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学者姓名:汤儆
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The electrochemical reduction of nitrate (NO3-) to ammonia (NH3) (NO3RR) represents an environmentally sustainable strategy for NH3 production while concurrently addressing water pollution challenges. Nevertheless, the intrinsic complexity of this multi-step reaction severely constrains both the selectivity and efficiency of NO3RR. Copper-based electrocatalysts have been extensively investigated for NO3RR but often suffer from nitrite (NO2-) accumulation, which stems from insufficient NO3-adsorption strength. This limitation often leads to rapid catalyst deactivation, hindered hydrogenation pathways, and reduced overall efficiency. Herein, we report a one-step green chemical reduction method to synthesize PtCuSnCo quarternary alloy nanoparticles with homogeneously distributed elements. Under practical NO3-concentrations, the optimized catalyst exhibited an impressive Faradaic efficiency approaching 100% and an outstanding selectivity of 95.6 +/- 2.9%. Mechanistic insights uncovered that SnCo sites robustly facilitated NO3-adsorption, complemented by the proficiency of PtCu sites in NO3-reduction. The synergistic spatial neighborhood effect between SnCo and PtCu sites efficiently stabilizes NO3-deoxygenation and suppresses NO2-accumulation. This tandem architecture achieves a finely tuned balance between adsorption strength and deoxygenation kinetics, enabling highly selective and efficient NO3RR. Our findings emphasize the indispensable role of engineered multi-metallic catalysts in overcoming persistent challenges of NO3RR, paving the way for advanced NH3 synthesis and environmental remediation. (c) 2025, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
Keyword :
Ammonia synthesis Ammonia synthesis Deoxidation Deoxidation In situ Raman spectroscopy In situ Raman spectroscopy Neighboring effect Neighboring effect Quaternary alloy Quaternary alloy
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GB/T 7714 | Ling, Yun , Su, Hui , Zhou, Ru-Yu et al. Neighboring effect in PtCuSnCo alloy catalysts for precisely regulating nitrate adsorption and deoxidation to achieve 100% faradaic efficiency in ammonia synthesis [J]. | CHINESE JOURNAL OF CATALYSIS , 2025 , 73 : 347-357 . |
MLA | Ling, Yun et al. "Neighboring effect in PtCuSnCo alloy catalysts for precisely regulating nitrate adsorption and deoxidation to achieve 100% faradaic efficiency in ammonia synthesis" . | CHINESE JOURNAL OF CATALYSIS 73 (2025) : 347-357 . |
APA | Ling, Yun , Su, Hui , Zhou, Ru-Yu , Feng, Qingyun , Zheng, Xuan , Tang, Jing et al. Neighboring effect in PtCuSnCo alloy catalysts for precisely regulating nitrate adsorption and deoxidation to achieve 100% faradaic efficiency in ammonia synthesis . | CHINESE JOURNAL OF CATALYSIS , 2025 , 73 , 347-357 . |
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Benzophenone derivatives (BPs), as synthetic chemicals widely used in personal care products, have drawn increasing attention due to their potential health risks. However, monitoring BPs in biological samples remains challenging due to their complex matrices and the deficiency in sensitivity and selectivity in current methods. Herein, a method combining hierarchically flower-like hollow covalent organic frameworks (HFH-COFs) with high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) was established for the enrichment and detection of BPs in serum samples. The HFH-COFs were synthesized at room temperature and employed as an adsorbent due to their advantageous properties. The as-prepared HFH-COFs exhibited high specific surface area (2286.53 m(2)/g), excellent chemical stability, and good thermal stability, making them ideal for efficient enrichment applications. Under optimized experimental conditions, five BPs were effectively enriched and quantified by HPLC-MS/MS in the range of 50.0-5000.0 ng/L with good linearity (r > 0.9992). The limit of detections was 0.5-10.0 ng/L. Furthermore, HFH-COFs showed high enrichment factors even over multiple adsorption-desorption cycles. This study proposed a reliable and efficient method for monitoring endocrine-disrupting compounds in complex biological samples and highlighted the potential of HFH-COFs as a superior adsorbent material for BP.
Keyword :
Benzophenone derivatives Benzophenone derivatives Hollow flower-like covalent organic frame works Hollow flower-like covalent organic frame works Mouse serum Mouse serum
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GB/T 7714 | Yang, Ziyi , Yu, Qing , Wu, Yijing et al. Facile synthesis of hierarchically flower-like hollow covalent organic frameworks for enrichment and metabolic analysis of benzophenone derivatives in mouse serum [J]. | JOURNAL OF CHROMATOGRAPHY A , 2025 , 1743 . |
MLA | Yang, Ziyi et al. "Facile synthesis of hierarchically flower-like hollow covalent organic frameworks for enrichment and metabolic analysis of benzophenone derivatives in mouse serum" . | JOURNAL OF CHROMATOGRAPHY A 1743 (2025) . |
APA | Yang, Ziyi , Yu, Qing , Wu, Yijing , Yuan, Jiahao , Dong, Shaofeng , Li, Songtao et al. Facile synthesis of hierarchically flower-like hollow covalent organic frameworks for enrichment and metabolic analysis of benzophenone derivatives in mouse serum . | JOURNAL OF CHROMATOGRAPHY A , 2025 , 1743 . |
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Designing efficient photocatalysts for photocatalysis hydrogen production is crucial for advancing green energy technologies. In this work, ZnIn2S4 photocatalyst with an asymmetric Zn-Zn-S unit ring structure and abundant in S vacancies was achieved by precisely tuning the molar mass of the Zn ion source using ethylene glycol as the reaction solvent. Z-type heterojunction was constructed via the electrostatic assembly by combining silver clusters (Agx@GSH) with ZnIn2S4 to enhance charge separation and photocatalytic activity. The structural transition from S-Zn-S to Zn-Zn-S led to local charge redistribution. Meanwhile, S vacancies acted as electron traps, promoting the charge state change of S in the S-H sites and significantly accelerates the hydrogen evolution reaction (HER). The composite catalyst Zn-Vs-ZIS/Agx@GSH exhibited a hydrogen production rate of 18.4 mmol & sdot;g-1 & sdot;h-1, under acidic conditions with lactic acid as the sacrificial agent, which is 3.7 times higher than pristine ZnIn2S4. Density functional theory (DFT) calculations revealed that the Zn-Zn-S distortion and heterojunction formation synergistically enhanced charge transfer and hydrogen adsorption kinetics. This work provides a novel approach for tailoring ZnIn2S4-based photocatalysts and provides new insights into the design of high-performance heterojunction systems for solar energy conversion.
Keyword :
Heterojunction Heterojunction Indium zinc sulfide Indium zinc sulfide Local charge redistribution Local charge redistribution Photocatalytic hydrogen production Photocatalytic hydrogen production Silver nanoclusters Silver nanoclusters
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GB/T 7714 | Jin, Guangrui , Ge, Baoxin , Hong, Xinle et al. Tuning structure and electronegativity of adjacent atoms of ZnIn2S4/ Agx@GSH via Zn modification for enhanced photocatalytic hydrogen production [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 519 . |
MLA | Jin, Guangrui et al. "Tuning structure and electronegativity of adjacent atoms of ZnIn2S4/ Agx@GSH via Zn modification for enhanced photocatalytic hydrogen production" . | CHEMICAL ENGINEERING JOURNAL 519 (2025) . |
APA | Jin, Guangrui , Ge, Baoxin , Hong, Xinle , Huang, Caijin , Tang, Jing . Tuning structure and electronegativity of adjacent atoms of ZnIn2S4/ Agx@GSH via Zn modification for enhanced photocatalytic hydrogen production . | CHEMICAL ENGINEERING JOURNAL , 2025 , 519 . |
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Designing high activity and stable oxygen evolution reaction (OER) catalysts is essential for improving the efficiency of the water splitting reaction. The high entropy transition metal sulfide (HES) catalyst will be a promising candidate for accelerating the OER due to its high intrinsic activity and excellent stability. However, the synthesis of HES by chemical methods and the investigation of the structural evolution during the reaction remain a challenging task. In this work, a HES catalyst has been synthesized by a simple thermal injection method. All elements are uniformly distributed in HES nanoparticles, which exhibit excellent activity with an exceptionally low overpotential of 263 at current densities of 100 mA center dot cm- 2 and a low Tafel slope of 51.5 mV center dot dec- 1. This work demonstrates the great potential of HES catalysts as OER electrocatalysts and provides new ideas for the construction and extension of this family of compounds.
Keyword :
High entropy sulfide High entropy sulfide In situ Raman In situ Raman Oxygen evolution reaction Oxygen evolution reaction Synergistic effect Synergistic effect Thermo injection Thermo injection
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GB/T 7714 | Shi, Jihua , Jiang, Haishun , Hong, Xinle et al. Non-noble metal high entropy sulfides for efficient oxygen evolution reaction catalysis [J]. | APPLIED SURFACE SCIENCE , 2024 , 642 . |
MLA | Shi, Jihua et al. "Non-noble metal high entropy sulfides for efficient oxygen evolution reaction catalysis" . | APPLIED SURFACE SCIENCE 642 (2024) . |
APA | Shi, Jihua , Jiang, Haishun , Hong, Xinle , Tang, Jing . Non-noble metal high entropy sulfides for efficient oxygen evolution reaction catalysis . | APPLIED SURFACE SCIENCE , 2024 , 642 . |
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Currently, transition metal phosphides (Cu, Fe, Co, and others) have been identified as potential candidates for both the oxygen evolution reaction (OER, anode) and hydrogen evolution reaction (HER, cathode). One of the copper based phosphides has shown efficiency for the HER, however, it displays greater theoretical potential and instability compared to noble metal materials in the OER process. Herein, Cu-MOF-NH2 nanocubes were subjected to pyrolysis treatment in a low phosphorus atmosphere to produce highly dispersed Cu3P nanoparticles. Dispersed Cu3P nanoparticles coated with nitrogen-carbon matrix composite layers provide numerous active sites and high stability. In situ Raman spectra confirmed a significant reduction in Cu+ oxidation to Cu2+. Furthermore, according to XPS resolution results, the Cu-P bond provides electrons to the Cu-P-O bond, thus accelerating the OER process. We integrated experimental electrochemistry to verify the potential enhancement of the OER performance and stability of Cu3P using appropriate nanostructure coating techniques. The Cu3P/NC@CF electrode was prepared by the phosphorylation and pyrolysis of Cu MOF-NH2. It retained superior structural stability for the OER process and served as both anode and cathode for the overall water splitting in 1 M KOH solution.
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GB/T 7714 | Jiang, Haishun , Shi, Jihua , Liu, Xiangyue et al. Highly dispersed copper phosphide nanoparticles accelerate the electrolytic water oxidation process [J]. | GREEN CHEMISTRY , 2024 , 26 (6) : 3388-3396 . |
MLA | Jiang, Haishun et al. "Highly dispersed copper phosphide nanoparticles accelerate the electrolytic water oxidation process" . | GREEN CHEMISTRY 26 . 6 (2024) : 3388-3396 . |
APA | Jiang, Haishun , Shi, Jihua , Liu, Xiangyue , Tang, Jing . Highly dispersed copper phosphide nanoparticles accelerate the electrolytic water oxidation process . | GREEN CHEMISTRY , 2024 , 26 (6) , 3388-3396 . |
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Electrolysis of seawater is currently a promising technology for efficient green hydrogen production and solving the energy crisis. Urea oxidation reaction (UOR) has a low thermodynamic onset potential, which is an effective reaction to replace the oxygen evolution reaction (OER) in overall seawater splitting and avoid toxic hypochlorite generation. In this paper, we report sulfur-doped NiFe LDH with ultrathin nanoflower morphology on the surface of three-dimensional nickel foam (NF) loaded with Ti3C2Tx MXene by the two-step electrodeposition method (S-NiFe LDH/MXene@NF). The catalytic performance of electrolytic seawater is boosted by the synergistic effect of the abundant interface between Ti3C2Tx MXene and sulfur-doped NiFe LDH, which promotes electron transfer. S-NiFe LDH/MXene@NF exhibited electrocatalytic performance values of 1.578 and 1.437 V (vs RHE) for OER and UOR at 500 mA cm(-2), respectively, and an overpotential of 336 mV for the hydrogen evolution reaction (HER) at 500 mA cm(-2) in an alkaline seawater electrolyte. As a bifunctional electrode, it can achieve a current density of 500 mA cm(-2) at 2.027 V with great stability. The in situ Raman detection of surface recombination of the S-NiFe LDH/MXene@NF electrode in the UOR demonstrates that Ti3C2Tx MXene accelerates the formation of the active species NiOOH on the electrode surface and facilitates the lattice disturbance of NiOOH. This helps to increase the catalytic activity of urea-assisted overall seawater splitting.
Keyword :
electrolysis of seawater electrolysis of seawater in situ Raman in situ Raman layered double hydroxides layered double hydroxides MXene MXene synergistic effect synergistic effect
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GB/T 7714 | Liu, Yijun , Hong, Xinle , Liu, Xiangyue et al. Electrolysis of Seawater: An Effective Path to Sustainable Hydrogen Production with Sulfur-Doped NiFe LDH/MXene@NF Electrodes [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (31) : 11520-11530 . |
MLA | Liu, Yijun et al. "Electrolysis of Seawater: An Effective Path to Sustainable Hydrogen Production with Sulfur-Doped NiFe LDH/MXene@NF Electrodes" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 12 . 31 (2024) : 11520-11530 . |
APA | Liu, Yijun , Hong, Xinle , Liu, Xiangyue , Chen, Wenjie , Tang, Jing . Electrolysis of Seawater: An Effective Path to Sustainable Hydrogen Production with Sulfur-Doped NiFe LDH/MXene@NF Electrodes . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (31) , 11520-11530 . |
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Plasmon-mediated chemical reaction (PMCR) is a highly attractive field of research. Here we report in situ surface-enhanced Raman spectroscopic (SERS) monitoring of plasmonic-mediated S-S bond-forming reaction. The reaction is thought to be a self-coupling reaction proceeding by photoinduced aromatic S-C bond arylation. Surprisingly, the S-C arylation and S-S coupling are found to be occurred on both partially oxidized silver and silver nanoparticles. The results demonstrated that silver oxide or hydroxide and small molecule donor sacrifice agent played a crucial role in the reaction. This work facilitates the in-situ manipulation and characterization of the active silver electrode interface in conjunction with electrochemistry, and also establishes a promising new guideline for surface plasmon resonance photocatalytic reactions on metal nanostructures with high efficiency.
Keyword :
S-C arylation S-C arylation Silver Silver S-S coupling S-S coupling Surface-enhanced Raman spectroscopy (SERS) Surface-enhanced Raman spectroscopy (SERS) Surface plasmon resonances (SPR) Surface plasmon resonances (SPR)
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GB/T 7714 | Ling, Yun , Zhang, Maosheng , Liu, Guokun et al. Plasmonic-mediated S-C arylation and S-S coupling on nanostructured silver electrodes monitored by in situ surface-enhanced Raman spectroscopy [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 668 : 154-160 . |
MLA | Ling, Yun et al. "Plasmonic-mediated S-C arylation and S-S coupling on nanostructured silver electrodes monitored by in situ surface-enhanced Raman spectroscopy" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 668 (2024) : 154-160 . |
APA | Ling, Yun , Zhang, Maosheng , Liu, Guokun , Wu, Deyin , Tang, Jing . Plasmonic-mediated S-C arylation and S-S coupling on nanostructured silver electrodes monitored by in situ surface-enhanced Raman spectroscopy . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 668 , 154-160 . |
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Atomically precise metal nanoclusters (NCs) present new opportunities for creating innovative solar-powered photoanodes due to their extraordinary physicochemical properties. Nevertheless, ultrasmall metal NCs tend to aggregate and lack active sites under light irradiation, which severely limits their widespread application. We have developed a strategy to design efficient ternary photoanodes by successively modifying AgAu NCs and CoNi-LDH on BiVO4 substrates using versatile impregnation and electrodeposition. The electronic properties of AgAu NCs facilitate the rapid transfer of photogenerated carriers on BiVO4 and CoNi-LDH. Additionally, ultrathin CoNi-LDH acts as a hole-collecting layer, which quickly extracts holes to the electrode/electrolyte interface. The synergistic effect and the matched energy levels between the ternary heterostructures promote the OER process, which significantly improved the photoelectrochemical (PEC) water oxidation performance. This study presents a new idea for further exploration of metal nanocluster-based PEC systems.
Keyword :
bismuth vanadate bismuth vanadate metal nanoclusters metal nanoclusters photoelectrochemical water splitting photoelectrochemical water splitting synergistic effect synergistic effect ternaryphotoanodes ternaryphotoanodes
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GB/T 7714 | Chen, Wenjie , Jin, Guangrui , Liu, Yijun et al. Ternary Photoanodes with AgAu Nanoclusters and CoNi-LDH for Enhanced Photoelectrochemical Water Oxidation [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (18) : 23296-23304 . |
MLA | Chen, Wenjie et al. "Ternary Photoanodes with AgAu Nanoclusters and CoNi-LDH for Enhanced Photoelectrochemical Water Oxidation" . | ACS APPLIED MATERIALS & INTERFACES 16 . 18 (2024) : 23296-23304 . |
APA | Chen, Wenjie , Jin, Guangrui , Liu, Yijun , Wei, Qiaohua , Tang, Jing . Ternary Photoanodes with AgAu Nanoclusters and CoNi-LDH for Enhanced Photoelectrochemical Water Oxidation . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (18) , 23296-23304 . |
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Direct electrochemical nitrate reduction to ammonia (NRA) synthesis is an efficient and environmentally friendly production technology. However, the development of highly selective electrocatalysts is still a challenge due to the nine-proton and eight-electron reduction reaction. High-entropy alloys (HEAs) contain a wide range of elements and have adjustable properties, giving them excellent application potential in multi-step reactions. In this work, we skillfully use the local high temperature and excellent thermal conductivity generated at the reduced graphene oxide (rGO) defect in a microwave process to achieve a rapid quenching process in 10 seconds. This approach overcomes element immiscibility and results in a self-supported, single-phase, non-precious metal and uniform FeCoNiCuSn alloy electrode. The HEAs reach a remarkable NH3 yield of 883.7 +/- 11.2 mu g h-1 cm-2, maximum faradaic efficiency (FE) of 94.5 +/- 1.4%, and highest NH3 selectivity of 90.4 +/- 2.7%. Experimental and theoretical calculations reveal that the presence of multiple adjacent elements in HEAs triggers a synergistic catalytic effect, while the excellent mass and charge transfer properties of rGO jointly encourage the performance of the electrochemical NRA. In particular, NO3- favors vertical adsorption at Fe-Fe sites, and the desorption of NH3 is identified as the rate-determining step (RDS) with an extremely small Delta G value of 0.7 eV.
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GB/T 7714 | Ling, Yun , Feng, Qingyun , Zheng, Xuan et al. Microwave-assisted fabrication of a self-supported graphene-based high-entropy alloy electrode for efficient and stable electrocatalytic nitrate reduction to ammonia [J]. | INORGANIC CHEMISTRY FRONTIERS , 2024 , 12 (2) : 682-691 . |
MLA | Ling, Yun et al. "Microwave-assisted fabrication of a self-supported graphene-based high-entropy alloy electrode for efficient and stable electrocatalytic nitrate reduction to ammonia" . | INORGANIC CHEMISTRY FRONTIERS 12 . 2 (2024) : 682-691 . |
APA | Ling, Yun , Feng, Qingyun , Zheng, Xuan , Su, Hui , Zhang, Yuanyuan , Zou, Zehua et al. Microwave-assisted fabrication of a self-supported graphene-based high-entropy alloy electrode for efficient and stable electrocatalytic nitrate reduction to ammonia . | INORGANIC CHEMISTRY FRONTIERS , 2024 , 12 (2) , 682-691 . |
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The water splitting reaction to produce hydrogen is one of the most promising and cleanest ways to resolve the energy crisis. However, the preparation of efficient and stable electrocatalysts with low-cost remains challenging. In this work, the noble-metal free N-doped carbon (NC) incorporated V-doped cobalt phosphide (CoP) nanosheets on nickel foam (NF) (denoted as V-CoP-NC/NF) are prepared by using two-dimension zeolitic imidazolate framework (ZIF-67) as precursor followed by NaVO3 etching/doping and phosphorization. The V doping is found to be essential to enhance the electrochemical performance of CoP for water splitting. In particular, V5-CoP-NC/ NF (V5 represents the concentration of NaVO3 for etching/doping is 5 mM) exhibits the highest hydrogen evolution performance in alkaline electrolyte, to achieve a current density of 10 mA cm-2, an overpotential of 119 mV (vs reversible hydrogen electrode) is required. X-ray photoelectron spectroscopy results show that the V doping significantly altered the binding energies of Co 2p, P 2p and N 1 s in V5-CoP-NC/NF, which is believed to facilitate the adsorption and dissociation of intermediates and accelerate interfacial charge transfer during hydrogen evolution reaction process. This work provides a simple route to prepare heteroatom doped CoP selfstanding electrocatalysts for water splitting.
Keyword :
2D ZIF-67 2D ZIF-67 CoP/NC CoP/NC Electrocatalytic water splitting Electrocatalytic water splitting Hydrogen evolution Hydrogen evolution V-doped V-doped
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GB/T 7714 | Liu, Xiangyue , Liu, Yijun , Li, Ye et al. 2D ZIF-67 derived V-doped CoP/NC nanosheets as efficient electrocatalysts for water splitting [J]. | ELECTROCHIMICA ACTA , 2023 , 471 . |
MLA | Liu, Xiangyue et al. "2D ZIF-67 derived V-doped CoP/NC nanosheets as efficient electrocatalysts for water splitting" . | ELECTROCHIMICA ACTA 471 (2023) . |
APA | Liu, Xiangyue , Liu, Yijun , Li, Ye , Zhuang, Jinliang , Tang, Jing . 2D ZIF-67 derived V-doped CoP/NC nanosheets as efficient electrocatalysts for water splitting . | ELECTROCHIMICA ACTA , 2023 , 471 . |
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