Improved hydrothermal stability of Pd nanoparticles on nitrogen-doped carbon supports

Huo, Jiajie; Duan, Pu; Pham, Hien N.; Chan, Yee Jher; Datye, Abhaya K.; Schmidt‐Rohr, Klaus; Shanks, Brent H.

doi:10.1039/c8cy00947c

Cited by 21 publications

(17 citation statements)

References 54 publications

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“…1b and Supplementary Fig. 1) 19,20 . Upon carbonization at 300°C for 10 min, an additional broad signal appeared in the range between −180 and −230 ppm in the 15 N{ 1 H} CPMAS spectrum (Fig.…”

Section: Resultsmentioning

confidence: 97%

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Transition metal-like carbocatalyst

et al. 2020

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Catalytic cleavage of strong bonds including hydrogen-hydrogen, carbon-oxygen, and carbonhydrogen bonds is a highly desired yet challenging fundamental transformation for the production of chemicals and fuels. Transition metal-containing catalysts are employed, although accompanied with poor selectivity in hydrotreatment. Here we report metal-free nitrogen-assembly carbons (NACs) with closely-placed graphitic nitrogen as active sites, achieving dihydrogen dissociation and subsequent transformation of oxygenates. NACs exhibit high selectivity towards alkylarenes for hydrogenolysis of aryl ethers as model biooxygenates without over-hydrogeneration of arenes. Activities originate from cooperating graphitic nitrogen dopants induced by the diamine precursors, as demonstrated in mechanistic and computational studies. We further show that the NAC catalyst is versatile for dehydrogenation of ethylbenzene and tetrahydroquinoline as well as for hydrogenation of common unsaturated functionalities, including ketone, alkene, alkyne, and nitro groups. The discovery of nitrogen assembly as active sites can open up broad opportunities for rational design of new metal-free catalysts for challenging chemical reactions.

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Section: Resultsmentioning

confidence: 97%

“…1e). Fast CP build-up suggests that the new signal can be assigned to the N-H-containing species, imidazolium 19 , in which the aromatic ring contains two nitrogen atoms ( Supplementary Fig. 2).…”

Section: Resultsmentioning

confidence: 99%

Transition metal-like carbocatalyst

et al. 2020

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“…For example, the doping of nitrogen on the carboncoated SBA-15 support significantly improved the stability of Pd metal against leaching and sintering during FUR hydrogenation. [103] The N-doped mesoporous carbon-supported Ru nanoparticles showed higher stability compared to the undoped carbon support during glycerol reforming. [104] The Ndoped CNT-supported Pd nanoparticles showed stability against sintering during nitrobenzene hydrogenation reaction.…”

Section: Improving the Stability Of Supported Metal Catalystsmentioning

confidence: 96%

The Size‐Dependent Catalytic Performances of Supported Metal Nanoparticles and Single Atoms for the Upgrading of Biomass‐Derived 5‐Hydroxymethylfurfural, Furfural, and Levulinic acid

2021

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The success of integrated biorefinery relies on developing robust and economical catalytic processes to produce liquid fuels and value-added chemicals from the waste lignocellulose biomass. Platform chemicals obtained from biomass are multifunctional molecules, and their upgrading via various catalytic processes requires active and selective catalysts. Supported transition metal nanoparticles have been used extensively to catalyze the upgrading of biomass-derived platform chemicals. Recent literature studies have focused on understanding the size-dependent catalytic performances of supported transition metal nanoparticles and single atoms in biomass-related chemical transformations. The catalytic behavior of transition metals depends on their size-dependent geometric and electronic structures, and by controlling the size, the catalytic behavior can be optimized. Herein, we have reviewed the synthesis methodologies and characterization techniques of supported metal nanoparticles of different sizes and supported single atoms and have summarized several literature examples employing these catalysts to upgrade biomass-derived platform chemicals such as; 5-hydroxymethylfurfural, furfural, and levulinic acid, into liquid fuels and value-added chemicals.

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“…34 It was also found that the metal leaching could be inhibited effectively due to graphite encapsulation. 35 In this work, we developed a series of MNC-T (M/T: different metals/pyrolysis temperatures) catalysts and tested their catalytic performances for the conversion of 2phenoxyacetophenone. It was demonstrated that CoNC-900 presented outstanding catalytic performance in the reaction.…”

Section: ■ Introductionmentioning

confidence: 99%

“…In addition, N-doped carbons could generate more active sites due to the tunable electron feature and improve the activity of the catalysts well. , In addition, the carbon materials enhanced the contact between the substrate and the catalyst by increasing wettability of the surface . It was also found that the metal leaching could be inhibited effectively due to graphite encapsulation …”

Section: Introductionmentioning

confidence: 99%

Selective Hydrogenolysis of Lignin Model Compounds to Aromatics over a Cobalt Nanoparticle Catalyst

Liu

et al. 2021

ACS Sustainable Chem. Eng.

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Catalytic conversion of renewable lignin to aromatics can effectively alleviate the fossil resource crisis. Herein, we prepared porous nitrogen-doped carbon-supported cobalt nanoparticle catalyst (CoNC) using a SiO2 template and tested its catalytic performance for cleavage of the β-O-4 ether bond in lignin model compounds. It was found that the catalyst pyrolyzed in a nitrogen atmosphere at 900 °C (CoNC-900) could catalyze 2-phenoxyacetophenone to ethylbenzene and phenol effectively, affording both in 99.0% yields. Further study indicated that the catalytic system was efficient for transformation of various β-O-4 ketones with methoxyl groups with high yields of desired products. The excellent catalytic performance was related to the cobalt nanoparticles, large pore volume, and specific surface area. Furthermore, the catalyst could be reused five times without obvious loss of the activity, indicating its stability during the reaction process. The reaction pathway was studied on the basis of some control experiments.

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Improved hydrothermal stability of Pd nanoparticles on nitrogen-doped carbon supports

Abstract: Carbon supports have been shown to provide better hydrothermal stability than alumina or silica supports, thus attracting more attention for aqueous-phase biomass conversion reactions.

Cited by 21 publications

References 54 publications

Transition metal-like carbocatalyst

Transition metal-like carbocatalyst

The Size‐Dependent Catalytic Performances of Supported Metal Nanoparticles and Single Atoms for the Upgrading of Biomass‐Derived 5‐Hydroxymethylfurfural, Furfural, and Levulinic acid

Selective Hydrogenolysis of Lignin Model Compounds to Aromatics over a Cobalt Nanoparticle Catalyst

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