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学者姓名：吴棱
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Abstract ：
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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A series of Al3+-doped UiO-66(Ce) MOFs (U(CexAl1−x)) was developed to reveal the roles of metal doping on active site formation and substrate activation in photocatalytic selective transformation of amines to imines. Al3+ doping induced crystal structure distortion to form coordinately unsaturated metal (Al, Ce) sites as Lewis acid sites to chemisorb and activate benzylamine (BA). In situ FTIR revealed that the Al site with stronger acid strength facilitated BA activation. The activation degree of N–H bonds in BA was evaluated by changes of calculated force constant. The intermediate products were confirmed through time-dependent in situ FTIR. The Al3+-doped sample U(Ce0.90Al0.10), the optimal catalyst, showed a significantly increased BA conversion (97.6 %) than that (47.5 %) of undoped sample, which was attributed to enough active sites and the optimal charge mobility. Finally, the present study proposes a synergistic photocatalytic mechanism associated with molecular activation to demonstrate selective oxidation pathways at the molecular level. © 2024 Elsevier Inc.
Keyword ：
Active sites Active sites Metal doping Metal doping Photocatalysis Photocatalysis UiO-66(Ce) UiO-66(Ce)
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| GB/T 7714 | Liu, C. , Chen, H. , Chen, Q. et al. Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis [J]. | Journal of Catalysis , 2024 , 437 . |
| MLA | Liu, C. et al. "Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis" . | Journal of Catalysis 437 (2024) . |
| APA | Liu, C. , Chen, H. , Chen, Q. , Bi, J. , Yu, J.C. , Wu, L. . Active site modulation in UiO-66(Ce) MOFs by Al3+ doping for boosting photocatalysis . | Journal of Catalysis , 2024 , 437 . |
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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 . |
| MLA | Liu, Cheng et al. "The defect-modulated UiO-66(Ce) MOFs for enhancing photocatalytic selective organic oxidations" . | RARE METALS (2024) . |
| 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 . |
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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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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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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.本综述重点总结了已报道的通过调控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...
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（英文） [J]. | Chinese Journal of Catalysis , 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（英文）" . | Chinese Journal of Catalysis 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（英文） . | Chinese Journal of Catalysis , 2023 , 55 (12) , 1-19 . |
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Abstract ：
Photocatalysis, a promising technology to convert solar energy to chemical energy, is expected to relieve the global energy shortage and environmental pollution and therefore has attracted widespread recent research attention. Metal-organic frameworks (MOFs), a class of micro-mesoporous hybrid material constructed from metal or metal nodes interconnected with multi-dentated organic linkers, have recently been demonstrated to be promising photocatalysts for a variety of reactions relevant to environmental and energy concerns due to their unique structure and characteristics. Considering that MOF-based photocatalysis burgeoned rapidly during the past several years, and with an aim to develop more efficient MOF-based photocatalytic materials, it is still necessary to summarize the strategies already reported to improve the performance of MOF-based photocatalytic materials, even though several excellent reviews on MOF-based photocatalysis have already been published. In this review, four structural engineering strategies to improve the efficiency of MOF-based photocatalysis have been summarized. These strategies include metal doping, ligand functionalization, the fabrication of ultrathin 2D MOFs, and defect engineering. These methods aim to enhance light absorption, improve charge separation and transportation, and create more catalytic active sites. Personal opinions on the opportunities, challenges, and developing trends of MOF-based photocatalysis were addressed. This review aims to provide guidance for the rational development of advanced MOF-based photocatalysts by elucidating the inherent relationship between their structural properties and catalytic activity. Published by Elsevier B.V. All rights reserved.
Keyword ：
Defect engineering Defect engineering Ligand functionalization Ligand functionalization Metal doping Metal doping Metal-organic framework Metal-organic framework Photocatalysis Photocatalysis Ultrathin 2D MOFs Ultrathin 2D MOFs
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| GB/T 7714 | Liu, Cheng , Liu, Hurunqing , Yu, Jimmy C. et al. Strategies to engineer metal-organic frameworks for efficient photocatalysis [J]. | CHINESE JOURNAL OF CATALYSIS , 2023 , 55 : 1-19 . |
| MLA | Liu, Cheng et al. "Strategies to engineer metal-organic frameworks for efficient photocatalysis" . | CHINESE JOURNAL OF CATALYSIS 55 (2023) : 1-19 . |
| APA | Liu, Cheng , Liu, Hurunqing , Yu, Jimmy C. , Wu, Ling , Li, Zhaohui . Strategies to engineer metal-organic frameworks for efficient photocatalysis . | CHINESE JOURNAL OF CATALYSIS , 2023 , 55 , 1-19 . |
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The social recommender system can accurately recommend information to users, according to their interests based on the characteristics of their social network, however, the interaction between users has not been fully captured in the existing social recommender systems. This study contributes to the literature by proposing a social recommendation method on the basis of opinion dynamics, which captures the information on the interactions between target users and opinion leaders. In our model, the impact of opinion leaders and the evolutionary opinion dynamics between opinion leaders and the target user are integrated to make a recommendation. Experiments based on two real rating datasets, Epinions and FilmTrust were conducted to test the proposed model. The results show that our proposed method can effectively solve the cold-start problem and outperforms the baseline models.
Keyword ：
Opinion dynamics Opinion dynamics Opinion leaders Opinion leaders Probabilistic matrix factorization Probabilistic matrix factorization Recommendation algorithm Recommendation algorithm Social recommender system Social recommender system
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| GB/T 7714 | Weng, Lijuan , Zhang, Qishan , Lin, Zhibin et al. Integrating interactions between target users and opinion leaders for better recommendations: An opinion dynamics approach [J]. | COMPUTER COMMUNICATIONS , 2023 , 198 : 98-107 . |
| MLA | Weng, Lijuan et al. "Integrating interactions between target users and opinion leaders for better recommendations: An opinion dynamics approach" . | COMPUTER COMMUNICATIONS 198 (2023) : 98-107 . |
| APA | Weng, Lijuan , Zhang, Qishan , Lin, Zhibin , Wu, Ling , Zhang, Jin-Hua . Integrating interactions between target users and opinion leaders for better recommendations: An opinion dynamics approach . | COMPUTER COMMUNICATIONS , 2023 , 198 , 98-107 . |
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ZnIn2S4 ultrathin 2D nanosheets with a positive surface charge are synthesized by a hydrothermal method and different contents of surface S vacancies are induced via heat treatment of as-prepared ZnIn2S4 (ZIS). As the S vacancies contents increased, the photocatalytic degradation efficiency of ceftriaxone (CTRX) sodium is promoted. Especially, ZIS-300 shows the best degradation efficiency (88.8%) for an initial CTRX concentration of 10 mg L-1 in 2 h. It is found that S vacancies cause the electron density of surface metal atoms (Zn, In) to be decreased, which makes the effective adsorption and activation of ceftriaxone anions through electrostatic adsorption interactions. Meanwhile, S vacancies also serve as active centers to promote the absorption of O-2 and gather electrons to form center dot O-2(-) species. The photogenerated holes quickly transfer to the surface of the catalyst to directly degrade the adsorbed CTRX. Thus, the photocatalytic CTRX degradation efficiency is significantly improved. Finally, a possible mechanism for over defective ZIS is proposed. This work provides a feasible strategy for the efficient degradation of antibiotics from the perspective of electrostatic adsorption and molecule activation.
Keyword ：
Electrostatic interaction Electrostatic interaction O-2 activation O-2 activation S vacancies S vacancies The degradation of ceftriaxone sodium The degradation of ceftriaxone sodium ZnIn2S4 ultrathin Nanosheets ZnIn2S4 ultrathin Nanosheets
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| GB/T 7714 | Zhang, Chen , Shi, Yingzhang , Wang, Zhiwen et al. Electrostatic interaction and surface S vacancies synergistically enhanced the photocatalytic degradation of ceftriaxone sodium [J]. | CHEMOSPHERE , 2023 , 311 . |
| MLA | Zhang, Chen et al. "Electrostatic interaction and surface S vacancies synergistically enhanced the photocatalytic degradation of ceftriaxone sodium" . | CHEMOSPHERE 311 (2023) . |
| APA | Zhang, Chen , Shi, Yingzhang , Wang, Zhiwen , Liu, Cheng , Hou, Yidong , Bi, Jinhong et al. Electrostatic interaction and surface S vacancies synergistically enhanced the photocatalytic degradation of ceftriaxone sodium . | CHEMOSPHERE , 2023 , 311 . |
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Bi2MoO6 hierarchical microspheres (BMO-SP) consisting of monolayer nanosheets with abundant surface oxygen defects and unsaturated Mo sites are constructed for the one-pot synthesis of secondary amine via a photocatalytic coupling reaction of nitrobenzene (NB) and benzyl alcohol (BA). The performance of this photocatalyst is 12 times higher than that of bulk Bi2MoO6 (BMO-bulk). Experiment results and density functional theory calculations reveal that surface oxygen defects induce more unsaturated Mo atoms facilitating the coordination activation of NB and BA molecules through the formation of -N-O center dot center dot center dot Mo and -C-O-Mo coordination, respectively. The surface oxygen defects also promote the separation of photogenerated carriers. More photogenerated holes transfer to the surface for oxidizing the activated BA while the photogenerated electrons are trapped by oxygen defects for reducing NB. Thus, the photo-catalytic performance is markedly improved. This work successfully designs an efficient photocatalyst for the tandem reaction via surface defect engineering.(c) 2023 Elsevier Ltd. All rights reserved.
Keyword ：
Coordination activation Coordination activation Hierarchical Bi 2 MoO 6 microspheres Hierarchical Bi 2 MoO 6 microspheres Nitrobenzene and benzyl alcohol Nitrobenzene and benzyl alcohol Photocatalysis Photocatalysis Surface defect engineering Surface defect engineering
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| GB/T 7714 | Shi, Yingzhang , Xie, Ke , Wang, Zhiwen et al. Defect engineering mediated molecules coordination activation for one-pot synthesis of secondary amine over Bi2MoO6 hierarchical microspheres [J]. | CHEMICAL ENGINEERING SCIENCE , 2023 , 275 . |
| MLA | Shi, Yingzhang et al. "Defect engineering mediated molecules coordination activation for one-pot synthesis of secondary amine over Bi2MoO6 hierarchical microspheres" . | CHEMICAL ENGINEERING SCIENCE 275 (2023) . |
| APA | Shi, Yingzhang , Xie, Ke , Wang, Zhiwen , Liu, Cheng , Lin, Sen , Wu, Ling et al. Defect engineering mediated molecules coordination activation for one-pot synthesis of secondary amine over Bi2MoO6 hierarchical microspheres . | CHEMICAL ENGINEERING SCIENCE , 2023 , 275 . |
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