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学者姓名:吴棱
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Moisture enabled electric generation (MEG) is an innovative green energy technology that converts the chemical potential energy of atmospheric water vapor into electricity. Here, we report a novel molecular-level zero-dimensional (0D) perovskite-based MEG device that efficiently harvests ambient moisture to generate electric power, which makes perovskite a new kind of potential MEG. The 0D perovskite, DAP(2)PbI(6), (where DAP is 1,3-bis(ammonium)-2-hydroxypropane diiodide.) features a unique hydrogen-bonding network formed between its ammonium (-NH3+) and hydroxyl (-OH) groups, imparting water stability and remarkable hydrophilicity. Such robust interactions facilitate water adsorption and the subsequent release of hydrogen ions under humid conditions. These protonic species establish an ion gradient, driving a directional current via the ion-gradient diffusion-induced voltage. We demonstrated a maximum volumetric power density of 45 mWcm-3-substantially exceeding previously reported values for protein- or carbon-based MEG. Additionally, SEM and AFM analyses confirm DAP(2)PbI(6) is stable upon moisture exposure, while temperature-dependent impedance spectroscopy and theoretical calculations reveal that proton diffusion is the primary mechanism for the observed moisture-driven electricity. These findings underscore the promise of hydrophilic 0D perovskite materials for high-efficiency MEG and pave the way for next-generation sustainable power applications.
Keyword :
High performance High performance Ionic transport Ionic transport Moisture enabled electric generation Moisture enabled electric generation Perovskite Perovskite Zero-dimensional halide structures Zero-dimensional halide structures
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GB/T 7714 | Xu, Yuehao , Wu, Jionghua , Chen, Zhaojie et al. High-Efficiency Moisture-Driven Electric Generator Enabled by Hydrophilic 0D Perovskite† [J]. | CHINESE JOURNAL OF CHEMISTRY , 2025 , 43 (19) : 2519-2524 . |
MLA | Xu, Yuehao et al. "High-Efficiency Moisture-Driven Electric Generator Enabled by Hydrophilic 0D Perovskite†" . | CHINESE JOURNAL OF CHEMISTRY 43 . 19 (2025) : 2519-2524 . |
APA | Xu, Yuehao , Wu, Jionghua , Chen, Zhaojie , Xie, Wenchao , Meng, Xin , Sun, Xiaohui et al. High-Efficiency Moisture-Driven Electric Generator Enabled by Hydrophilic 0D Perovskite† . | CHINESE JOURNAL OF CHEMISTRY , 2025 , 43 (19) , 2519-2524 . |
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Photocatalytic N-2 fixation is a green and sustainable pathway for the synthesis of ammonia. However, its efficiency is considerably restricted by the energy-intensive activation of N-2 molecules. Herein, a series of MOF-74(Co) with varying contents of coordinatively unsaturated Co sites were synthesized through the thermal treatment at different temperatures (T = 100, 150, 200, 250 degrees C). These photocatalysts were used for the photocatalytic fixation of N-2 in the absence of a sacrificial agent. The experimental results and theoretical computations indicate that the amount of coordinatively unsaturated Co sites increases as the temperature elevates by the removal of coordinated H2O from MOF-74(Co). These Co sites can function as active sites to promote chemisorption and activation of N-2 molecules. The sample MOF-74(Co)-200 exhibits the highest NH4+ production rate of 84 mu molg(-1)h(-1), which is six times higher than that of the pristine MOF-74(Co) (13.9 mu molg(-1)h(-1)). The enhanced performance can be ascribed to the abundance of active sites and the optimal mobility of the photogenerated charges. Finally, a mechanism is proposed for the photocatalytic N-2 activation at the molecular level.
Keyword :
coordinatively unsaturated Co sites coordinatively unsaturated Co sites MOF-74(Co) MOF-74(Co) N-2 activation N-2 activation photocatalysis photocatalysis thermal treatment thermal treatment
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GB/T 7714 | Ye, Binghua , Liu, Cheng , Chen, Yueling et al. Regulating the Unsaturated Co Sites on MOF-74(Co) for Enhancing Photocatalytic N2 to NH3 Conversion [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2025 , 13 (9) : 3588-3599 . |
MLA | Ye, Binghua et al. "Regulating the Unsaturated Co Sites on MOF-74(Co) for Enhancing Photocatalytic N2 to NH3 Conversion" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 13 . 9 (2025) : 3588-3599 . |
APA | Ye, Binghua , Liu, Cheng , Chen, Yueling , Chen, Qi , Jing, Kaiqiang , Yu, Jimmy C. et al. Regulating the Unsaturated Co Sites on MOF-74(Co) for Enhancing Photocatalytic N2 to NH3 Conversion . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2025 , 13 (9) , 3588-3599 . |
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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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Single-atom catalysts (SACs) hold great promise for the electrocatalytic N2 reduction reaction (NRR), yet a comprehensive understanding of coordination microenvironment modulation remains elusive. Herein, Ni SACs with diverse Ni-Nx-C configurations (square-planar: Ni-N4, triangle-cone: Ni-N1-N3, pentagon-planar: Ni-N5, and square-cone: Ni-N1-N4) were theoretically studied. Ni SACs with the Ni-N1-N4 configuration demonstrated the highest stability and suitability for N2 adsorption, hydrogenation (*NN -> *NNH), and inhibition of *H adsorption for H2 evolution. Notably, the additionally coordinated N disrupted the axisymmetric distribution of electrons in Ni-N1-N4, particularly in the z-direction of Ni d z 2 orbitals, inducing the end-adsorbed N2 to adopt an inclined position. The variation in electronic states facilitated the simultaneous sigma and pi interaction between Ni d z2 and N2, forming a strong Ni-N bond (1.89 & Aring;) and promoting N2 activation via p-d hybridization. In light of the calculation results, Ni SACs with the Ni-N1-N4 configuration (Ni20-FAN) were fabricated and displayed a superior NRR activity and Faradaic efficiency of 35.74% at -0.4 V vs RHE. In situ spectroscopic techniques together with density functional theory calculations further unraveled a facile distal pathway for ammonia evolution over Ni-N1-N4 SACs. This work offers an innovative perspective for theory-guided modulation of the SAC coordination microenvironment, introducing asymmetric coordination as an effective strategy for the activation of symmetric inert molecules.
Keyword :
asymmetric coordination asymmetric coordination coordinationmicroenvironment modulation coordinationmicroenvironment modulation nitrogen electroreduction nitrogen electroreduction p-d hybridization p-d hybridization single atom single atom
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GB/T 7714 | Chen, Yueling , Luo, Laihao , Wu, Houyi et al. Boosting Nitrogen Activation with Asymmetric Coordinated Ni-N1-N4 Site through p-d Hybridization [J]. | ACS CATALYSIS , 2025 , 15 (13) : 11103-11112 . |
MLA | Chen, Yueling et al. "Boosting Nitrogen Activation with Asymmetric Coordinated Ni-N1-N4 Site through p-d Hybridization" . | ACS CATALYSIS 15 . 13 (2025) : 11103-11112 . |
APA | Chen, Yueling , Luo, Laihao , Wu, Houyi , Kong, Xiangyu , Liu, Yan , Huang, Guocheng et al. Boosting Nitrogen Activation with Asymmetric Coordinated Ni-N1-N4 Site through p-d Hybridization . | ACS CATALYSIS , 2025 , 15 (13) , 11103-11112 . |
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The construction of metal-organic frameworks that possesses the tunable metal active sites and synergistic effect for the reactant activation is an attractive strategy for the optimization of photocatalytic performance. Herein, a series of MIL-88A(Fe1-xCux) were synthesized for photocatalytic nitrogen reduction reaction (NRR). It was characterized that the Fe2+ and oxygen vacancies were produced in MIL-88A(Fe) due to the partly reduction of ligand fumaric acid in synthesis process. The substitution of Fe3+ with Cu2+ induces charge imbalance and lattice distortion, further increasing the content of Fe2+ and oxygen vacancies. The optimal sample MIL-88A (Fe0.95Cu0.05) (CMA-5 %) exhibits the highest nitrogen fixation performance of 68.6 mu mol & sdot;g- 1 & sdot;h- 1, which is 8 times higher than that of the pristine material. It is attributable to the synergistic effect of the abundant Fe2+ and oxygen vacancies as active sites to promote N2 coordination and photogenerated carrier separation, resulting in the efficient conversion of activated N2 to NH3. Furthermore, the in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy provide clear evidence of the behavior of the N2 adsorption and activation on the catalyst. Finally, we propose a potential mechanism at molecular level regarding the relationship between the synergistic effect and the nitrogen fixation activity.
Keyword :
Active sites Active sites Coordination activation Coordination activation Defect manipulation Defect manipulation MIL-88A(Fe1-xCux) MIL-88A(Fe1-xCux) Photocatalytic N 2 fixation Photocatalytic N 2 fixation
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GB/T 7714 | Liu, Runlai , Chen, Qi , Qiu, Jinjing et al. Cu mediated defect manipulation in MIL-88A(Fe) for boosting photocatalytic N2 fixation [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 692 . |
MLA | Liu, Runlai et al. "Cu mediated defect manipulation in MIL-88A(Fe) for boosting photocatalytic N2 fixation" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 692 (2025) . |
APA | Liu, Runlai , Chen, Qi , Qiu, Jinjing , Liu, Cheng , Wu, Jionghua , Yu, Jimmy C. et al. Cu mediated defect manipulation in MIL-88A(Fe) for boosting photocatalytic N2 fixation . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 692 . |
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Subspace clustering can capture the structural features of complex networks. However, existing subspace-based methods encounter challenges related to dependence on priori knowledge, difficulties in exploiting the connection between two stages and addressing networks with fuzzy boundaries. In response to these challenges, a novel subspace clustering-based community detection algorithm, Structured Adaptive Block Diagonal Subspace Learning with Fusion (SABDSLF) is proposed. First, adaptive block diagonal subspace learning strategy is designed. This approach establishes a convex objective function without the need for prior knowledge. Second, structured subspace learning strategy uses a structure matrix to capture the connection between the two stages of the subspace algorithm. Finally, an information fusion strategy is designed to combine topological information and subspace information, enabling the handling of complex networks with fuzzy boundaries. Experiments were conducted on real-world and synthetic networks, demonstrating that SABDSLF outperforms several state-of-the-art community detection methods in terms of precision and robustness.
Keyword :
Adaptive block-diagonal learning Adaptive block-diagonal learning Community detection Community detection One-stage One-stage Subspace clustering Subspace clustering Subspace structured representation Subspace structured representation
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GB/T 7714 | Wu, Ling , Cai, Ziqi , Yang, Yingjie et al. Community detection via structured adaptive block-diagonal learning with topology-subspace fusion [J]. | MACHINE LEARNING , 2025 , 114 (8) . |
MLA | Wu, Ling et al. "Community detection via structured adaptive block-diagonal learning with topology-subspace fusion" . | MACHINE LEARNING 114 . 8 (2025) . |
APA | Wu, Ling , Cai, Ziqi , Yang, Yingjie , Guo, Kun . Community detection via structured adaptive block-diagonal learning with topology-subspace fusion . | MACHINE LEARNING , 2025 , 114 (8) . |
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Photocatalytic chemical transformations for green organic synthesis has attracted much interest. However, their development is greatly hampered by the lack of sufficient reactive sites on the photocatalyst surface for the adsorption and activation of substrate molecules. Herein, we demonstrate that the introduction of well-defined Lewis and Br & oslash;nsted acid sites coexisting on the surface of TiO2 (SO42-/N-TiO2) creates abundant active adsorption sites for photoredox reactions. The electron-deficient Lewis acid sites supply coordinatively unsaturated surface sites to adsorb molecular oxygen, and the Br & oslash;nsted acid sites are liable to donate protons to form hydrogen bonds with the OH groups of alcohols like benzyl alcohol (BA). These coexistent acid sites result in a strong synergistic effect in photocatalytic aerobic oxidation of BA. For example, the conversion of BA to benzaldehyde was found to be 88.6 %, being much higher than those of pristine TiO2 (14.7 %), N-doped TiO2 (N-TiO2, 24.6 %), sulfated TiO2 (SO42-/ TiO2, 35.4 %), and even their sum. The apparent quantum efficiency (AQE) was determined to be 58.1 % at 365 nm and 12.9 % at 420 nm over SO42-/N-TiO2. This strategy to create effective synergistic Lewis and Br & oslash;nsted acids on the catalyst surfaces enables us to apply it to other semiconducting photocatalytic organic transformations.
Keyword :
br & oslash;nsted acids br & oslash;nsted acids heterogeneous catalysis heterogeneous catalysis lewis acids lewis acids oxidation oxidation photocatalysis photocatalysis
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GB/T 7714 | Yu, Dexi , Zou, Junhua , Zeng, Lingdong et al. Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (15) . |
MLA | Yu, Dexi et al. "Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 15 (2025) . |
APA | Yu, Dexi , Zou, Junhua , Zeng, Lingdong , Hou, Yidong , Lin, Wei , Wu, Ling et al. Lewis and Brønsted Acids Synergy in Photocatalytic Aerobic Alcohol Oxidations . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (15) . |
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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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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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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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