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学者姓名：吴棱
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Abstract ：
Here, the mixed metal nodes MOFs, Pd/MIL-100(FeaCub), were constructed as photocatalysts for hydrogenation of alpha,beta-unsaturated aldehyde (UAL) under visible light. 1 wt% Pd/MIL-100(Fe0.81Cu0.19) can convert a range of UAL to saturated aldehydes (SAL) with a high efficiency (approximate to 100 %) and selectivity (approximate to 98 %). The results of XPS and in situ DRIFTS reveal that UAL can be selectively activated via a coordination of -C--C- on Cu2+ sites, determining the high selectivity of the photocatalytic reaction. The mixed metal nodes and Pd clusters can improve the transformation and separation of photogenerated electrons-holes. EPR result suggests that photogenerated carriers can facilitate the generation of H center dot on Pd/MIL-100(Fe0.81Cu0.19), enhancing the catalytic activity. A possible mechanism is proposed for elucidating the catalytic processes at the molecular level. This work provides a valuable strategy for tailoring the selectivity of photocatalytic hydrogenation via selective coordination activation.
Keyword ：
alpha alpha beta-Unsaturated aldehydes beta-Unsaturated aldehydes Coordination activation Coordination activation Hydrogenation Hydrogenation MIL-100(Fe/Cu) MIL-100(Fe/Cu) Photocatalyst Photocatalyst
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| GB/T 7714 | Wang, Zhiwen , Kang, Yueyue , Shi, Yingzhang et al. Selective coordination activation regulating the selectivity for photocatalytic hydrogenation of α,β-unsaturated aldehyde over Pd/ MIL-100(FeaCub) [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2024 , 340 . |
| MLA | Wang, Zhiwen et al. "Selective coordination activation regulating the selectivity for photocatalytic hydrogenation of α,β-unsaturated aldehyde over Pd/ MIL-100(FeaCub)" . | APPLIED CATALYSIS B-ENVIRONMENTAL 340 (2024) . |
| APA | Wang, Zhiwen , Kang, Yueyue , Shi, Yingzhang , Liu, Cheng , Liu, Yunni , Lin, Jun et al. Selective coordination activation regulating the selectivity for photocatalytic hydrogenation of α,β-unsaturated aldehyde over Pd/ MIL-100(FeaCub) . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2024 , 340 . |
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Photocatalytic N2 fixation is a green process for ammonia synthesis by converting N2 and H2O to NH3 and O2 directly using solar energy. Its efficiency is largely limited by the chemisorption and activation of N2. This work adopts defect engineering strategy to develop a series of MIL-68(Fe) MOFs with varying concentrations of defects by doping Cu2+ on the metal nodes of MOFs. Upon Cu2+ doping, a larger number of oxygen vacancy defects are created due to the induced crystal distortion to form coordinatively unsaturated Fe2+ sites, which can serve as the active sites for promoting the chemisorption and activation of N2. The photogenerated holes oxidize H2O to O2 and H+, and the photogenerated electrons combine with formed H+ to reduce the activated N2 to NH3. It was found that the sample with 10 mol% Cu2+ doping shows the highest NH3 production rate (21.0 mu mol center dot g- 1 center dot h-1), which is 8.4 times higher than that (2.50 mu mol center dot g- 1 center dot h-1) of the pristine MIL-68(Fe). The excellent performance is ascribed to the adequate Fe2+ active sites to chemisorb and activate N2 and the optimal mobility of photogenerated charges. Finally, a mechanism is proposed to illustrate how the number of defects affects the photocatalytic N2 fixation performance at the molecular level.
Keyword ：
Active sites Active sites Defect engineering Defect engineering MIL-68(Fe) MIL-68(Fe) N2 fixation N2 fixation Photocatalysis Photocatalysis
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| GB/T 7714 | Zhang, Zewei , Liu, Cheng , Chen, Yueling et al. Defect modulation of MIL-68(Fe) MOFs by Cu doping for boosting photocatalytic N 2 fixation [J]. | JOURNAL OF CATALYSIS , 2024 , 432 . |
| MLA | Zhang, Zewei et al. "Defect modulation of MIL-68(Fe) MOFs by Cu doping for boosting photocatalytic N 2 fixation" . | JOURNAL OF CATALYSIS 432 (2024) . |
| APA | Zhang, Zewei , Liu, Cheng , Chen, Yueling , Chen, Qi , Shi, Yingzhang , Wang, Zhiwen et al. Defect modulation of MIL-68(Fe) MOFs by Cu doping for boosting photocatalytic N 2 fixation . | JOURNAL OF CATALYSIS , 2024 , 432 . |
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Heterogeneous photocatalytic degradation of antibiotic involves the activation of antibiotic molecules and the photocatalytic oxidation process. However, the simultaneous improvement of these processes is still a challenge. Herein, S-scheme heterojunctions consisted of Cu2O nanocluster with defective WO3 nanosheets were constructed for efficient photocatalytic degradation of levofloxacin (LVX). The typical CNS-5 composite (5 wt% Cu2O/WO3) achieves an optimal LVX degradation efficiency of 97.9% within 80 min. The spatial charge separation and enhancement of redox capacity were realized by the formation of S-scheme heterojunction between Cu2O and WO3. Moreover, their interfacial interaction would lead to the loss of lattice oxygen and the generation of W5+ sites. It is witnessed that the C–N of piperazine ring and C[dbnd]O of carboxylic acid in LVX are coordinated with W5+ sites to build the electronic bridge to activate LVX, greatly promoting the further degradation. This work highlights the important role of selective coordination activation cooperated with S-type heterojunctions for the photocatalytic degradation and offers a new view to understand the degradation of antibiotics at molecular level. © 2024 Elsevier Ltd
Keyword ：
Coordination activation Coordination activation Cu2O/WO3 S-Scheme heterojunction Cu2O/WO3 S-Scheme heterojunction Interfacial interaction Interfacial interaction Levofloxacin photodegradation Levofloxacin photodegradation
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| GB/T 7714 | Chen, Q. , Hu, L. , Shi, Y. et al. Cu2O/WO3 S-scheme heterojunctions for photocatalytic degradation of levofloxacin based on coordination activation [J]. | Chemosphere , 2024 , 352 . |
| MLA | Chen, Q. et al. "Cu2O/WO3 S-scheme heterojunctions for photocatalytic degradation of levofloxacin based on coordination activation" . | Chemosphere 352 (2024) . |
| APA | Chen, Q. , Hu, L. , Shi, Y. , Liu, C. , Hou, Y. , Bi, J. et al. Cu2O/WO3 S-scheme heterojunctions for photocatalytic degradation of levofloxacin based on coordination activation . | Chemosphere , 2024 , 352 . |
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Defect engineering in metal organic frameworks (MOFs) has captured significant attention in the field of photocatalysis. A series of UiO-66(Ce) (UiO = University of Oslo) MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine (BA) and thioanisole (TA) under visible light. The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce3+ content. It also generates a high concentration of oxygen vacancies. In situ Fourier transform infrared spectroscopy (FTIR) results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H-NCe and the C-SCe interactions, respectively. Simulated in situ electron paramagnetic resonance (EPR) data indicate that O-2 activation and reduction occur at coordinatively unsaturated Ce3+ sites to form O-2(-). This is accelerated by the Ce3+/Ce4+ redox cycle associated with the photogenerated electrons. The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA. The most active sample exhibits 98.4% and 95.5% conversion rates for BA and TA oxidation. Mechanisms for the molecular activation are proposed at the molecular level.
Keyword ：
Ce3+/Ce4+ redox cycling Ce3+/Ce4+ redox cycling Defective MOFs Defective MOFs Molecular activation Molecular activation Photocatalytic selective organic oxidation Photocatalytic selective organic oxidation UiO-66(Ce) UiO-66(Ce)
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| GB/T 7714 | Liu, Cheng , Shi, Ying-Zhang , Chen, Qi et al. The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations [J]. | RARE METALS , 2024 . |
| MLA | Liu, Cheng et al. "The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations" . | RARE METALS (2024) . |
| APA | Liu, Cheng , Shi, Ying-Zhang , Chen, Qi , Ye, Bing-Hua , Bi, Jin-Hong , Yu, Jimmy C. et al. The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations . | RARE METALS , 2024 . |
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The efficient removal of highly toxic polyhalogenated biphenyls is rather challenging, mainly due to the difficulties in splitting C-X (X = Cl or Br) bond with high bond energy, as well as the transfer of active hydrogen species during the reduction dehalogenation process. In this work, sub-nanometer Pd-Pt alloy clusters (ca. 1 nm) supported on defect-containing TiO2(B) nanosheets (PdPt/TB), on absorption of visible light illumination (lambda > 400 nm), were prepared and served as an efficient photocatalysts for dehalogenation of polyhalogenated biphenyls with H2O as the hydrogen source. An optimal sample (Pd0.7Pt0.3/TB) shows the highest photocatalytic dehalogenation efficiency for 3,3 ',4,4 '-trtrachlorobiphenyl (PCB77) within 30 mins, which is 12.5, 3.5 and 3 times higher than that of Pt-1/TB, Pd-1/TB, and Pd-0.7 + Pt-0.3/TB samples, respectively. Besides, 4,4 '-dibromobiphenyl (PBB15) was also completely removed within 10 mins by using Pd0.7Pt0.3/TB photocatalyst, demonstrating its potential applications. Experiments and d-band theory calculations revealed that the introduction of Pt can regulate the d-band center of Pd to strength the interaction between active hydrogen with alloy and promote the transfer of hydrogen species. Meanwhile, Pd-Pt alloy is conducive to activate the C-X bond of polyhalogenated biphenyls. Finally, a mechanism based on Pd-Pt alloy clusters synergistic interaction is proposed at the molecular level. This work demonstrates the successful synthesis of sub-nanometer Pd-Pt alloy nanoclusters and elucidates the effect of interaction among Pd, Pt and supports, providing an efficient method for the removal of polyhalogenated compounds by photocatalytic technology.
Keyword ：
d -band center d -band center Pd-Pt alloy Pd-Pt alloy Photocatalysis Photocatalysis Polyhalogenated biphenyls Polyhalogenated biphenyls Sub-nanometer cluster Sub-nanometer cluster
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| GB/T 7714 | Li, Dexuan , Liu, Cheng , Huang, Danlei et al. Optimizing the d-band center of sub-nanometer Pd-Pt alloy clusters for improved photocatalytic dehalogenation of polyhalogenated biphenyls [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 342 . |
| MLA | Li, Dexuan et al. "Optimizing the d-band center of sub-nanometer Pd-Pt alloy clusters for improved photocatalytic dehalogenation of polyhalogenated biphenyls" . | SEPARATION AND PURIFICATION TECHNOLOGY 342 (2024) . |
| APA | Li, Dexuan , Liu, Cheng , Huang, Danlei , Wu, Ling , Li, Chuanhao , Guo, Wei . Optimizing the d-band center of sub-nanometer Pd-Pt alloy clusters for improved photocatalytic dehalogenation of polyhalogenated biphenyls . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 342 . |
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Covalent organic frameworks (COFs) with excellent structural tunability have emerged as fascinating photocatalysts to fulfill future energy demands. Here, we developed a COFs heterostructure by assembling two COFs for photocatalytic overall water splitting. The resulting heterostructure exhibited an effective spatial separation of photoredox sites originating from the efficient separation of photoinduced charge carriers through an orientated interfacial electron transfer pathway. Accordingly, the heterostructure of the COFs displays excellent activity for stoichiometric water splitting into H-2 and O-2 under 5 W white LED light irradiation. Our efficiencies of H-2 and O-2 evolution rates up to 120 and 58 mu mol g(-1) h(-1) are significantly higher than those reported previously. The combination of experiments and theoretical calculations shows that water oxidation proceeds by a metal-free hydration-mediated pathway. This work sheds light on a rational design of the COF heterostructure with spatially separated photoredox for water splitting.
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| GB/T 7714 | Niu, Qing , Chen, Wei , Pan, Guodong et al. Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting [J]. | ACS MATERIALS LETTERS , 2024 , 6 (4) : 1411-1417 . |
| MLA | Niu, Qing et al. "Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting" . | ACS MATERIALS LETTERS 6 . 4 (2024) : 1411-1417 . |
| APA | Niu, Qing , Chen, Wei , Pan, Guodong , Li, Liuyi , Yu, Yan , Bi, Jinhong et al. Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting . | ACS MATERIALS LETTERS , 2024 , 6 (4) , 1411-1417 . |
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Adsorption and activation of C-H bonds by photocatalysts are crucial for the efficient conversion of C-H bonds to produce high-value chemicals. Nevertheless, the delivery of surface-active oxygen species for C-H bond oxygenation inevitably needs to overcome obstacles due to the separated active centers, which suppresses the catalytic efficiency. Herein, Ni dopants are introduced into a monolayer Bi2WO6 to create cascaded active units consisting of unsaturated W atoms and Bi/O frustrated Lewis pairs. Experimental characterizations and density functional theory calculations reveal that these special sites can establish an efficient and controllable C-H bond oxidation process. The activated oxygen species on unsaturated W are readily transferred to the Bi/O sites for C-H bond oxygenation. The catalyst with a Ni mass fraction of 1.8% exhibits excellent toluene conversion rates and high selectivity towards benzaldehyde. This study presents a fascinating strategy for toluene oxidation through the design of efficient cascaded active units.
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| GB/T 7714 | Shi, Yingzhang , Li, Peng , Chen, Huiling et al. Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers [J]. | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
| MLA | Shi, Yingzhang et al. "Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers" . | NATURE COMMUNICATIONS 15 . 1 (2024) . |
| APA | Shi, Yingzhang , Li, Peng , Chen, Huiling , Wang, Zhiwen , Song, Yujie , Tang, Yu et al. Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers . | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
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A series of Al3+-doped UiO-66(Ce) MOFs (U(CexAl1−x)) was developed to reveal the roles of metal doping on active site formation and substrate activation in photocatalytic selective transformation of amines to imines. Al3+ doping induced crystal structure distortion to form coordinately unsaturated metal (Al, Ce) sites as Lewis acid sites to chemisorb and activate benzylamine (BA). In situ FTIR revealed that the Al site with stronger acid strength facilitated BA activation. The activation degree of N–H bonds in BA was evaluated by changes of calculated force constant. The intermediate products were confirmed through time-dependent in situ FTIR. The Al3+-doped sample U(Ce0.90Al0.10), the optimal catalyst, showed a significantly increased BA conversion (97.6 %) than that (47.5 %) of undoped sample, which was attributed to enough active sites and the optimal charge mobility. Finally, the present study proposes a synergistic photocatalytic mechanism associated with molecular activation to demonstrate selective oxidation pathways at the molecular level. © 2024 Elsevier Inc.
Keyword ：
Active sites Active sites Metal doping Metal doping Photocatalysis Photocatalysis UiO-66(Ce) UiO-66(Ce)
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| GB/T 7714 | Liu, C. , Chen, H. , Chen, Q. et al. Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis [J]. | Journal of Catalysis , 2024 , 437 . |
| MLA | Liu, C. et al. "Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis" . | Journal of Catalysis 437 (2024) . |
| APA | Liu, C. , Chen, H. , Chen, Q. , Bi, J. , Yu, J.C. , Wu, L. . Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis . | Journal of Catalysis , 2024 , 437 . |
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Designing efficient metal organic frameworks (MOF)-based photocatalysts has recently attracted wide attention. In this work, Au nanoparticles (NPs)-decorated defective DUT-67(Zr) (Au@DUT-67(Zr)) with enlarged channels was successfully fabricated and achieved 7.5 times higher conversion than Au NPs -decorated UiO-66(Zr) (Au@UiO-66(Zr)) for photocatalytic selective oxidation of amines to imines driven by visible light. Au NPs are more effectively fixed on DUT-67(Zr) due to its partially hollow structure. Au@DUT-67(Zr) possesses more active sites including unsaturated Zr atoms and oxygen vacancies (VO) than Au@UiO-66(Zr). In situ Fourier transform infrared (FTIR) spectrum reveals that benzylamine is acti-vated on unsaturated Zr sites via HAN...Zr species, facilitating deprotonation of -CH2 in benzylamine. VO can not only adsorb and activate oxygen (O-2) but also capture plasmonic hot electrons, enhancing the forming of superoxide radical (O-.(2)). Plasmonic hot holes assisted with center dot O(2)effectively achieve the selective oxidation of benzylamine. Finally, a possible synergetic mechanism combining the plasmon with the molecular activation is presented to illustrate the photocatalytic pathway at the molecular level. (c) 2022 Elsevier Inc. All rights reserved.
Keyword ：
Active site Active site DUT-67(Zr) DUT-67(Zr) Molecular activation Molecular activation Oxygen vacancy Oxygen vacancy Photocatalysis Photocatalysis Plasmon Plasmon
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| GB/T 7714 | Liu, Cheng , Liu, Yanyang , Shi, Yingzhang et al. Au nanoparticles-anchored defective metal-organic frameworks for photocatalytic transformation of amines to imines under visible light [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 631 : 154-163 . |
| MLA | Liu, Cheng et al. "Au nanoparticles-anchored defective metal-organic frameworks for photocatalytic transformation of amines to imines under visible light" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 631 (2023) : 154-163 . |
| APA | Liu, Cheng , Liu, Yanyang , Shi, Yingzhang , Wang, Zhiwen , Guo, Wei , Bi, Jinhong et al. Au nanoparticles-anchored defective metal-organic frameworks for photocatalytic transformation of amines to imines under visible light . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 631 , 154-163 . |
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ZnIn2S4 ultrathin 2D nanosheets with a positive surface charge are synthesized by a hydrothermal method and different contents of surface S vacancies are induced via heat treatment of as-prepared ZnIn2S4 (ZIS). As the S vacancies contents increased, the photocatalytic degradation efficiency of ceftriaxone (CTRX) sodium is promoted. Especially, ZIS-300 shows the best degradation efficiency (88.8%) for an initial CTRX concentration of 10 mg L-1 in 2 h. It is found that S vacancies cause the electron density of surface metal atoms (Zn, In) to be decreased, which makes the effective adsorption and activation of ceftriaxone anions through electrostatic adsorption interactions. Meanwhile, S vacancies also serve as active centers to promote the absorption of O-2 and gather electrons to form center dot O-2(-) species. The photogenerated holes quickly transfer to the surface of the catalyst to directly degrade the adsorbed CTRX. Thus, the photocatalytic CTRX degradation efficiency is significantly improved. Finally, a possible mechanism for over defective ZIS is proposed. This work provides a feasible strategy for the efficient degradation of antibiotics from the perspective of electrostatic adsorption and molecule activation.
Keyword ：
Electrostatic interaction Electrostatic interaction O-2 activation O-2 activation S vacancies S vacancies The degradation of ceftriaxone sodium The degradation of ceftriaxone sodium ZnIn2S4 ultrathin Nanosheets ZnIn2S4 ultrathin Nanosheets
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| GB/T 7714 | Zhang, Chen , Shi, Yingzhang , Wang, Zhiwen et al. Electrostatic interaction and surface S vacancies synergistically enhanced the photocatalytic degradation of ceftriaxone sodium [J]. | CHEMOSPHERE , 2023 , 311 . |
| MLA | Zhang, Chen et al. "Electrostatic interaction and surface S vacancies synergistically enhanced the photocatalytic degradation of ceftriaxone sodium" . | CHEMOSPHERE 311 (2023) . |
| APA | Zhang, Chen , Shi, Yingzhang , Wang, Zhiwen , Liu, Cheng , Hou, Yidong , Bi, Jinhong et al. Electrostatic interaction and surface S vacancies synergistically enhanced the photocatalytic degradation of ceftriaxone sodium . | CHEMOSPHERE , 2023 , 311 . |
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