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学者姓名：吴棱
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Abstract ：
Defect engineering and single atom incorporation can provide more active sites to modulate the surface electronic structure of a catalyst and to activate reactant molecules. Herein, a series of Ru-anchored DUT-67(Zr) MOFs with explicit defect sites have been prepared for photocatalytic nitrogen reduction. It is characterized that Ru/DUT-67(Zr) possesses uniformly dispersed Ru single atoms and unsaturated Zr. Typically, 1.0 %Ru/DUT-67 (Zr) shows best performance with a NH4+ yield of 61.1 mu mol center dot g-1 center dot h-1, which is approximately 6-folds higher than that of defective DUT-67(Zr) without Ru single atom (DUT-L), while pristine DUT-67(Zr) exhibits a lack of the photocatalytic N2 reduction activity. The observed enhancement can be attributed to the introduction of Ru and unsaturated Zr sites induced by irradiation. Both of them can work together act as active centers to absorb and activate dinitrogen molecule. Furthermore, benefited from the electronic channel (Ru-S) between Ru and DUT-67 (Zr), the separation of photogenerated carriers has been greatly improved, contributing to the collaborative conversion of activated N2 to NH3. This study provides a new insight for designing a dual active sites photo- catalyst with unsaturated coordinated sites and the single atoms by the coordinately interaction of functionalized linker.
Keyword ：
Nitrogen activation Nitrogen activation Ru/DUT-67 MOF Ru/DUT-67 MOF Single atoms Single atoms Synergistic effect Synergistic effect
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| GB/T 7714 | Qiu, Jinjing , Chen, Qi , Liu, Cheng et al. Ru single atom modified DUT-67(Zr) with unsaturated Zr for high-efficiency photocatalytic nitrogen reduction [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 366 . |
| MLA | Qiu, Jinjing et al. "Ru single atom modified DUT-67(Zr) with unsaturated Zr for high-efficiency photocatalytic nitrogen reduction" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 366 (2025) . |
| APA | Qiu, Jinjing , Chen, Qi , Liu, Cheng , Chen, Yueling , Wu, Jionghua , Jing, Kaiqiang et al. Ru single atom modified DUT-67(Zr) with unsaturated Zr for high-efficiency photocatalytic nitrogen reduction . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 366 . |
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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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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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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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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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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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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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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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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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