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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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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 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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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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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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PtS/ZnIn2S4 nanocomposites are obtained via a microwave-assisted synthesis followed by a photoreduction. The resultant PtS/ZnIn2S4 nanocomposites are used as an effective multifunctional photocatalyst for the reaction between alcohols and o-aminobenzamide to coproduce quinazolinones and hydrogen under visible light, via a cascade alcohols/aldehydes transformation, condensation between aldehydes and o-aminobenzamide, as well as the dehydrogenation/cyclization to produce quinazolinones. PtS acts as an efficient cocatalyst to promote the dehydrogenation of both the alcohols and the condensation intermediates for the production of quinazolinones. An almost complete conversion of o-aminobenzamide was achieved in 24 h, with a yield of 98.8% to 2-phenyl-quinazline-4(3H)-one and quantitative hydrogen produced over PtS/ZnIn2S4 after irradiated for 24 h. The apparent quantum yield at 450 nm is determined to 15.2%. The superior activity observed over PtS/ZnIn2S4 nanocomposite as compared with that over either NiS/ZnIn2S4 or MoS2/ZnIn2S4 can be ascribed to a moderate binding between PtS and the surface adsorbed H*. This study supplies an effective, green, and atom-economic strategy for the synthesis of quinazolinones with coproduction of hydrogen under visible light. This work also demonstrates the high potential of fabrication of metal sulfide-based multifunctional catalysts for light-driven one-pot tandem/cascade reactions.
Keyword ：
multifunctionality multifunctionality PtS PtS quinazolinones quinazolinones visible light visible light ZnIn2S4 ZnIn2S4
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| GB/T 7714 | Du, Xiao , Wang, Jiaqi , Liu, Hurunqing et al. Visible-Light-Initiated Dehydrogenative Cyclization of o-Aminobenzamide and Alcohols for Coproduction of Quinazolinones and Hydrogen over PtS/ZnIn2S4 [J]. | SOLAR RRL , 2023 , 7 (24) . |
| MLA | Du, Xiao et al. "Visible-Light-Initiated Dehydrogenative Cyclization of o-Aminobenzamide and Alcohols for Coproduction of Quinazolinones and Hydrogen over PtS/ZnIn2S4" . | SOLAR RRL 7 . 24 (2023) . |
| APA | Du, Xiao , Wang, Jiaqi , Liu, Hurunqing , Yuan, Rusheng , Li, Zhaohui . Visible-Light-Initiated Dehydrogenative Cyclization of o-Aminobenzamide and Alcohols for Coproduction of Quinazolinones and Hydrogen over PtS/ZnIn2S4 . | SOLAR RRL , 2023 , 7 (24) . |
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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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面对全球能源短缺和环境污染等问题,发展绿色、可持续的能源来替代传统的化石能源成为迫切需求.太阳能作为一种清洁可再生能源,其有效转化与利用受到了广泛关注.光催化将太阳能转化为化学能,其核心是新型高效的光催化材料.金属有机框架材料(MOFs),是一类由金属或金属节点与多齿有机配体相互连接而成的微介孔材料,具有独特的组成结构和特性,有望成为有应用前景的光催化材料.目前已有一些关于MOFs基光催化的综述,但考虑到该领域在过去几年迅速发展,为了研发高效的MOFs基光催化材料,非常有必要对已经报道的用于提高MOFs基光催化剂性能的策略进行总结. 本综述重点总结了己报道的通过调控MOFs基材料的组成和结构的策略来提升其光催化性能的最新研究进展.首先,简要介绍了MOFs基材料的结构特点及其在光催化领域应用的优势,阐述了MOFs基材料光催化的基本原理,提出了影响其光催化性能的关键因素,包括光吸收能力、光生载流子的分离和迁移以及催化活性位点.其次,阐明不同结构调控策略通过优化关键因素进而提高光催化性能的原理,具体包括MOFs基材料中金属掺杂、配体功能化、超薄二维材料构筑以及缺陷工程策略.然后,通过总结典型案例,详细讨论了上述策略如何通过调控MOFs基材料的组成和结构来优化关键因素,从而提高MOFs基材料的光催化性能.最后,针对MOFs基材料光催化所面临的机遇、挑战及其发展趋势提出展望:(1)影响MOFs基光催化剂效率的因素是多方面的,因此将不同策略相结合有利于更好地提高MOFs基光催化剂的性能.除了本文总结的四种构筑策略,最近其它一些关于提升MOFs基材料光催化性能的结构调控策略也有零星报道,如微环境调控、晶面工程等,也值得进一步关注.(2)与无机半导体光催化剂相比,MOFs基材料的结构稳定性较差,因此应特别注意其在光催化条件下的稳定性,特别是MOFs基材料在水中的反应体系.(3)先进原位表征技术的发展和理论研究的深化对于高效MOF基光催化系统的设计及机理研究至关重要.(4)MOFs基材料的多功能性可以使其作为光诱导一锅多步反应的多功能催化材料,应大力开展研究. 综上,本文系统地总结了通过调控MOFs基材料的组成和结构从而达到提升其光催化性能的不同策略,并就MOFs基材料光催化所面临的机遇、挑战及其发展趋势提出展望.希望本文能够为深入了解MOFs基光催化体系中组成-结构-性能关系以及从原子水平来设计研发高效的MOFs基光催化剂提供参考.
Keyword ：
光催化 光催化 缺陷工程 缺陷工程 超薄二维MOFs 超薄二维MOFs 配体功能化 配体功能化 金属掺杂 金属掺杂 金属有机框架 金属有机框架
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| GB/T 7714 | 刘成 , 刘胡润卿 , 余济美 et al. 高效光催化金属有机框架(MOFs)的构筑策略 [J]. | 催化学报 , 2023 , 55 (12) : 1-19 . |
| MLA | 刘成 et al. "高效光催化金属有机框架(MOFs)的构筑策略" . | 催化学报 55 . 12 (2023) : 1-19 . |
| APA | 刘成 , 刘胡润卿 , 余济美 , 吴棱 , 李朝辉 . 高效光催化金属有机框架(MOFs)的构筑策略 . | 催化学报 , 2023 , 55 (12) , 1-19 . |
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2D Ni-Fe-MOF ultrathin nanosheets (NSs), with dimensions of ca. 1.0 mu m and thickness of ca. 5.0 nm, were successfully fabricated. Small-sized Pd nanoparticles of ca. 3.0 nm were deposited on 2D Ni-Fe-MOF NSs to afford Pd/Ni-Fe-MOF NSs, which were used as an efficient multifunctional catalyst to realize the N-alkylation reactions of amines by alcohols under visible light. The superior performance observed over the resultant Pd/Ni-Fe-MOF NSs as compared with Pd/bulk Ni-Fe-MOF, their 3D counterpart, can be ascribed to the ultrathin nanosheet morphology of 2D Ni-Fe-MOF NSs, which not only shortens the transportation path for the photogenerated charge carriers, but also can provide more efficient interaction between the active site and substrates. This work provides a green and sustainable strategy for the production of secondary amines using alcohols as the alkylating agent. This study also demonstrates the unique advantages of 2D MOF ultrathin nanosheets in the fabrication of multifunctional catalytic systems for light initiated one-pot tandem/cascade reactions.
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| GB/T 7714 | Yuan, Yun , Wang, Jiaqi , Liu, Hurunqing et al. Deposition of Pd nanoparticles on 2D Ni-Fe-MOF ultrathin nanosheets for efficient N-alkylation of amines by alcohols under visible light [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2023 , 11 (44) : 24127-24135 . |
| MLA | Yuan, Yun et al. "Deposition of Pd nanoparticles on 2D Ni-Fe-MOF ultrathin nanosheets for efficient N-alkylation of amines by alcohols under visible light" . | JOURNAL OF MATERIALS CHEMISTRY A 11 . 44 (2023) : 24127-24135 . |
| APA | Yuan, Yun , Wang, Jiaqi , Liu, Hurunqing , Li, Zhaohui . Deposition of Pd nanoparticles on 2D Ni-Fe-MOF ultrathin nanosheets for efficient N-alkylation of amines by alcohols under visible light . | JOURNAL OF MATERIALS CHEMISTRY A , 2023 , 11 (44) , 24127-24135 . |
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