المؤلفون: Lv, Yang, Han, Miaomiao, Gong, Wanbing, Wang, Dongdong, Chen, Chun, Wang, Guozhong, Zhang, Haimin, Zhao, Huijun

مصطلحات موضوعية: Chemical sciences, Cinnamaldehyde, Fe-Co nanoalloys, H2O solvent, Metal-organic frameworks, selective hydrogenation

الوصف: Selective hydrogenation of C=O against the conjugated C=C in cinnamaldehyde (CAL) is indispensable to produce cinnamyl alcohol (COL), nonetheless, challenged by the low selectivity and the need to use organic solvents. Herein, for the first time, we report the use of Fe-Co alloy nanoparticles (NPs) on N-doped carbon support as a selective hydrogenation catalyst to efficiently convert CAL to COL. The resultant catalyst with the optimized Fe/Co ratio of 0.5 can achieve an exceptional COL selectivity of 91.7% at a CAL conversion of 95.1% in pure water medium under mild reaction conditions, ranking it the best performed catalyst reported to date. The experimental results confirm that the COL selectivity and CAL conversion efficiency are respectively promoted by the presence of Co and Fe, while the synergism of the alloyed Fe-Co is the key to concurrently achieve high COL selectivity and CAL conversion efficiency . ; Full Text

العلاقة: Angewandte Chemie International Edition; Lv, Y; Han, M; Gong, W; Wang, D; Chen, C; Wang, G; Zhang, H; Zhao, H, Fe-Co Alloyed Nanoparticles Catalyzing Efficient Hydrogenation of Cinnamaldehyde to Cinnamyl Alcohol in Water, Angewandte Chemie International Edition, 2020, 59 (52), pp. 23521-23526; http://hdl.handle.net/10072/397730Test

الإتاحة: https://doi.org/10.1002/anie.202009913Test
http://hdl.handle.net/10072/397730Test

المؤلفون: Bindra, Anivind Kaur, Wang, Dongdong, Zhao, Yanli

المساهمون: School of Chemistry, Chemical Engineering and Biotechnology

مصطلحات موضوعية: Science::Chemistry, Hybrids, Metal–Organic Frameworks

الوصف: Metal–organic frameworks (MOFs) have been at the forefront of nanotechnological research for the past decade owing to their high porosity, high surface area, diverse configurations, and controllable chemical structures. They are a rapidly developing class of nanomaterials that are predominantly applied in batteries, supercapacitors, electrocatalysis, photocatalysis, sensors, drug delivery, gas separation, adsorption, and storage. However, the limited functions and unsatisfactory performance of MOFs resulting from their low chemical and mechanical stability hamper further development. Hybridizing MOFs with polymers is an excellent solution to these problems, because polymers—which are soft, flexible, malleable, and processable—can induce unique properties in the hybrids based on those of the two disparate components while retaining their individuality. This review highlights recent advances in the preparation of MOF–polymer nanomaterials. Furthermore, several applications wherein the incorporation of polymers enhances the MOF performance are discussed, such as anticancer therapy, bacterial elimination, imaging, therapeutics, protection from oxidative stress and inflammation, and environmental remediation. Finally, insights from the focus of existing research and design principles for mitigating future challenges are presented. ; Agency for Science, Technology and Research (A*STAR) ; National Research Foundation (NRF) ; Submitted/Accepted version ; This research work was supported by the Singapore Agency for Sci-ence, Technology and Research (A*STAR) AME IRG grant (A20E5c0081)and the Singapore National Research Foundation Investigatorship (NRF-NRFI2018-03).

وصف الملف: application/pdf

العلاقة: A20E5c0081; NRF-NRFI2018-03; Advanced Materials; Bindra, A. K., Wang, D. & Zhao, Y. (2023). Metal–organic frameworks meet polymers: from synthesis strategies to healthcare applications. Advanced Materials, 35(40), 2300700-. https://dx.doi.org/10.1002/adma.202300700Test; https://hdl.handle.net/10356/170860Test; 40; 35; 2300700

الإتاحة: https://doi.org/10.1002/adma.202300700Test
https://hdl.handle.net/10356/170860Test

المؤلفون: Yang, Guangbao, Bindra, Anivind Kaur, Phua, Soo Zeng Fiona, Liu, Jiawei, Wu, Hongwei, Wang, Dongdong, Qian, Cheng, Liu, Guofeng, Zhao, Yanli

المصدر: Advanced Optical Materials; 6/15/2023, Vol. 11 Issue 11, p1-10, 10p

مصطلحات موضوعية: METAL-organic frameworks, REACTIVE oxygen species, TUMOR treatment, PHOTODYNAMIC therapy, SERUM albumin, HYPOXEMIA

مستخلص: Photodynamic therapy (PDT), as a noninvasive therapeutic tool, can result in a high level of hypoxia in tumors. Herein, hypoxia‐responsive nanoscale metal‐organic frameworks (UiO‐AZB) are prepared, which contain an azo group in its organic linker. After modifying the surface of UiO‐AZB with chlorin e6 (Ce6)‐conjugated human serum albumin (HSA), tirapazamine (TPZ) is employed as a hypoxia‐activated prodrug to be encapsulated into UiO‐AZB. The obtained nanosystem (UiO‐AZB/HC‐TPZ) can efficiently produce singlet oxygen under 660 nm light irradiation and cause severe hypoxia in tumors. This process in turn triggers the degradation of the frameworks and controllable release of activated TPZ for chemotherapy, finally leading to improved antitumor treatment through combinational PDT and hypoxia‐activated chemotherapy. This research demonstrates a distinctive treatment strategy, that is, using a simple stimulus (light irradiation) to trigger a series of activities (PDT, disintegration of UiO‐AZB structure, activation of TPZ, and controllable release) for realizing an effective treatment of tumors. [ABSTRACT FROM AUTHOR]

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المؤلفون: Wang, Dongdong^1,2 (AUTHOR) wangdd13@ustc.edu.cn, Zhang, Lei¹ (AUTHOR), Wang, Changlai³ (AUTHOR), Cheng, Zhiyu³ (AUTHOR), Zheng, Wei³ (AUTHOR), Xu, Pengping³ (AUTHOR), Chen, Qianwang^1,3 (AUTHOR) cqw@ustc.edu.cn, Zhao, Yanli² (AUTHOR) zhaoyanli@ntu.edu.sg

المصدر: Angewandte Chemie International Edition. 5/2/2023, Vol. 62 Issue 19, p1-10. 10p.

مصطلحات موضوعية: *SYNTHETIC enzymes, *PLATINUM nanoparticles, *REACTIVE oxygen species, *COMPANION diagnostics, *METAL-organic frameworks, *PHOTODYNAMIC therapy, *PHOTOSENSITIZERS

مستخلص: Conventional nanozymes often possess low active site density. Pursuing effective strategies for constructing highly active single‐atomic nanosystems with maximum atom utilization efficiency is exceptionally attractive. Herein, we develop a facile "missing‐linker‐confined coordination" strategy to fabricate two self‐assembled nanozymes, i.e. conventional nanozyme (NE) and single‐atomic nanozyme (SAE), which respectively consist of Pt nanoparticles and single Pt atoms as active catalytic sites anchored in metal–organic frameworks (MOFs) with encapsulated photosensitizers for catalase‐mimicking enhanced photodynamic therapy. Compared to a Pt nanoparticle‐based conventional nanozyme, a Pt single‐atomic nanozyme shows enhanced catalase‐mimicking activity in generating oxygen for overcoming tumor hypoxia, thus exhibiting a more efficient reactive oxygen species generation and high tumor inhibition rate. [ABSTRACT FROM AUTHOR]

المؤلفون: Wang, Dongdong, Wu, Huihui, Yang, Guangbao, Qian, Cheng, Gu, Long, Wang, Hou, Zhou, Weiqiang, Liu, Jiawei, Wu, Yinglong, Zhang, Xiaodong, Guo, Zhen, Chen, Hongzhong, Jana, Deblin, Zhao, Yanli

المساهمون: School of Physical and Mathematical Sciences

مصطلحات موضوعية: Science::Medicine, Glutathione, Metal-organic Frameworks

الوصف: Intracellular antioxidants such as glutathione (GSH) play a critical role in protecting malignant tumor cells from apoptosis induced by reactive oxygen species (ROS) and in mechanisms of multidrug and radiation resistance. Herein, we rationally design two multicomponent self-assembled photodynamic therapy (PDT) nanoagents, that is, Glup-MFi-c and Glud-MFo-c, which consist of respective GSH-passivation and GSH-depletion linkers in metal−organic frameworks encapsulated with photosensitizers for a deeply comprehensive understanding of GSH-based tumor PDT. Multicomponent coordination, π−π stacking, and electrostatic interactions among metal ions, photosensitizers, and bridging linkers under the protection of a biocompatible polymer generate homogeneous nanoparticles with satisfied size, good colloid stability, and ultrahigh loading capacity. Compared to the GSH-passivated Glup-MFi-c, the GSH-depleted Glud-MFo-c shows pH-responsive release of photosensitizer and [FeIII(CN)6] linker in tumor cells to efficiently deplete intracellular GSH, thus amplifying the cell-killing efficiency of ROS and suppressing the tumor growth in vivo. This study demonstrates that Glud-MFo-c acts as a ROS amplifier, providing a useful strategy to deeply understand the role of GSH in combating cancer. ; Ministry of Education (MOE) ; National Research Foundation (NRF) ; Accepted version ; This research is supported by the Singapore National Research Foundation Investigatorship (NRF-NRFI2018-03), the Singapore Academic Research Fund (RT12/19), the National Natural Science Foundation of China (31471268), and the National Key Research and Development Program of China (Stem Cell and Translational Research, 2016YFA0101202).

وصف الملف: application/pdf

العلاقة: ACS Nano; Wang, D., Wu, H., Yang, G., Qian, C., Gu, L., Wang, H., . Zhao, Y. (2020). Metal−organic framework derived multicomponent nanoagent as a reactive oxygen species amplifier for enhanced photodynamic therapy. ACS Nano, 14(10), 13500–13511. doi:10.1021/acsnano.0c05499; https://hdl.handle.net/10356/146323Test; 10; 14; 13500; 13511

الإتاحة: https://doi.org/10.1021/acsnano.0c05499Test
https://hdl.handle.net/10356/146323Test

المؤلفون: Wang, Dongdong¹ (AUTHOR), He, Isabel Wenjia¹ (AUTHOR), Liu, Jiawei¹ (AUTHOR), Jana, Deblin¹ (AUTHOR), Wu, Yinglong¹ (AUTHOR), Zhang, Xiaodong¹ (AUTHOR), Qian, Cheng¹ (AUTHOR), Guo, Yi¹ (AUTHOR), Chen, Xiaokai¹ (AUTHOR), Bindra, Anivind Kaur¹ (AUTHOR), Zhao, Yanli^1,2 (AUTHOR) zhaoyanli@ntu.edu.sg

المصدر: Angewandte Chemie International Edition. 12/6/2021, Vol. 60 Issue 50, p26254-26259. 6p.

مصطلحات موضوعية: *CANCER treatment, *REACTIVE oxygen species, *CATALYSTS, *CYANIDES, *PHOTODYNAMIC therapy, *METAL-organic frameworks, *NANOMEDICINE, *GLUTATHIONE

مستخلص: Clinical translation of artesunate (ATS) as a potent antitumor drug has been obstructed by its rapid degradation and low bioavailability. Herein, we report the development of an ATS nanomedicine through the self‐assembly with Mn[Co(CN)6]2/3□1/3 metal–organic frameworks (MOFs) that have hidden missing linkers. The defects in MOFs originating from the missing linkers play a key role in increasing the biological stability and tumor accumulation of ATS. Chlorin e6 (Ce6) and ATS can be co‐loaded into MOFs for a synergistic antitumor efficacy. In the presence of intracellular HCO3−, Mn2+ acts as an efficient catalyst to promote the bicarbonate‐activated H2O2 system which oxidizes ATS to generate reactive oxygen species and induce oxidative death to cancer cells. The released [CoIII(CN)6] linker undergoes a redox reaction with intracellular glutathione to prevent the scavenging ability of reactive oxygen species, contributing to synergistic chemodynamic therapy of ATS and photodynamic therapy of Ce6. Thus, defect‐engineered MOFs with hidden missing linkers hold great promise in advancing the practical use of ATS as an antitumor medicine. [ABSTRACT FROM AUTHOR]

المؤلفون: Zhou, Weiqiang, Teo, Wei Liang, Phua, Soo Zeng Fiona, Xi, Shibo, Chen, Bo, Jana, Deblin, Wang, Dongdong, Qian, Cheng, Wang, Hou, Zhang, Hua, Zhao, Yanli

المصدر: Small Methods; 5/11/2020, Vol. 4 Issue 5, p1-8, 8p

مصطلحات موضوعية: METAL-organic frameworks, AQUEOUS solutions, METAL catalysts, CATALYTIC activity, PRECIOUS metals, DEOXYGENATION

مستخلص: Deactivation of noble metal catalysts often occurs in many hydrocarbon reactions. In particular, sulfur species may cause significant poisoning of metal catalysts, even at minimal concentration, due to strong metal–S bond formation. In this work, hierarchical porous composites are prepared by integrating melamine foam with metal–organic frameworks, demonstrating excellent catalytic activity with anti‐sulfur poisoning properties. Several techniques are employed to elucidate the mechanism of anti‐sulfur poisoning. This study offers a functional composite system capable of acting as sulfur‐resistant noble metal catalysts in solution. [ABSTRACT FROM AUTHOR]

: Copyright of Small Methods is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)

المؤلفون: Wang, Dongdong, Wu, Huihui, Phua, Soo Zeng Fiona, Yang, Guangbao, Qi Lim, Wei, Gu, Long, Qian, Cheng, Wang, Haibao, Guo, Zhen, Chen, Hongzhong, Zhao, Yanli

المصدر: Nature Communications; 1/17/2020, Vol. 11 Issue 1, p1-13, 13p

مصطلحات موضوعية: PHOTODYNAMIC therapy, TUMOR treatment, REACTIVE oxygen species, TUMOR microenvironment, METAL-organic frameworks, COORDINATE covalent bond

مستخلص: Hypoxia of solid tumor compromises the therapeutic outcome of photodynamic therapy (PDT) that relies on localized O2 molecules to produce highly cytotoxic singlet oxygen (¹O2) species. Herein, we present a safe and versatile self-assembled PDT nanoagent, i.e., OxgeMCC-r single-atom enzyme (SAE), consisting of single-atom ruthenium as the active catalytic site anchored in a metal-organic framework Mn3[Co(CN)6]2 with encapsulated chlorin e6 (Ce6), which serves as a catalase-like nanozyme for oxygen generation. Coordination-driven self-assembly of organic linkers and metal ions in the presence of a biocompatible polymer generates a nanoscale network that adaptively encapsulates Ce6. The resulted OxgeMCC-r SAE possesses well-defined morphology, uniform size distribution and high loading capacity. When conducting the in situ O2 generation through the reaction between endogenous H2O2 and single-atom Ru species of OxgeMCC-r SAE, the hypoxia in tumor microenvironment is relieved. Our study demonstrates a promising self-assembled nanozyme with highly efficient single-atom catalytic sites for cancer treatment. The hypoxic microenvironment in solid tumors limits the efficacy of photodynamic therapy (PDT) since oxygen is necessary to produce high cytotoxic singlet oxygen species. Here, the authors develop an improved self-assembled single-atom nanozyme which allows oxygen generation to enhance PDT efficacy. [ABSTRACT FROM AUTHOR]

: Copyright of Nature Communications is the property of Springer Nature and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)

المؤلفون: Chai, Shaohua^1,2 (AUTHOR), Li, Shuangde¹ (AUTHOR) sdli@ipe.ac.cn, Li, Weiman¹ (AUTHOR), Zheng, Qinzhong^1,2 (AUTHOR), Wang, Dongdong^1,2 (AUTHOR), Chen, Yunfa^1,2,3 (AUTHOR) chenyf@ipe.ac.cn

المصدر: Applied Surface Science. Jan2022, Vol. 572, pN.PAG-N.PAG. 1p.

مصطلحات موضوعية: *METAL-organic frameworks, *CHLOROBENZENE, *TITANIUM dioxide, *CATALYSTS, *VANADIUM catalysts, *SELF-propagating high-temperature synthesis

مستخلص: [Display omitted] • MIL-125(Ti) was used as the support for the fabrication of V 2 O 5 /TiO 2. • TiO 2 with high specific surface area facilitated the dispersion of vanadium. • The high-vanadium-loading catalysts showed excellent catalytic activity. • Transient species deteriorated the stability of the catalysts. A series of V 2 O 5 /TiO 2 catalysts with high vanadium loading (6.0 ∼ 43.9 wt%) were prepared by wet impregnation over metal–organic framework (MOF) MIL-125(Ti) support following calcination, and were tested for catalytic combustion of 100 ppm chlorobenzene. Taking advantage of MIL-125(Ti) with high surface area, copious catalytically active VO x species generated in the case of high vanadium loading, among which 0.4VTi, 0.6VTi and 0.8VTi showed 100% chlorobenzene conversion at 250 °C. The effect of vanadium loading on the catalysts have been characterized by means of XRD, SEM, TEM, ICP-OES, N 2 adsorption–desorption at 77 K, Raman, NH 3 -TPD and H 2 -TPR. The reaction mechanism of chlorobenzene over the as-prepared catalysts was also proposed by in situ DRIFTS. [ABSTRACT FROM AUTHOR]

المؤلفون: Liu, Youzhen¹ (AUTHOR), Li, Chenhui¹ (AUTHOR), Loubidi, Mohammed¹ (AUTHOR), Wang, Dongdong¹ (AUTHOR), Zhou, Ling¹ (AUTHOR), Niu, Songyang¹ (AUTHOR), Liu, Qingquan² (AUTHOR), Huo, Jia^1,2 (AUTHOR) jiahuo@hnu.edu.cn

المصدر: Chemical Engineering Journal. Dec2021, Vol. 426, pN.PAG-N.PAG. 1p.

مصطلحات موضوعية: *CATALYSTS, *ELECTROLYTIC reduction, *POROUS materials, *ELECTROCATALYSIS, *METAL catalysts, *CARBON dioxide, *ORGANIC conductors, *CATALYST supports

مستخلص: [Display omitted] • A facile strategy is developed for preparing atomically dispersed Ni sites. • Ni active sites can be fully exposed on hierarchically porous thin-wall carbons. • The electrocatalyst shows enhanced CO 2 RR activity with high FE CO and TOF value. • Excellent activity can be attributed to the increased exposure of Ni active sites. Atomically dispersed metal catalysts have been widely utilized for electrocatalysis, such as the electrochemical reduction of CO 2 , due to their low coordination number and maximum utilization of metal active sites. However, it remains a major challenge to develop an effective and convenient strategy for fully exposing the active sites of atomically dispersed metal catalysts within supports. Herein, we describe an operationally simple and sustainable strategy for preparing hierarchically porous thin-wall carbon networks with highly exposed atomically dispersed Ni sites by directly pyrolyzing a ground mixture of metal salts and organic ligands. Compared with the preformed metal organic framework-derived materials, the amount of exposed active Ni sites can be increased by ~50% for hierarchically porous materials. The hierarchically porous atomically dispersed Ni electrocatalyst shows obviously enhanced CO 2 RR catalytic performance with higher CO Faradaic efficiency (over 99% at −0.88 V) and high TOF value of 7025 h−1 (72.6% higher than that for the metal organic framework-derived materials). The excellent activity can be attributed to the increased exposure of atomically dispersed Ni sites with hierarchically porous structure and interconnected thin-wall carbon networks, which ensure the fully exposure of electrocatalytically active sites and promotion of mass transport and electron transfer. Density functional theory calculations further suggest that the fully exposed Ni sites are responsible for highly efficient activation of CO 2 rather than the carbon layer-covered Ni sites. [ABSTRACT FROM AUTHOR]