination and electron environment and strong metal-support interaction, SACs have shown remarkable catalytic performance on many reactions. Over the last decade, great potential of SACs has been witnessed in the elimination of air pollutants. In this review, we first briefly summarize the synthesis methods and modulation strategies together with the characterization techniques of SACs. Next, we highlight the application of SACs in the abatement of air pollutants including CO, volatile organic compounds (VOCs) and NOx, unveiling the related catalytic mechanism of SACs. Finally, we propose the remaining challenges and future perspectives of SACs in fundamental research and practical application in the field of air pollutant removal.

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N-Coordinated Ir single atoms anchored on carbon octahedrons for catalytic oxidation of formaldehyde under ambient conditions

Abstract: N-Coordinated Ir single atoms using N-doped carbon as a non-oxide support for formaldehyde removal under ambient conditions for the first time.

Cited by 7 publications

References 47 publications

Direct Construction of Julolidines via Reductive Annulation of Quinolines and Conjugated Enones by a MOF-Derived Hierarchically Porous Iridium Catalyst

Direct Construction of Julolidines via Reductive Annulation of Quinolines and Conjugated Enones by a MOF-Derived Hierarchically Porous Iridium Catalyst

How the Support Defines Properties of 2D Metal–Organic Frameworks: Fe-TCNQ on Graphene versus Au(111)

Recent progresses on single-atom catalysts for the removal of air pollutants

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