Rational Design of Main Group Metal-Embedded Nitrogen-Doped Carbon Materials as Frustrated Lewis Pair Catalysts for CO<sub>2</sub> Hydrogenation to Formic Acid

Zhang, Yue; Mo, Yirong; Cao, Zexing

doi:10.1021/acsami.1c20230

Cited by 27 publications

(13 citation statements)

References 79 publications

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“…The carbon nitride group is another 2D material that is widely used in heterogeneous catalysis [90]. For example, Wan et al reported Al/B doping C 2 N and g-C 3 N 4 to construct FLPs from their DFT calculations [55].…”

Section: Flps Based On Functionalized Surfacesmentioning

confidence: 99%

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Frustrated Lewis Pairs in Heterogeneous Catalysis: Theoretical Insights

2022

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Frustrated Lewis pair (FLP) catalysts have attracted much recent interest because of their exceptional ability to activate small molecules in homogeneous catalysis. In the past ten years, this unique catalysis concept has been extended to heterogeneous catalysis, with much success. Herein, we review the recent theoretical advances in understanding FLP-based heterogeneous catalysis in several applications, including metal oxides, functionalized surfaces, and two-dimensional materials. A better understanding of the details of the catalytic mechanism can help in the experimental design of novel heterogeneous FLP catalysts.

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Section: Flps Based On Functionalized Surfacesmentioning

confidence: 99%

“…catalysis [90]. For example, Wan et al reported Al/B doping C2N and g-C3N4 to construct FLPs from their DFT calculations [55].…”

Section: Flps Based On Functionalized Surfacesmentioning

confidence: 99%

Frustrated Lewis Pairs in Heterogeneous Catalysis: Theoretical Insights

2022

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“…With the massive consumption of fossil fuels, excessive carbon dioxide (CO 2 ) emissions are considered as a thorny climate and environmental problem. , However, as a reproducible and nontoxic C1 resource, CO 2 can be converted into high-value-added chemicals under certain conditions, realizing the efficient utilization of resources and reducing environment hazards. , The production of cyclic carbonates from CO 2 and epoxide by cycloaddition, as an atom-economic reaction, has attracted a surge of attention. , In view of the large-scale application of cyclic carbonates, homogeneous catalysts and heterogeneous catalysts such as ionic liquids (ILs), metal oxides, metal–organic frameworks (MOFs), zeolites, etc., have been extensively utilized for CO 2 cycloaddition. − A homogeneous system is not conducive to product separation . For most heterogeneous catalysts, the toxic metals can be released from metal oxides.…”

Section: Introductionmentioning

confidence: 99%

“…With the massive consumption of fossil fuels, excessive carbon dioxide (CO 2 ) emissions are considered as a thorny climate and environmental problem. 1,2 However, as a reproducible and nontoxic C1 resource, CO 2 can be converted into high-valueadded chemicals under certain conditions, realizing the efficient utilization of resources and reducing environment hazards. 3,4 The production of cyclic carbonates from CO 2 and epoxide by cycloaddition, as an atom-economic reaction, has attracted a surge of attention.…”

Section: Introductionmentioning

confidence: 99%

Amino-Functionalized Ionic-Liquid-Grafted Covalent Organic Frameworks for High-Efficiency CO₂Capture and Conversion

Yin

Wang

Tang

2022

ACS Appl. Mater. Interfaces

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Rationally integrating desired functional components into a composite material can endow the tailored function to achieve the corresponding purpose. This is the first case where a series of [AeImBr] X% -TAPT-COFs (X = 0, 17,33,50, 67, 83, 100) were fabricated by chemically integrating the amino-functionalized imidazole ionic liquid (NH 2 -IL) onto channel walls of mesoporous covalent organic framework materials ([HO] X% -TAPT-COFs). By virtue of the polar groups (amino groups) and abundant imidazole cations of NH 2 -IL and its microporous nature, the obtained [AeImBr] X% -TAPT-COFs exhibit higher CO 2 capture activity than [HO] X% -TAPT-COFs. Correspondingly, the CO 2 equilibrium capture capacity increases from 62.6 to 117.4 mg/g, which is crucial to the storage of enough CO 2 around the catalytic active sites. Additionally, the synergistic effect of −NH 2 and Br − in NH 2 -IL can also improve the cycloaddition reaction rate. The characteristics of [AeImBr] X% -TAPT-COFs contribute to the efficient generation of cyclic carbonate through heterogeneously catalyzing CO 2 -epoxide cycloaddition without any solvents and cocatalysts. Specifically, [AeImBr] 83% -TAPT-COF has a CO 2 equilibrium capture capacity of 117.4 mg/g and cyclochloroallyl carbonate yield of 99.1%. As a result of the use of the chemical grafting method, [AeImBr] X% -TAPT-COFs possess excellent stability and cycle life. The equilibrium capture capacity and cyclochloroallyl carbonate yield reach 112.7 mg CO 2 /g adsorbent and 95.0% at the eighth cycle.

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“…Huang et al found that the Faraday efficiency for the electrocatalytic reduction of CO 2 to HCOOH can be remarkably enhanced on the single Mo atom loaded N-doped graphene (Mo@NG) compared to N-doped graphene (NG) . In addition, some studies have reported that single-atom Fe-, Co-, or Al-incorporated 2D substrates can also promote CO 2 hydrogenation. − However, the main product of CO 2 hydrogenation catalyzed by such SACs is usually HCOOH, while the formation of other C1 products is rarely reported. Herein, a crucial issue then arises: Is there a metal-embedded SAC catalyst that can produce different C1 products of CO 2 hydrogenation such as CH 3 OH?…”

Section: Introductionmentioning

confidence: 99%

Unraveling the Catalytic Performance of the Nonprecious Metal Single-Atom-Embedded Graphitic s-Triazine-Based C₃N₄ for CO₂ Hydrogenation

Zhang

Cao

2022

ACS Appl. Mater. Interfaces

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Graphitic carbon nitride (g-C3N4) is regarded as a promising potent photoelectrocatalyst for CO2 reduction. Here, extensive first-principles calculations and ab initio molecular dynamics (AIMD) simulations are performed to systematically explore the structural and electronic properties of nonprecious metal single-atom-embedded graphitic s-triazine-based C3N4 (M@gt-C3N4, M = Mn, Fe, Co, Ni, Cu, and Mo) monolayer materials and their catalytic performances as the single-atom catalysts (SACs) for CO2 hydrogenation to HCOOH, CO, and CH3OH. It is found that the atomically dispersed non-noble metal Mn, Fe, Co, and Mo sites anchored on gt-C3N4 can efficiently activate both H2 and CO2, and their coadsorbed state serves as a precursor to the hydrogenation of CO2 to different C1 products. Among these SACs (M@gt-C3N4, M = Mn, Fe, Co, and Mo), Co@gt-C3N4 was predicted to have the best catalytic performance for CO2 hydrogenation to C1 products, although their mechanistic details are somewhat different. The predicted energy barriers of the rate-determining steps for the conversion of CO2 into HCOOH, CO, and CH3OH on Co@gt-C3N4 are 0.58, 0.67, and 1.19 eV, respectively. The desorption of products is generally energy-demanding, but it can be facilitated remarkably by the subsequent adsorption of H2, which regenerates M@gt-C3N4 for the next catalytic cycle. The present study demonstrates that the catalytic performance of gt-C3N4 can be well regulated by embedding the non-noble metal single atom, and the porous gt-C3N4 is nicely suited for the construction of high-performance single-atom catalysts.

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Rational Design of Main Group Metal-Embedded Nitrogen-Doped Carbon Materials as Frustrated Lewis Pair Catalysts for CO₂ Hydrogenation to Formic Acid

Cited by 27 publications

References 79 publications

Frustrated Lewis Pairs in Heterogeneous Catalysis: Theoretical Insights

Frustrated Lewis Pairs in Heterogeneous Catalysis: Theoretical Insights

Amino-Functionalized Ionic-Liquid-Grafted Covalent Organic Frameworks for High-Efficiency CO₂Capture and Conversion

Unraveling the Catalytic Performance of the Nonprecious Metal Single-Atom-Embedded Graphitic s-Triazine-Based C₃N₄ for CO₂ Hydrogenation

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Rational Design of Main Group Metal-Embedded Nitrogen-Doped Carbon Materials as Frustrated Lewis Pair Catalysts for CO2 Hydrogenation to Formic Acid

Cited by 27 publications

References 79 publications

Frustrated Lewis Pairs in Heterogeneous Catalysis: Theoretical Insights

Frustrated Lewis Pairs in Heterogeneous Catalysis: Theoretical Insights

Amino-Functionalized Ionic-Liquid-Grafted Covalent Organic Frameworks for High-Efficiency CO2Capture and Conversion

Unraveling the Catalytic Performance of the Nonprecious Metal Single-Atom-Embedded Graphitic s-Triazine-Based C3N4 for CO2 Hydrogenation

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Rational Design of Main Group Metal-Embedded Nitrogen-Doped Carbon Materials as Frustrated Lewis Pair Catalysts for CO₂ Hydrogenation to Formic Acid

Amino-Functionalized Ionic-Liquid-Grafted Covalent Organic Frameworks for High-Efficiency CO₂Capture and Conversion

Unraveling the Catalytic Performance of the Nonprecious Metal Single-Atom-Embedded Graphitic s-Triazine-Based C₃N₄ for CO₂ Hydrogenation