Significantly accelerated photochemical and photocatalytic reactions in microdroplets

Li, Kejian; Gong, Kedong; Liu, Juan; Ohnoutek, Lukáš; Ao, Jianpeng; Liu, Yangyang; Chen, Xi; Xu, Guanjun; Ruan, Xuejun; Cheng, Heyong; Han, Jin; Sui, Guodong; Ji, Minbiao; Valev, Ventsislav K.; Zhang, Liwu

doi:10.1016/j.xcrp.2022.100917

Cited by 23 publications

(39 citation statements)

References 56 publications

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“…In addition, the details about the proof-of-concept of the large-scale application of microdroplet photoreaction are also described. Regarding the organics oxidation by Fe(III)-oxalate photochemistry and by g-C 3 N 4 photocatalysis in microdroplets, the expected results would be almost consistent with our previous report on Cell Reports Physical Science ( Li et al., 2022 ), and some expected outcomes list below.…”

Section: Expected Outcomessupporting

confidence: 90%

“…Meanwhile, the photoreactions in cloud and fog droplets also play significant roles in atmospheric chemistry and global climate. With these considerations in mind, we have reported that microdroplet reactor shows great accelerations on photochemistry and photocatalysis compared to the bulk phase counterpart ( Li et al., 2022 ). Herein, in this protocol, we detail the specific steps for investigating the microdroplet photoreaction at an individual droplet level, including the preparation of superhydrophobic substrate, microdroplets generation, in-situ Raman measurements, data analysis, and proof-of-concept of the large-scale application of microdroplet photoreaction.…”

Section: Before You Beginmentioning

confidence: 99%

“…Unless otherwise stated, the experimental conditions were: FeCl 3 , 1 mM; Na 2 C 2 O 4 , 7 mM; MO, 350 mg L −1 ; initial pH, 4.75; Xe lamp irradiation, ∼35.7 mW cm −2 . Data were adopted with changes from ( Li et al, 2022 ). …”

Section: Expected Outcomesmentioning

confidence: 99%

“…In addition, we show the operational details of preliminary scale-up tests of microdroplet photoreaction for practical application. For complete details on the use and execution of this protocol, please refer to Li et al. (2022) .…”

mentioning

confidence: 99%

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A protocol to study microdroplet photoreaction at an individual droplet level using in situ micro-Raman spectroscopy

Wang

Liu

et al. 2022

STAR Protocols

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Section: Expected Outcomessupporting

confidence: 90%

Section: Before You Beginmentioning

confidence: 99%

Section: Expected Outcomesmentioning

confidence: 99%

mentioning

confidence: 99%

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A protocol to study microdroplet photoreaction at an individual droplet level using in situ micro-Raman spectroscopy

Wang

Liu

et al. 2022

STAR Protocols

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“…Solar light-driven photocatalytic conversion of CO2 into valuable derivatives (e.g. CH4, CH3OH, and HCOOH) is a promising route for renewable energy production and carbon neutrality [5][6][7][8][9][10] . However, photocatalytic CO2 reduction reaction (CO2RR) suffers from several limitations including rapid photogenerated charge carriers recombination, poor CO2 adsorption, and sluggish CO2 transfer capacity in water [11][12][13] , which largely constrain its wide applications on the industrial scale.…”

Section: Introductionmentioning

confidence: 99%

Significant Acceleration of Photocatalytic CO2 Reduction to HCOOH at Gas-Liquid Interface

Liu

Li³

et al. 2022

Preprint

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Solar‐driven CO2 reduction reaction (CO2RR) is largely constrained by the sluggish mass transfer and fast combination of photogenerated charge carriers. Herein, we find that the photocatalysis CO2RR efficiency at the abundant gas-liquid interface provided by microdroplets is two orders of magnitude higher than that of the corresponding bulk phase reaction. Even in the absence of sacrificial agents, the production rate of HCOOH over WO3·0.33H2O mediated by microdroplets reaches 2536.23 μmol h-1g-1 (vs. 13.32 μmol h-1g-1 in bulk phase), which is significantly superior to the previously reported photocatalysis CO2RR in bulk phase water. Beyond the efficient delivery of CO2 to photocatalyst surfaces within microdroplets, we reveal that the strong electric field at the gas-liquid interface of microdroplets essentially promotes the separation of photogenerated electron-hole pairs. A scalable HCOOH photocatalysis production is further demonstrated by using an electric nebulizer to generate a large number of microdroplets. This study provides a deep understanding of ultrafast reaction kinetics mediated by the gas-liquid interface of microdroplets and a novel way of addressing the low efficiency of photocatalytic CO2 reduction.

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Significant Acceleration of Photocatalytic CO₂ Reduction at the Gas‐Liquid Interface of Microdroplets**

Liu

et al. 2023

Angewandte Chemie

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Solar‐driven CO2 reduction reaction (CO2RR) is largely constrained by the sluggish mass transfer and fast combination of photogenerated charge carriers. Herein, we find that the photocatalytic CO2RR efficiency at the abundant gas‐liquid interface provided by microdroplets is two orders of magnitude higher than that of the corresponding bulk phase reaction. Even in the absence of sacrificial agents, the production rates of HCOOH over WO3 ⋅ 0.33H2O mediated by microdroplets reaches 2536 μmol h−1 g−1 (vs. 13 μmol h−1 g−1 in bulk phase), which is significantly superior to the previously reported photocatalytic CO2RR in bulk phase reaction condition. Beyond the efficient delivery of CO2 to photocatalyst surfaces within microdroplets, we reveal that the strong electric field at the gas‐liquid interface of microdroplets essentially promotes the separation of photogenerated electron‐hole pairs. This study provides a deep understanding of ultrafast reaction kinetics promoted by the gas‐liquid interface of microdroplets and a novel way of addressing the low efficiency of photocatalytic CO2 reduction to fuel.

show abstract

Significantly accelerated photochemical and photocatalytic reactions in microdroplets

Cited by 23 publications

References 56 publications

A protocol to study microdroplet photoreaction at an individual droplet level using in situ micro-Raman spectroscopy

A protocol to study microdroplet photoreaction at an individual droplet level using in situ micro-Raman spectroscopy

Significant Acceleration of Photocatalytic CO2 Reduction to HCOOH at Gas-Liquid Interface

Significant Acceleration of Photocatalytic CO₂ Reduction at the Gas‐Liquid Interface of Microdroplets**

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Significantly accelerated photochemical and photocatalytic reactions in microdroplets

Cited by 23 publications

References 56 publications

A protocol to study microdroplet photoreaction at an individual droplet level using in situ micro-Raman spectroscopy

A protocol to study microdroplet photoreaction at an individual droplet level using in situ micro-Raman spectroscopy

Significant Acceleration of Photocatalytic CO2 Reduction to HCOOH at Gas-Liquid Interface

Significant Acceleration of Photocatalytic CO2 Reduction at the Gas‐Liquid Interface of Microdroplets**

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Product

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Significant Acceleration of Photocatalytic CO₂ Reduction at the Gas‐Liquid Interface of Microdroplets**