Fabrication of highly oxidized Pt single-atom catalysts to suppress the deep hydrogenation of unsaturated aldehydes

Yu, Liang; Tang, Qiong; Liu, Lei; Wang, Dingsheng

doi:10.1016/j.apcatb.2023.122783

Cited by 18 publications

(10 citation statements)

References 62 publications

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“…Liang et al utilized Pt(acac) 2 as a precursor to synthesize highly oxidized Pt SAC (Pt 1 −FeO x / SBA-15) by preconstructing well-dispersed FeO x NCs on SBA-15 support through the impregnation method and evaluated its catalytic performance in cinnamaldehyde hydrogenation to cinnamyl alcohol. 93 Characterization results showed that Pt atoms possessed a high coordination number of Pt−O and were stabilized by FeO x NCs. Preferential adsorption of the C�O bond over a C�C bond on Pt−FeO x sites was key to generate cinnamyl alcohol.…”

Section: Furfuryl Alcohol Dehydrogenative Cyclizationmentioning

confidence: 99%

“…Hydrogenation of the CC bond in α,β-unsaturated aldehydes is kinetically feasible and thermodynamically favorable as compared to that of the CO bond, thus leaving a big challenge in the selective hydrogenation of the CO bond while reserving the CC bond. Liang et al utilized Pt(acac) 2 as a precursor to synthesize highly oxidized Pt SAC (Pt 1 –FeO x /SBA-15) by preconstructing well-dispersed FeO x NCs on SBA-15 support through the impregnation method and evaluated its catalytic performance in cinnamaldehyde hydrogenation to cinnamyl alcohol . Characterization results showed that Pt atoms possessed a high coordination number of Pt–O and were stabilized by FeO x NCs.…”

Section: Application Of Sacs In Biomass Chemical Conversionmentioning

confidence: 99%

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Single-Atom Metal Catalysts for Catalytic Chemical Conversion of Biomass to Chemicals and Fuels

Chen,

Xiao,

Guo

et al. 2024

ACS Catal.

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Among all renewable energy sources (e.g., solar energy, wind, and biomass), biomass is the only organic carbon resource which has great potential to partly replace nonrenewable fossil resources to produce high value-added chemicals and biofuels. Singleatom catalysts (SACs) have shown compelling prospects and arguably become one of the most active research fields in biomass chemical catalysis due to their fascinating strengths in maximum atomic utilization, highly efficient catalytic reactivity, high selectivity, and good stability. Numerous achievements about the SACs have recently been amassed, including advanced synthesis methods, characterization techniques, and theoretical calculation, allowing us to forecast their working mechanisms and the catalytic roles of metals and coordination sites in the catalytic process. Based on the relevant literatures on SACs over the past few years, this review summarizes the preparation methods of SACs and their catalysis applications for biomass conversions with a special focus on the structure−activity relationship and catalytic reaction mechanism as well as prospects for the future developments of SACs. This review provides fundamental information for the development of the SACs in biomass valorization, clearly stimulating the development in this emerging research field.

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Section: Furfuryl Alcohol Dehydrogenative Cyclizationmentioning

confidence: 99%

Section: Application Of Sacs In Biomass Chemical Conversionmentioning

confidence: 99%

Single-Atom Metal Catalysts for Catalytic Chemical Conversion of Biomass to Chemicals and Fuels

Chen,

Xiao,

Guo

et al. 2024

ACS Catal.

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“…48,49 A redshift of 9 cm −1 appears for the C�O vibration from 1676 to 1667 cm −1 , a new C−O vibration at 1046 cm −1 , and a significant reduction in the intensity of alkenyl C−H vibration at 972 cm −1 , while the signals of C�C at 1625 cm −1 and phenyl C−H at 1123 cm −1 are unchanged. 46,47 It is probably due to the hydrogen-bonding between H 2 O and CAL, resulting in the η 1 (C−O) adsorption mode of CAL by C�O but not by C�C 46,47,50 and weakening of alkenyl C−H on the surface of α-MoC 1−x . It has been regarded as the most selective adsorption mode of CAL for the hydrogenation of unsaturated C�O groups.…”

Section: Spectroscopic Measurementsmentioning

confidence: 99%

Accelerating Semihydrogenation of Cinnamaldehyde by Water over a Au/α-MoC Catalyst

Lu,

Chen,

Zhang

et al. 2024

ACS Catal.

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“…Selective hydrogenation of carbonyl against the conjugated alkenyl group in unsaturated aldehydes is regarded as a critical chemical transformation for the production of fine chemicals and pharmaceutical agents. − However, as a multipath reaction, selective hydrogenation of unsaturated aldehydes to unsaturated alcohols is challenged by the unfavorable thermodynamics and kinetics of carbonyl group hydrogenation relative to the alkenyl group. − Several structure design strategies on metal catalysts have been reported, including particle size regulation, alloying strategy, and surface modification, which were demonstrated as effective ways to improve chemoselectivity but suffered from largely decreased activity. − Achieving high chemoselectivity and activity simultaneously represents a great challenge. In addition, the industrial production of unsaturated alcohols has been conducted exclusively in the organic phase; − and the application of water rather than conventional organic solvents is also a critical issue considering the benefits to the economy and environment as well as the simplification of postproduction.…”

Section: Introductionmentioning

confidence: 99%

Highly Selective Hydrogenation of Unsaturated Aldehydes in Aqueous Phase

Zhou,

Yang,

Shen

et al. 2024

ACS Appl. Mater. Interfaces

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Chemoselective hydrogenation of carbonyl in unsaturated aldehydes is a significant process in the chemical industry, in which the development of aqueous-phase reaction systems as a substitution to organic ones is challenging. Herein, we report Ir atomic cluster catalysts anchored onto WO 3−x nanorods via a reduction treatment at various temperatures (denoted as Ir/WO x -T, T = 200, 300, 400, and 500 °C), which accelerates the chemoselective hydrogenation of carbonyl groups in aqueous solutions. The optimal catalyst Ir/WO x -300 exhibits exceptional activity (TOF value: 1313.7 min −1 ) and chemoselectivity toward cinnamaldehyde (CAL) hydrogenation to cinnamyl alcohol (COL) (yield: ∼98.0%) in water medium, which is, to the best of our knowledge, the highest level compared with previously reported heterogeneous catalysts in liquid-phase reaction. Ac-HAADF-STEM, XAFS, and XPS verify the formation of interface structure (Ir δ+ −O v −W 5+ (0 ≤ δ ≤ 4); O v denotes oxygen vacancy) induced by metal−support interaction and the largest concentration of interfacial Ir (Ir δ+ ) in Ir/WO x -300. In situ studies (Raman, FT-IR), isotopic labeling measurements combined with DFT calculations substantiate that the hydrogenation of the C=O group consists of two pathways: water-mediated hydrogenation (predominant) and direct hydrogenation via H 2 dissociation (secondary). In the former case, W 5+ −O v site accelerates the activation adsorption of H 2 O, while Ir 0 site facilitates the H−H bond cleavage of H 2 and Ir δ+ promotes the CAL adsorption. H 2 O molecule, as the source of hydrogen species, participates directly in the hydrogenation of the carbonyl group through a hydrogenbonded network, with a largely reduced energy barrier relative to the H 2 dissociation path. This work demonstrates a green catalytic route that breaks the activity-selectivity trade-off toward the selective hydrogenation of unsaturated aldehydes, which shows great potential in heterogeneous catalysis.

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Fabrication of highly oxidized Pt single-atom catalysts to suppress the deep hydrogenation of unsaturated aldehydes

Cited by 18 publications

References 62 publications

Single-Atom Metal Catalysts for Catalytic Chemical Conversion of Biomass to Chemicals and Fuels

Single-Atom Metal Catalysts for Catalytic Chemical Conversion of Biomass to Chemicals and Fuels

Accelerating Semihydrogenation of Cinnamaldehyde by Water over a Au/α-MoC Catalyst

Highly Selective Hydrogenation of Unsaturated Aldehydes in Aqueous Phase

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