C–O bond activation using ultralow loading of noble metal catalysts on moderately reducible oxides

Fu, Jiayi; Lym, Jonathan; Zheng, Weiqing; Alexopoulos, Konstantinos; Mironenko, Alexander V.; Li, Na; Boscoboinik, J. Anibal; Su, Dong; Weber, Ralph T.; Vlachos, Dionisios G.

doi:10.1038/s41929-020-0445-x

Cited by 159 publications

(119 citation statements)

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“…3 ). The peaks at 76.1 and 72.9 eV correspond to the Pt δ+ 4 f 5/2 and Pt δ+ 4 f 7/2 , respectively 35 – 37 . These results imply that there is a strong electron interaction between Nb 2 O 5 -Ov and Pt, and the electron transfers from Pt to the Nb 2 O 5 -Ov support.…”

Section: Resultsmentioning

confidence: 99%

“…This step was calculated to be exothermic by 1.55 eV and exhibited a barrier of 0.45 eV (from c to e). It is generally accepted that the activity of Pt–H species is higher than that of O–H species 37 . The Pt–H species attacked the C site of C–OH in HMF accompanied by the breakage of C–O, leading to the formation of MF and -OH adsorbed on the Nb site.…”

Section: Discussionmentioning

confidence: 99%

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Selective hydrogenation of 5-(hydroxymethyl)furfural to 5-methylfurfural over single atomic metals anchored on Nb2O5

et al. 2021

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Abstract5-Methylfurfural (MF) is a very useful chemical. Selective hydrogenation of biomass platform molecule 5-(hydroxymethyl)furfural (HMF) to MF using H2 as the reducing agent is very attractive, but challenging because hydrogenation of C=O bond in HMF is more favourable than C–OH both kinetically and thermodynamically, and this route has not been realized. In this work, we prepare isolated single atomic catalysts (SACs) Pt1/Nb2O5-Ov, Pd1/Nb2O5-Ov, and Au1/Nb2O5-Ov, in which single metal atoms are supported on oxygen defective Nb2O5 (Nb2O5-Ov). It is discovered that the SACs can efficiently catalyze the hydrogenation of HMF to MF using H2 as the reducing agent with MF selectivity of >99% at complete conversion, while the selectivities of the metal nanocatalysts supported on Nb2O5 are very poor. A combination of experimental and density function theory (DFT) studies show that the unique features of the SACs for the reaction result from the cooperation of the Nb and Pt sites near the interface in the Pt1/Nb2O5-Ov. The Pt atoms are responsible for the activation of H2 and the Nb sites activate C-OH in the reaction. This work opens the way for producing MF by direct hydrogenation of biomass-derived HMF using H2 as the reductant.

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Section: Resultsmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Selective hydrogenation of 5-(hydroxymethyl)furfural to 5-methylfurfural over single atomic metals anchored on Nb2O5

et al. 2021

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“…In contrast, a series of IR bands are observed on 0.1Pt-2Zn/Si-Beta and two stable bands at 2120 cm À1 and 2075 cm À1 are preserved after He purging. According to literature reports [33][34][35], the band of 2075 cm À1 can be assigned to the CO molecules linearly adsorbed in an on-top geometry on Pt atoms on single-crystal or nanoparticle surfaces and the band of 2120 cm À1 belongs to the CO molecules linearly adsorbed on Pt single atoms. The formation of solely linearly-adsorbed CO hints to the existence of highly dispersed Pt species of 0.1Pt-2Zn/Si-Beta zeolite, in good agreement with TEM observations.…”

Section: Catalyst Preparation and Characterizationmentioning

confidence: 97%

Optimizing zeolite stabilized Pt-Zn catalysts for propane dehydrogenation

Xie

Chai

Sun

et al. 2021

Journal of Energy Chemistry

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“…76,77 Such an atomic-level understanding will provide valuable guidance in designing and preparing advanced catalysts. 24,[78][79][80][81][82][83][84][85][86] Moreover, in situ and operando studies concerning the dynamic changes during the catalytic reactions are required to further reveal the mechanism involved in catalysis. Compared with SACs made by wet chemistry that are indeed closer to practical applications, single atoms fabricated by physical deposition on ultrathin oxide lms (surface free energy approach) provide better-dened models for fundamental studies, especially for local and dynamic characterization studies, of practical catalysts.…”

Section: Summary and Perspectivesmentioning

confidence: 99%