Selective oxidation of ethyl lactate to ethyl pyruvate by a photocatalytic strategy under room temperature

Lu, Tianliang; Yang, Zhiyun; Li, Hongji; Chen, Haijun; Xu, Jun; Xu, Chunbao; Wang, Jianshe; Li, Zhongjun; Zhang, Yongsheng

doi:10.1016/j.jcat.2022.04.020

Cited by 17 publications

(4 citation statements)

References 56 publications

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“…All the products were characterized by GC-MS. The structure of some products was further confirmed by NMR, which showed constant results with previous reports. − All of these spectroscopy analyses are provided in the Supporting Information. The above experiments verify that the V M -BMO catalyst can be used for other hydroxyl compounds, indicating the generality of the photocatalytic system.…”

Section: Resultssupporting

confidence: 81%

“…It is speculated that 1 O 2 is the final oxidation species while • O 2 – is the intermediate for the production of 1 O 2 , since the latter can be generated from the oxidation of • O 2 – by holes, which also precludes the possibility of the energy transfer mechanism through an intersystem crossing process . This is similar to the photocatalytic oxidation mechanism over ZnIn sulfide catalysts . The generation of 1 O 2 was also verified by the triple peak with an intensity ratio of 1:1:1 in the electron paramagnetic resonance (EPR) spectrum (Figure b). , The influence of Mo vacancy on the production of 1 O 2 was evaluated by the photocatalytic oxidation of anthracene, which could form endoperoxide with singlet oxygen .…”

Section: Resultsmentioning

confidence: 71%

“…53 This is similar to the photocatalytic oxidation mechanism over ZnIn sulfide catalysts. 44 The generation of 1 O 2 was also verified by the triple peak with an intensity ratio of 1:1:1 in the electron paramagnetic resonance (EPR) spectrum (Figure 5b). 54,55 The influence of Mo vacancy on the production of 1 O 2 was evaluated by the photocatalytic oxidation of anthracene, which could form endoperoxide with singlet oxygen.…”

Section: Mechanistic Insights Into the Photocatalytic Oxidation Over ...mentioning

confidence: 99%

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Subsurface Mo Vacancy in Bismuth Molybdate Promotes Photocatalytic Oxidation of Lactate to Pyruvate

Chen,

Xu,

Chen

et al. 2024

ACS Catal.

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Disclosing the role of subsurface metal defects in photocatalysts remains challenging, although defect engineering has been a fundamental method for manipulating the photocatalytic transformation performance. Herein, the subsurface Mo vacancy-rich Bi 2 MoO 6 was prepared and the role of its effects on photocatalysis was revealed. The presence of metal vacancy enhances the separation efficiency of photogenerated carriers through both the holes captured by the oxygen atoms neighboring the Mo vacancy and the generation of an internal electric field, which is revealed by experimental results and density functional theory calculations. The boosted separation efficiency of electron−hole pairs improves the generation of 1 O 2 , which is the final active species for photocatalytic oxidation of ethyl lactate. The conversion of ethyl lactate reaches to >99% over the subsurface Mo vacancy-rich Bi 2 MoO 6 after 3 h of illumination, much higher than that of bulk Bi 2 MoO 6 , which gives only 28.6%. Meanwhile, the yield of ethyl pyruvate is 90.2%, which is the highest value in heterogeneous systems using molecular oxygen as oxidant. Moreover, the catalyst is rather stable and can be applied for the selective oxidation of other hydroxyl compounds. This work unveils the role of metal defects engineering in affecting electron−hole separation, highlighting possible opportunities for highly efficient photocatalytic organic transformation.

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Section: Resultssupporting

confidence: 81%

Section: Resultsmentioning

confidence: 71%

Section: Mechanistic Insights Into the Photocatalytic Oxidation Over ...mentioning

confidence: 99%

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Subsurface Mo Vacancy in Bismuth Molybdate Promotes Photocatalytic Oxidation of Lactate to Pyruvate

Chen,

Xu,

Chen

et al. 2024

ACS Catal.

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“…As a platform chemical, the selective conversion of LA and its derivatives into high-value-added products is of great significance. [9] Herein, CdS/MoO 2 /MoS 2 hollow spheres are employed to couple photocatalytic hydrogen evolution with PA production. The one-step conversion of CdMoO 4 provides a unique synthetic route to form MoS 2 and MoO 2 dual cocatalysts simultaneously.…”

Section: Introductionmentioning

confidence: 99%

A Bifunctional CdS/MoO₂/MoS₂ Catalyst Enhances Photocatalytic H₂ Evolution and Pyruvic Acid Synthesis

et al. 2022

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The best use of photogenerated electrons and holes is crucial to boosting photocatalytic activity. Herein, a bifunctional dual‐cocatalyst‐modified photocatalyst is constructed based on CdS/MoO2/MoS2 hollow spheres for hydrogen evolution coupled with selective pyruvic acid (PA) production from lactic acid (LA) oxidation. MoS2 and MoO2 are simultaneously obtained from the conversion of CdMoO4 in one step. In a photocatalytic process, the MoS2 and MoO2 function as the reduction and oxidation centers on which photogenerated electrons and holes accumulate and are used for hydrogen evolution reaction (HER) and PA synthesis, respectively. By monitoring the intermediates, a two‐step single‐electron route for PA production is proposed, initiated by the cleavage of the α‐C(sp3)−H bond in the LA. The conversion of LA and the selectivity of PA can reach ca. 29 % and 95 % after a five‐hour reaction, respectively.

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Distinct Pathways Determined by Photocatalytic C─H or O─H Bond Activation for Hydroxyl Compounds Conversion Paired With Hydrogen Production

Li,

Zhu,

et al. 2024

Advanced Sustainable Systems

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Selective control of C─H or O─H bond activation in photocatalytic conversion coupled with hydrogen production is a promising yet challenging goal. Here, an efficient photocatalytic system is reported that can produce high‐valued tartaric acid or formaldehyde and simultaneous producing hydrogen. At optimized conditions, the directional conversion of glycolic acid into tartaric acid is achieved with a selectivity of 76.24%, and the selectivity of methanol oxidation into formaldehyde reaches 88.21%. A high hydrogen production rate of 21.43 mmol·g−1·h−1 is obtained using glycolic acid as substrate. Mechanism studies reveal that α‐C─H bond is preferentially activated in glycolic acid adsorbed on the photocatalyst, while O─H bond is preferentially activated in methanol, forming carbon‐centered radical (•CH(OH)COOH) or oxygen‐centered radical (CH3O•) for subsequent coupling or oxidation reactions. This work demonstrates the selective control of the photocatalytic conversion process of different hydroxyl compounds, providing a new perspective for achieving organic compounds selective activation coupled with hydrogen production.

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Selective oxidation of ethyl lactate to ethyl pyruvate by a photocatalytic strategy under room temperature

Cited by 17 publications

References 56 publications

Subsurface Mo Vacancy in Bismuth Molybdate Promotes Photocatalytic Oxidation of Lactate to Pyruvate

Subsurface Mo Vacancy in Bismuth Molybdate Promotes Photocatalytic Oxidation of Lactate to Pyruvate

A Bifunctional CdS/MoO₂/MoS₂ Catalyst Enhances Photocatalytic H₂ Evolution and Pyruvic Acid Synthesis

Distinct Pathways Determined by Photocatalytic C─H or O─H Bond Activation for Hydroxyl Compounds Conversion Paired With Hydrogen Production

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Selective oxidation of ethyl lactate to ethyl pyruvate by a photocatalytic strategy under room temperature

Cited by 17 publications

References 56 publications

Subsurface Mo Vacancy in Bismuth Molybdate Promotes Photocatalytic Oxidation of Lactate to Pyruvate

Subsurface Mo Vacancy in Bismuth Molybdate Promotes Photocatalytic Oxidation of Lactate to Pyruvate

A Bifunctional CdS/MoO2/MoS2 Catalyst Enhances Photocatalytic H2 Evolution and Pyruvic Acid Synthesis

Distinct Pathways Determined by Photocatalytic C─H or O─H Bond Activation for Hydroxyl Compounds Conversion Paired With Hydrogen Production

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A Bifunctional CdS/MoO₂/MoS₂ Catalyst Enhances Photocatalytic H₂ Evolution and Pyruvic Acid Synthesis