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学者姓名：吴棱
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Abstract ：
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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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 , 44 (4) : 2462-2473 . |
| MLA | Liu, Cheng et al. "The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations" . | RARE METALS 44 . 4 (2024) : 2462-2473 . |
| 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 , 44 (4) , 2462-2473 . |
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Photocatalysis, which uses sunlight, N-2 and H2O to produce NH3, is a more sustainable approach to N-2 fixation than the Haber-Bosch process. However, its efficiency is severely limited by the difficulty of activating N N bonds. This work presents metal (M = Cu, Fe, V)-substituted MIL-125(Ti) (MIL-(MTi)) for photocatalytic N-2 fixation without using any sacrificial agents. Structural characterizations reveal that the active sites including oxygen vacancies (OV) and Ti3+ species are formed by the resulting crystal distortion due to the partial substitution of Ti4+ by other metal ions (Cu+, Fe2+, V3+) in MIL-125(Ti). MIL-(CuTi) possesses a larger number of OV and Ti3+ compared to MIL-(FeTi) and MIL-(VTi) due to the larger valence difference between Cu+ and Ti4+. These active sites not only promote the adsorption and activation of N-2 and H2O, but also facilitate the photo-generated charge mobility. Photogenerated holes oxidize H2O to produce O-2 and H+. Photogenerated electrons reduce N-2 activated on Ti3+ sites by combining with H+ to form NH4+. Therefore, MIL-(CuTi) shows the highest NH4+ production rate 46.5 mu mol center dot h(-1)center dot g(-1), which is much higher than that (1.2 mu mol center dot h(-1)center dot g(-1)) of the pristine MIL-125(Ti). This work provides a new insight into rational design for artificial N-2 fixation systems by the construction of the active site.
Keyword ：
MOFs MOFs N-2 activation N-2 activation Photocatalysis Photocatalysis Ti3+ Ti3+
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| GB/T 7714 | Liu, Cheng , Chen, Qi , Chen, Yueling et al. Ti3+-mediated MIL-125(Ti) by metal substitution for boosting photocatalytic N2 fixation [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 678 : 616-626 . |
| MLA | Liu, Cheng et al. "Ti3+-mediated MIL-125(Ti) by metal substitution for boosting photocatalytic N2 fixation" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 678 (2024) : 616-626 . |
| APA | Liu, Cheng , Chen, Qi , Chen, Yueling , Yu, Jimmy C. , Wu, Jionghua , Wu, Ling . Ti3+-mediated MIL-125(Ti) by metal substitution for boosting photocatalytic N2 fixation . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 678 , 616-626 . |
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Designing photocatalysts with well-defined structure-function relationships is imperative for propelling the progression of desired photocatalytic oxidation. Herein, the efficient conversion of solar energy to H2O2 and subsequently to hydroxyl radicals (center dot OH) is achieved through a synergistic interplay between olefin linkage (-C = C-) and spatially separated benzene-triazine dual reaction sites within covalent organic frameworks (COFs). The upgraded -C = C- can increase the conjugation degree of COFs, which establishes an expanded superstructure for boosting charge separation/transfer and stability. This precise modulation renders more opportunities for the hot electrons to migrate to the benzene site for solar-to-H2O2 generation, and to the triazine site for H2O2-to-center dot OH, separately. The optimized center dot OH generation pathway enables remarkable oxidation performances against recalcitrant organic pollutants, and pathogenic microorganisms under visible light irradiation. This work provides new insights for tuning the synergistic interactions of various building blocks within the COFs for the selective generation of highly reactive center dot OH for environmental remediation.
Keyword ：
Covalent organic frameworks Covalent organic frameworks H2O2 activation H2O2 activation Hydroxyl radicals Hydroxyl radicals Photocatalysis Photocatalysis Spatial dual sites Spatial dual sites
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| GB/T 7714 | Zhang, Jinpeng , Huang, Guocheng , Chen, Qiaoshan et al. Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 356 . |
| MLA | Zhang, Jinpeng et al. "Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 356 (2024) . |
| APA | Zhang, Jinpeng , Huang, Guocheng , Chen, Qiaoshan , Wu, Ling , Li, Liuyi , Bi, Jinhong . Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 356 . |
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Two-dimensional (2D) semiconductors with unique structures and surface physicochemical characteristics have been extensively employed for efficient photocatalysis. Recently, surface coordination activation interactions have obtained attention in promoting photocatalytic efficiency as they establish bridges between reactants and photocatalysts. Accordingly, a burgeoning trend in the design of 2D photocatalysts is regulating the surface active centers for coordinating with reactants. These attempts have developed various effective strategies to optimize the 2D photocatalysts and provide in-depth insights into the structure-function relationship for heterogeneous photocatalysis. Herein, we summarize recent advances in surface engineering in designing efficient 2D photocatalysts, focusing on coordination activation. We emphasize the advantages of coordination activation as a versatile medium for engineering the surface of photocatalysts. In particular, the discussion includes various strategies for surface engineering and the structure-function relationship in photocatalysis. This work systematically concludes the significance and future challenges of coordination activation in the surface functionalization of 2D photocatalysis, shedding light on the design of next-generation photocatalysts.
Keyword ：
2D photocatalyst 2D photocatalyst Coordination activation Coordination activation Surface engineering Surface engineering
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| GB/T 7714 | Shi, Yingzhang , Wang, Zhiwen , Song, Yujie et al. Designing Efficient 2D Photocatalysts through Coordination Activation Mediated Surface Engineering [J]. | CHEMCATCHEM , 2024 , 16 (21) . |
| MLA | Shi, Yingzhang et al. "Designing Efficient 2D Photocatalysts through Coordination Activation Mediated Surface Engineering" . | CHEMCATCHEM 16 . 21 (2024) . |
| APA | Shi, Yingzhang , Wang, Zhiwen , Song, Yujie , Yu, Jimmy C. , Wu, Ling . Designing Efficient 2D Photocatalysts through Coordination Activation Mediated Surface Engineering . | CHEMCATCHEM , 2024 , 16 (21) . |
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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.
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, Cheng , Chen, Huiling , Chen, Qi et al. Active site modulation in UiO-66(Ce) MOFs by Al3+doping for boosting photocatalysis [J]. | JOURNAL OF CATALYSIS , 2024 , 437 . |
| MLA | Liu, Cheng et al. "Active site modulation in UiO-66(Ce) MOFs by Al3+doping for boosting photocatalysis" . | JOURNAL OF CATALYSIS 437 (2024) . |
| APA | Liu, Cheng , Chen, Huiling , Chen, Qi , Bi, Jinhong , Yu, Jimmy C. , Wu, Ling . Active site modulation in UiO-66(Ce) MOFs by Al3+doping for boosting photocatalysis . | JOURNAL OF CATALYSIS , 2024 , 437 . |
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This work develops a series of bimetallic MIL-68(InFe) MOF nanorods (NM(In1-xFex)) mimicking the nitrogenase for biomimetic photocatalytic N-2 fixation. The partial substitution of In3+ with Fe3+ leads to the electron redistribution from In3+ to Fe3+, generating electron-poor In3+ (In(3+delta)+) sites and electron-rich Fe3+ (Fe(3-delta)+) sites as an electron acceptor-donor combination to promote the N-2 activation by a pi back-donation mechanism. The smaller size of the nanorods further provides more accessible active sites than the bulk counterpart. In cooperation with the H+ released from the H2O, the activated N-2 molecules were reduced by photogenerated electrons to give NH3. The optimal sample NM(In0.90Fe0.10) exhibited the highest NH4+ production rate of 30.8 mu molh(-1)g(-1) without any sacrificial agent, attributed to the presence of abundant In/Fe bimetallic sites for N-2 activation and enhanced charge mobility. This work provides new insights into rational design for artificial N-2 fixation systems by mimicking natural nitrogenase.
Keyword ：
Dual-metal sites Dual-metal sites MOFs MOFs N-2 activation N-2 activation Photocatalysis Photocatalysis
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| GB/T 7714 | Liu, Cheng , Chen, Mengning , Chen, Yueling et al. Bimetallic MIL-68(InFe) MOF nanorods for biomimetic photocatalytic N2 fixation [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 498 . |
| MLA | Liu, Cheng et al. "Bimetallic MIL-68(InFe) MOF nanorods for biomimetic photocatalytic N2 fixation" . | CHEMICAL ENGINEERING JOURNAL 498 (2024) . |
| APA | Liu, Cheng , Chen, Mengning , Chen, Yueling , Chen, Qi , Wu, Jionghua , Lin, Sen et al. Bimetallic MIL-68(InFe) MOF nanorods for biomimetic photocatalytic N2 fixation . | CHEMICAL ENGINEERING JOURNAL , 2024 , 498 . |
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A series of 2D/2D MoS2/Bi2WO6 S-scheme heterojunctions consisting of ultrathin MoS2 nanosheets (MS, 1.6 nm) and ultrathin Bi2WO6 nanosheets (BWO, 1.5 nm) were developed for photocatalytic degradation of ciprofloxacin. The samples with 5 % mass ratio of MS (5 %MS/BWO) exhibits the almost complete degradation of ciprofloxacin (approximate to 100 %) under visible light. It is evidenced that the formation of S-scheme heterojunction with close interfacial interaction facilitates the photoinduced carrier separation and the generation of surface acid sites. The activation of ciprofloxacin molecules is realized through the coordinately interaction of C-N and C=O with the surface W sites. Moreover, the OVs in BWO side is a convenient pathway for activated of O-2, embodying in the generation of center dot O-2(-) and center dot OH under visible light over photocatalyst. Such an association of charge transfer mechanism with coordination activation shows the enhanced photocatalytic performance toward ciprofloxacin. This work provides a motivation which designs an S-scheme heterojunction photocatalyst with the ability to activate the specific group in molecules to comprehend the degradation of antibiotics.
Keyword ：
Bi2WO6 nanosheet Bi2WO6 nanosheet Molecule coordination activation Molecule coordination activation MoS2 nanosheet MoS2 nanosheet Photocatalysis Photocatalysis S-scheme heterojunctions S-scheme heterojunctions
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| GB/T 7714 | Chen, Qi , Liu, Cheng , Liu, Rui et al. Ultrathin 2D/2D MoS2/Bi2WO6 S-scheme heterojunction for boosting photocatalytic degradation of ciprofloxacin [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 355 . |
| MLA | Chen, Qi et al. "Ultrathin 2D/2D MoS2/Bi2WO6 S-scheme heterojunction for boosting photocatalytic degradation of ciprofloxacin" . | SEPARATION AND PURIFICATION TECHNOLOGY 355 (2024) . |
| APA | Chen, Qi , Liu, Cheng , Liu, Rui , Hou, Yidong , Bi, Jinhong , Yu, Jimmy C. et al. Ultrathin 2D/2D MoS2/Bi2WO6 S-scheme heterojunction for boosting photocatalytic degradation of ciprofloxacin . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 355 . |
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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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