Ligand functionalization on Zr-MOFs enables efficient visible-light-driven H<sub>2</sub>O<sub>2</sub>evolution in pure water

Qiu, Jianhao; Zhang, Lu; Xia, Guanglu; Dai, Dingliang; Tang, Yonghong; Yao, Jianfeng

doi:10.1039/d3cy00130j

Cited by 20 publications

(16 citation statements)

References 39 publications

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“…Meanwhile, the highest occupied molecular orbital (HOMO) potential of ZIF-8-NH 2 and valence band (VB) potential of Bi 2 MoO 6 were determined as 3.1 and 1.7 eV according to their corresponding HOMO and VB XPS spectra, respectively (Figure 3c). Since the potentials of the conduction band (CB) or lowest unoccupied molecular orbital (LUMO) are estimated by E CB or LUMO = E VB or HOMO − E g , 28 the CB potential of Bi 2 MoO 6 and LUMO potential of ZIF-8-NH 2 correspond to −1 and −0.6 eV, respectively. Consequently, the band configurations of ZIF-8-NH 2 and Bi 2 MoO 6 were illustrated in Figure 3d.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Defect Engineering Promoted Photocatalysis for Lignin Depolymerization: Performance and Mechanism Insight

Dai,

Qiu,

Xia

et al. 2023

ACS Catal.

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Defect engineering has shown a pronounced promise in photocatalysis. In this study, ZIF-8-NH2@Bi/Bi2MoO6 with oxygen vacancies was elaborately developed for efficient Cβ–O bond cleavage of a typical lignin model, 2-phenoxy-1-phenylethanol (PP-ol) and alkali lignin. The surface plasmon resonance effect of Bi nanoparticles, the heterojunction between ZIF-8-NH2 and Bi2MoO6, and the Schottky junction between Bi and Bi2MoO6 together facilitate charge separation and transfer. More significantly, the oxygen vacancy could efficiently facilitate O2 capture and activation to generate 1O2 that acts as a dominant role in promoting Cβ–O bond cleavage while holes could only convert PP-ol into 2-phenoxy-1-acetophenone. As a result, 93% of PP-ol was converted into phenol and acetophenone (AP) with yields of 57% and 48%, respectively, over ZIF-8-NH2@Bi/Bi2MoO6 in air, which is obviously higher than those over ZIF-8-NH2@Bi2MoO6 (46% of PP-ol conversion, 8.7% of phenol yield and 6.2% of AP yield). Moreover, in a pure O2 environment, 100% of PP-ol conversion, 69% of phenol yield, and 68% of AP yield could be achieved. As for alkali lignin extracted from Pinus massoniana, a high vanillin yield of 25 mg/glignin could be obtained with Cβ–O bond cleavage. This work could offer an in-depth insight into catalyst design as well as photocatalytic valorization of biomass.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Defect Engineering Promoted Photocatalysis for Lignin Depolymerization: Performance and Mechanism Insight

Dai,

Qiu,

Xia

et al. 2023

ACS Catal.

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“…The H 2 O 2 concentration was determined through iodometry measured by a UV spectrophotometer at 350 nm. 22 For the recycling test, the used photocatalysts were filtered (directly taken out from the reaction liquid for TpTt-COF/MS), washed with N,Ndimethylformamide and dimethyl sulfoxide, and finally dried at 80 C overnight. The apparent quantum yield (AQY) was calculated at different wavelengths (360, 420, 550, and 650 nm) using Equation ( 1):…”

Section: Photocatalytic Activity Measurementsmentioning

confidence: 99%

Electron‐deficient covalent organic frameworks anchored on melamine sponges for visible‐light‐driven H₂O₂ evolution

et al. 2023

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A series of covalent organic frameworks (COFs) with β‐ketoenamine linkages named TpTt‐COF, TAPT‐COF, and TpPa‐1 were constructed for photocatalytic H2O2 generation in pure water and ambient air under visible light. Among them, TpTt‐COF performed striking H2O2 yield of 2647 μmol L−1, which is 3.5, 17.5, and 176.5‐fold those of TAPT‐COF, TpPa‐1, and bulk g‐C3N4, respectively, attributing to the electron‐deficient trait, short charge diffusion distance, and the narrowest bandgap of TpTt‐COF. Additionally, to achieve the facile recovery, TpTt‐COF was firmly and evenly anchored on melamine sponges (MS) because plenty of amino groups on the surface of MS could be involved in the β‐ketoenamine formation and guide the synthesis of TpTt‐COF on MS. The corresponding H2O2 evolution over this photocatalyst monolith is also respectable and can be well repeated at least four times. This work is quite instructive for photocatalyst construction based on covalent organic frameworks and facile photocatalytic applications.

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“…[33][34][35] However, the pure water reaction system is the real sense of photosynthesis, which extremely depends on the stability and band structure of the catalyst and is rarely used in the field of MOF photocatalysts, especially for Ti MOFs. 19,[36][37][38] To date, only MOF-based composites have been applied in the two-phase system including MeCN/H 2 O and 1-octanol/benzyl alcohol (BnOH), and have performed higher photocatalytic activities for H 2 O 2 and benzaldehyde (BzN) production. 39,40 In addition, compared with the single-phase system, the stratified two-phase reaction system is easier to extract the product.…”

Section: Photocatalytic Systemsmentioning

confidence: 99%

Metal–organic frameworks for the photocatalytic oxygen reduction reaction to hydrogen peroxide

Wang

Teishima

2023

Mater. Chem. Front.

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Ligand functionalization on Zr-MOFs enables efficient visible-light-driven H₂O₂evolution in pure water

Abstract: Different ligand functionalized UiO-66 (UiO-66-X, X = OH, (OH)2 and NH2) was prepared and then modified by ZnIn2S4 lamellas to form ZnIn2S4/UiO-66-X heterostructures for visible-light-driven H2O2 evolution in pure water....

Cited by 20 publications

References 39 publications

Defect Engineering Promoted Photocatalysis for Lignin Depolymerization: Performance and Mechanism Insight

Defect Engineering Promoted Photocatalysis for Lignin Depolymerization: Performance and Mechanism Insight

Electron‐deficient covalent organic frameworks anchored on melamine sponges for visible‐light‐driven H₂O₂ evolution

Metal–organic frameworks for the photocatalytic oxygen reduction reaction to hydrogen peroxide

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Ligand functionalization on Zr-MOFs enables efficient visible-light-driven H2O2evolution in pure water

Abstract: Different ligand functionalized UiO-66 (UiO-66-X, X = OH, (OH)2 and NH2) was prepared and then modified by ZnIn2S4 lamellas to form ZnIn2S4/UiO-66-X heterostructures for visible-light-driven H2O2 evolution in pure water....

Cited by 20 publications

References 39 publications

Defect Engineering Promoted Photocatalysis for Lignin Depolymerization: Performance and Mechanism Insight

Defect Engineering Promoted Photocatalysis for Lignin Depolymerization: Performance and Mechanism Insight

Electron‐deficient covalent organic frameworks anchored on melamine sponges for visible‐light‐driven H2O2 evolution

Metal–organic frameworks for the photocatalytic oxygen reduction reaction to hydrogen peroxide

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Product

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Ligand functionalization on Zr-MOFs enables efficient visible-light-driven H₂O₂evolution in pure water

Electron‐deficient covalent organic frameworks anchored on melamine sponges for visible‐light‐driven H₂O₂ evolution