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学者姓名：李朝晖
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Abstract ：
A rational design of MNPs@MOFs (MNPs = metal nanoparticles, MOFs = metal-organic frameworks) nanocomposites is important for their application as multifunctional catalysts for light-initiated one-pot tandem/cascade reactions. Herein, the Pd@MIL-100(Fe) nanocomposite with a core-shell structure, in which Pd colloids of ca. 3 nm are encapsulated inside the matrix of MIL-100(Fe), was constructed successfully via self-assembly of MIL-100(Fe) in preformed PVP-capped Pd colloids (PVP = polyvinylpyrrolidone) at room temperature. Via a successful combination of MOF-based photocatalysis with Pd-based hydrogenation, Pdrpvp@MIL-100(Fe), with PVP partially removed, exhibited superior performance for the reaction between nitro aromatics and benzyl alcohols to produce secondary amines. Comparison of activity over Pdrpvp@MIL-100(Fe) with that of the other two types of MNPs/MIL-100(Fe) nanocomposites suggests that its superior activity can be attributed to the presence of well-stabilized stable Pd nanoparticles (NPs) for hydrogenation and the unoccupied cavities in MOFs to promote the mass diffusion, especially in the case of larger substrates, as well as an efficient charge transfer from the MOF to Pd NPs for their cooperation. This study indicates that a rational strategy in the construction of metal NPs/MOFs nanocomposites is important for their application as multifunctional catalysts for light-initiated one-pot tandem/cascade reactions.
Keyword ：
core-shell structure core-shell structure MIL-100(Fe) MIL-100(Fe) one-pottandem/cascade reaction one-pottandem/cascade reaction Pd NPs Pd NPs visible light visible light
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| GB/T 7714 | Hu, Liangliang , Liu, Hurunqing , Li, Zhaohui . Rational Design of Core-Shell Structured Pd@MIL-100(Fe) for Efficient Visible Light-Initiated Syntheses of Secondary Amines from Nitro Aromatics and Benzyl Alcohols [J]. | ACS CATALYSIS , 2025 , 15 (3) : 2262-2269 . |
| MLA | Hu, Liangliang 等. "Rational Design of Core-Shell Structured Pd@MIL-100(Fe) for Efficient Visible Light-Initiated Syntheses of Secondary Amines from Nitro Aromatics and Benzyl Alcohols" . | ACS CATALYSIS 15 . 3 (2025) : 2262-2269 . |
| APA | Hu, Liangliang , Liu, Hurunqing , Li, Zhaohui . Rational Design of Core-Shell Structured Pd@MIL-100(Fe) for Efficient Visible Light-Initiated Syntheses of Secondary Amines from Nitro Aromatics and Benzyl Alcohols . | ACS CATALYSIS , 2025 , 15 (3) , 2262-2269 . |
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Pt/Ni-Fe-MOF nanosheets (NSs), with small sized Pt nanoparticles of ca. 2 nm deposited on 2D Ni-Fe-MOF NSs of ca. 5.5 nm, were successfully fabricated and was used as a multifunctional catalyst for one-pot reaction between o-phenylenediamines and alcohols to produce benzimidazoles under visible light. By modulation on the reaction medium and the composition of the catalyst to regulate the individual reaction step involved, an optimum activity was achieved over 4 wt% Pt/Ni-Fe-MOF NSs in a mixed solvent of benzyl alcohol/toluene (v/v, 2/1), which showed a superior yield of 92.0 % to 2-phenylbenzimidazole. In comparison with its bulk counterpart, the superior activity observed over 2D Pt/Ni-Fe-MOF NSs can be attributed to a reduced recombination of the photogenerated charge carriers due to their short transportation path. This study first demonstrated that in addition to the different catalytic sites required, the individual reaction step involved in a one-pot tandem/cascade reaction can be regulated to enable an efficient whole reaction. Such a regulation of the rate of the individual reaction step can, to a certain degree, be achieved by modulation on the reaction medium and the component of the multifunctional catalyst. This study also provides the great potential of using 2D MOF for the construction of multifunctional catalysts for light initiated one-pot tandem/cascade reaction.
Keyword ：
Benzimidazoles Benzimidazoles One-pot tandem/cascade reaction One-pot tandem/cascade reaction Pt/Ni-Fe-MOF nanosheets Pt/Ni-Fe-MOF nanosheets Visible light Visible light
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| GB/T 7714 | Liu, Hurunqing , Wu, Siyang , Li, Zhaohui . Enabling an efficient light initiated one-pot synthesis of benzimidazoles over multifunctional 2D Pt/Ni-Fe-MOF nanosheets [J]. | JOURNAL OF CATALYSIS , 2025 , 447 . |
| MLA | Liu, Hurunqing 等. "Enabling an efficient light initiated one-pot synthesis of benzimidazoles over multifunctional 2D Pt/Ni-Fe-MOF nanosheets" . | JOURNAL OF CATALYSIS 447 (2025) . |
| APA | Liu, Hurunqing , Wu, Siyang , Li, Zhaohui . Enabling an efficient light initiated one-pot synthesis of benzimidazoles over multifunctional 2D Pt/Ni-Fe-MOF nanosheets . | JOURNAL OF CATALYSIS , 2025 , 447 . |
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The valorization of native lignin to functionalized aromatic compounds under visible light is appealing yet challenging. In this communication, colloidal mercaptoalkanoic acid capped ultrathin ZnIn2S4 (ZIS) microbelts was successfully fabricated, which was used as a superior catalyst for depolymerization of native lignin in birch woodmeal under visible light, with an optimum yield of 28.8 wt % to functionalized aromatic monomers achieved in 8 h. The capped mercaptoalkanoic acid not only enables a solvent modulated reversible interchange of ZIS between the colloidal state for efficient reaction and the aggregated state for facile separation, but also serves as a precursor for light initiated generation of reactive thiyl radical for highly selective cleavage of β-O-4 bond in native lignin. This work provides a green and efficient strategy for the depolymerization of native lignin to functionalized aromatic monomers under mild conditions, which involves a new mechanism for the cleavage of β-O-4 bonds in native lignin. The capability of cleavage of β-O-4 bonds in native lignin by photogenerated thiyl radicals also demonstrates the great potential of using photogenerated thiyl radicals in organics transformations. © 2024 Wiley-VCH GmbH.
Keyword ：
Depolymerization Depolymerization Heterogeneous Catalysis Heterogeneous Catalysis Lignin Lignin Photochemistry Photochemistry Radicals Radicals
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| GB/T 7714 | Wang, J. , Li, Y. , Liu, H. et al. Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical [J]. | Angewandte Chemie - International Edition , 2024 , 63 (37) . |
| MLA | Wang, J. et al. "Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical" . | Angewandte Chemie - International Edition 63 . 37 (2024) . |
| APA | Wang, J. , Li, Y. , Liu, H. , Ding, Z. , Yuan, R. , Li, Z. . Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical . | Angewandte Chemie - International Edition , 2024 , 63 (37) . |
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A 2D Mn-based MOF ([Mn4(PDI)2(DMF)7(H2O)]n (MOF 1)) (H4PDI = 5,5 '-(1,3,6,8-tetraoxo-1,3,6,8-tetrahydrobenzo[lmn][3,8]phenanthroline-2,7-diyl)diisophthalic acid) was synthesized. Visible light excited Mn-PDI unit in MOF 1 oxidizes NaSO2CF3 to generate center dot CF3 radical and enables MOF 1 to exhibit activity for trifluoromethylation of (hetero)arenes under visible light. The unusual stability of MOF 1 in the trifluoromethylation reactions can be attributed to its unique structure, which prevents it from corrosion by acid byproduct. The peeling of MOF 1 to ultrathin nanosheets or partial oxidation of Mn(II) to Mn(III) in MOF 1 led to MOL 1 and NB 1 with significant improved activity for trifluoromethylation reactions, demonstrating the important role of composition and morphology of a catalyst on its performance. The light initiated trifluoromethylation reactions over these Mn-based MOFs was applied to a variety of substrates. This study provides an efficient strategy for synthesis of trifluoromethylated compounds and highlights the potential of MOFs in light initiated organic syntheses.
Keyword ：
Acid tolerance Acid tolerance CF 3 radicals CF 3 radicals Mn-based MOF Mn-based MOF Photocatalysis Photocatalysis Trifluoromethylation Trifluoromethylation
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| GB/T 7714 | Ma, Xiong-Feng , Wen, Bo , Zhang, Shaohui et al. Stable Mn(II) metal-organic framework for efficient visible light initiated trifluoromethylation reaction [J]. | JOURNAL OF CATALYSIS , 2024 , 436 . |
| MLA | Ma, Xiong-Feng et al. "Stable Mn(II) metal-organic framework for efficient visible light initiated trifluoromethylation reaction" . | JOURNAL OF CATALYSIS 436 (2024) . |
| APA | Ma, Xiong-Feng , Wen, Bo , Zhang, Shaohui , Wang, Deshun , Wang, Lele , Lin, Huaxiang et al. Stable Mn(II) metal-organic framework for efficient visible light initiated trifluoromethylation reaction . | JOURNAL OF CATALYSIS , 2024 , 436 . |
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Abstract ：
The valorization of native lignin to functionalized aromatic compounds under visible light is appealing yet challenging. In this communication, colloidal mercaptoalkanoic acid capped ultrathin ZnIn2S4 (ZIS) microbelts was successfully fabricated, which was used as a superior catalyst for depolymerization of native lignin in birch woodmeal under visible light, with an optimum yield of 28.8 wt % to functionalized aromatic monomers achieved in 8 h. The capped mercaptoalkanoic acid not only enables a solvent modulated reversible interchange of ZIS between the colloidal state for efficient reaction and the aggregated state for facile separation, but also serves as a precursor for light initiated generation of reactive thiyl radical for highly selective cleavage of beta-O-4 bond in native lignin. This work provides a green and efficient strategy for the depolymerization of native lignin to functionalized aromatic monomers under mild conditions, which involves a new mechanism for the cleavage of beta-O-4 bonds in native lignin. The capability of cleavage of beta-O-4 bonds in native lignin by photogenerated thiyl radicals also demonstrates the great potential of using photogenerated thiyl radicals in organics transformations.
Keyword ：
Depolymerization Depolymerization Heterogeneous Catalysis Heterogeneous Catalysis Lignin Lignin Photochemistry Photochemistry Radicals Radicals
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| GB/T 7714 | Wang, Jiaqi , Li, Yaxin , Liu, Hurunqing et al. Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (37) . |
| MLA | Wang, Jiaqi et al. "Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 37 (2024) . |
| APA | Wang, Jiaqi , Li, Yaxin , Liu, Hurunqing , Ding, Zhengxin , Yuan, Rusheng , Li, Zhaohui . Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (37) . |
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Heterojunctions combining two photocatalysts of staggered conduction and valence band energy levels can increase the photocatalytic efficiency compared to their individual components. This activity enhancement is due to the minimization of undesirable charge recombination by the occurrence of carrier migration through the heterojunction interface with separated electrons and holes on the reducing and oxidizing junction component, respectively. Metal-organic frameworks (MOFs) are currently among the most researched photocatalysts due to their tunable light absorption, facile charge separation, large surface area and porosity. The present review summarizes the current state-of-the-art in MOF-based heterojunctions, providing critical comments on the construction of these heterostructures. Besides including examples showing the better performance of MOF heterojunctions for three important photocatalytic processes, such as hydrogen evolution reaction, CO2 photoreduction and dye decolorization, the focus of this review is on describing synthetic procedures to form heterojunctions with MOFs and on discussing the experimental techniques that provide evidence for the operation of charge migration between the MOF and the other component. Special attention has been paid to the design of rational MOF heterojunctions with small particle size and controlled morphology for an appropriate interfacial contact. The final section summarizes the achievements of the field and provides our views on future developments. The present review summarizes the current state-of-the-art in MOF-based heterojunctions in three important photocatalytic processes: hydrogen evolution reaction, CO2 photoreduction and photodegradation of dyes.
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| GB/T 7714 | Dhakshinamoorthy, Amarajothi , Li, Zhaohui , Yang, Sihai et al. Metal-organic framework heterojunctions for photocatalysis [J]. | CHEMICAL SOCIETY REVIEWS , 2024 , 53 (6) : 3002-3035 . |
| MLA | Dhakshinamoorthy, Amarajothi et al. "Metal-organic framework heterojunctions for photocatalysis" . | CHEMICAL SOCIETY REVIEWS 53 . 6 (2024) : 3002-3035 . |
| APA | Dhakshinamoorthy, Amarajothi , Li, Zhaohui , Yang, Sihai , Garcia, Hermenegildo . Metal-organic framework heterojunctions for photocatalysis . | CHEMICAL SOCIETY REVIEWS , 2024 , 53 (6) , 3002-3035 . |
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CdS/UiO-66-NH2 nanocomposite was solvothermally fabricated from cadmium acetate and the pre -synthesized UiO-66-NH2 in dimethyl sulfoxide (DMSO), which acted as the sulfur source. The as -obtained CdS/UiO-66-NH2 nanocomposite was immobilized on a glass fiber cloth (GF) and was applied for hydrogen sulfide (H2S) removal. The resultant GF immobilized CdS/UiO-66-NH2 nanocomposite exhibited a superior activity and high stability for H2S removal under visible light, in which UiO-66-NH2 acts as the main adsorbent and enriches H2S to promote CdS-based photocatalysis, while photocatalysis by CdS decomposes H2S adsorbed on UiO-66-NH2 to realize an in -situ regeneration of the adsorbent. The introduction of UiO-66-NH2 as the main adsorbent suppresses a fast deactivation of CdS due to an irreversible coordination between metal cation Cd2+ and H2S. This study not only developed a new type of material for fast and efficient removal of H2S, but also underscores the high potential of coupling physical adsorption and photocatalysis for the removal of volatile organic compounds (VOCs) and other gaseous pollutants in the environment.
Keyword ：
Adsorption Adsorption CdS CdS Hydrogen sulfide Hydrogen sulfide Photocatalysis Photocatalysis UiO-66-NH 2 UiO-66-NH 2
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| GB/T 7714 | Bai, Yaohui , Chen, Honghan , Cheng, Hao et al. Coupling physical adsorption and photocatalysis over CdS/UiO-66-NH2 for efficient removal of hydrogen sulfide [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
| MLA | Bai, Yaohui et al. "Coupling physical adsorption and photocatalysis over CdS/UiO-66-NH2 for efficient removal of hydrogen sulfide" . | SEPARATION AND PURIFICATION TECHNOLOGY 341 (2024) . |
| APA | Bai, Yaohui , Chen, Honghan , Cheng, Hao , Ding, Zhengxin , Yuan, Rusheng , Li, Zhaohui . Coupling physical adsorption and photocatalysis over CdS/UiO-66-NH2 for efficient removal of hydrogen sulfide . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
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The coupling between aryl halides and thiols to synthesize aryl thioethers via the formation of a C-S bond is an important reaction. In this manuscript, a Pd/ZnIn2S4 nanocomposite obtained via photoreduction of PdCl2(CH3CN)(2) in the presence of ZnIn2S4 was found to be an efficient bifunctional catalyst to realize the coupling reaction between thiophenols and aryl halides (X = Br and I) to yield aryl thioethers. A mechanism study reveals that the reaction involves the light-initiated generation of thiyl radicals as important intermediates. This reaction protocol can be applied to a wide range of substrate scopes, with moderate to excellent yields for the desired thioethers. This study provides a facile, green and economic strategy for the synthesis of aryl thioethers under mild conditions. This work also highlights the great potential of semiconductor-based photocatalysis in light-initiated organic syntheses.
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| GB/T 7714 | Liu, Hurunqing , Wang, Xinglin , Li, Zhaohui . Visible light-initiated cross-coupling between thiophenols and aryl halides (X = I and Br) to synthesize aryl thioethers over Pd/ZnIn2S4 [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2023 , 13 (3) : 917-924 . |
| MLA | Liu, Hurunqing et al. "Visible light-initiated cross-coupling between thiophenols and aryl halides (X = I and Br) to synthesize aryl thioethers over Pd/ZnIn2S4" . | CATALYSIS SCIENCE & TECHNOLOGY 13 . 3 (2023) : 917-924 . |
| APA | Liu, Hurunqing , Wang, Xinglin , Li, Zhaohui . Visible light-initiated cross-coupling between thiophenols and aryl halides (X = I and Br) to synthesize aryl thioethers over Pd/ZnIn2S4 . | CATALYSIS SCIENCE & TECHNOLOGY , 2023 , 13 (3) , 917-924 . |
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Carbon quantum dot (CQD)-decorated CdS nanocomposites were successfully fabricated via the self-assembly of CdS in the presence of preformed CQDs and were found to be efficient photocatalysts for the hydrogenation of nitrobenzene under visible light. Due to the presence of the frustrated Lewis acid-base pairs (FLPs) in their structure, CQDs act as an efficient catalyst to promote the proton-coupled hydrogenation of nitrobenzene over CQDs/CdS nanocomposites. Controllable and chemoselective hydrogenation of nitrobenzene to produce aniline, azoxybenzene, azobenzene and hydrazobenzene can be realized over CQDs/CdS via simply regulating the reaction medium including the hydrogen source, the solvent and the alkalinity. This study provides a highly efficient and economical photocatalytic system for the controllable and chemoselective hydrogenation of nitrobenzene under visible light. This work also highlights the great potential of semiconductor-based photocatalysis in light-initiated organic syntheses. Visible light-initiated chemoselective hydrogenation of nitrobenzene into different products is realized over CQDs/CdS via simply regulating the reaction medium.
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| GB/T 7714 | Liu, Hurunqing , Deng, Zirong , Wang, Bingqing et al. Efficient visible light-initiated hydrogenation of nitrobenzene for chemoselective production of aniline, azoxybenzene, azobenzene and hydrazobenzene over CQDs/CdS nanocomposites [J]. | DALTON TRANSACTIONS , 2023 , 52 (37) : 13129-13136 . |
| MLA | Liu, Hurunqing et al. "Efficient visible light-initiated hydrogenation of nitrobenzene for chemoselective production of aniline, azoxybenzene, azobenzene and hydrazobenzene over CQDs/CdS nanocomposites" . | DALTON TRANSACTIONS 52 . 37 (2023) : 13129-13136 . |
| APA | Liu, Hurunqing , Deng, Zirong , Wang, Bingqing , Ding, Zhengxin , Li, Zhaohui . Efficient visible light-initiated hydrogenation of nitrobenzene for chemoselective production of aniline, azoxybenzene, azobenzene and hydrazobenzene over CQDs/CdS nanocomposites . | DALTON TRANSACTIONS , 2023 , 52 (37) , 13129-13136 . |
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Ternary NiTiFe-LDH with an ultrathin nanosheet morphology was successfully fabricated via a facile co-precipitation method, followed by refluxing, and was used as a catalyst for oxidative coupling of amines to produce imines under visible light. The obvious superior activity observed in NiTiFe-LDH ultrathin nanosheets compared with binary NiTi-LDH and bulk NiTiFe-LDH can be ascribed to an enhanced light absorption capability caused by the introduction of Fe3+ ions as well as the ultrathin nanosheets which can minimize the recombination of the photogenerated charge carriers and provide more catalytically active sites for the reaction. As a result, more catalytically active O2- radicals are generated over NiTiFe-LDH ultrathin nanosheets, which leads to their superior activity. This study not only shows the possibility of using LDHs in photocatalytic organic transformations but also demonstrates an effective strategy to promote the activity of LDH-based photocatalysts via simultaneous composition and morphology modulation of LDHs. Due to the introduced Fe3+ for enhanced light absorption and the ultrathin nanosheets to minimize the recombination of photogenerated charge carriers, NiTiFe-LDH NSs exhibit superior activity for conversion of amines to imines under visible light.
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| GB/T 7714 | Li, Shaojin , Wang, Jiaqi , Liu, Hurunqing et al. Facile fabrication of ternary NiTiFe-LDH ultrathin nanosheets for efficient conversion of amines into imines under visible light [J]. | DALTON TRANSACTIONS , 2023 , 53 (3) : 1040-1047 . |
| MLA | Li, Shaojin et al. "Facile fabrication of ternary NiTiFe-LDH ultrathin nanosheets for efficient conversion of amines into imines under visible light" . | DALTON TRANSACTIONS 53 . 3 (2023) : 1040-1047 . |
| APA | Li, Shaojin , Wang, Jiaqi , Liu, Hurunqing , Li, Zhaohui . Facile fabrication of ternary NiTiFe-LDH ultrathin nanosheets for efficient conversion of amines into imines under visible light . | DALTON TRANSACTIONS , 2023 , 53 (3) , 1040-1047 . |
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