- 作 者: ( "hexiang deng" OR "he-xiang deng" )
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Molecular Compartments Created in Metal–Organic Frameworks for Efficient Visible-Light-Driven CO2 Overall ConversionJournal of the American Chemical Society (IF 16.383) Pub Date : 2022-12-15 ,DOI:10.1021/jacs.2c10687Chengbin Zhao, Zhuo Jiang, Yin Liu, Yi Zhou, Panchao Yin, Yubin Ke, Hexiang DengWe report the construction of molecular compartments by the growth of narrow-band semiconductor nanoparticles, tungsten oxide and its hydrate, in the mesopores of a metal–organic framework (MOF), MIL-100-Fe. The location of these nanoparticles in pores and their spatial arrangement across the MOF crystal are unveiled by powder X-ray diffraction and small-angle neutron scattering, respectively. Such ...
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High-entropy-alloy nanoparticles synthesized by laser metallurgy using a multivariate MOFMaterials Chemistry Frontiers (IF 8.683) Pub Date : 2022-08-16 ,DOI:10.1039/d2qm00588cWei Yan, Haoqing Jiang, Wendi Yi, Chengbin Zhao, Yucong Xia, Hengjiang Cong, Lin Tang, Gary J. Cheng, Jianhua He, Hexiang DengWe report the synthesis of multivariate MOFs with combinations of metal ions, including Mn2+, Fe3+, Co2+, Ni2+, Cu2+ and Zn2+. The permanent porosity and the evenly distributed metal components make these porous crystals ideally suited for the synthesis of alloy nanoparticles. Using a laser, these MOFs are converted in air to alloy nanoparticles of binary (FeNi, FeCo), ternary (FeCoNi) and high-entropy-alloys ...
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Packing Metal–Organic Frameworks into an Opal StructureACS Central Science (IF 18.728) Pub Date : 2022-06-06 ,DOI:10.1021/acscentsci.2c00589Haoqing Jiang, Shujuan Liu, Hexiang DengMOFs with an ordered opal structure were synthesized using the template method in a confined space, generating mesopores in addition to the intrinsic micropores. ...
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Covalent organic frameworks catalyzed by organic Lewis acidScience China Chemistry (IF 10.138) Pub Date : 2022-05-25 ,DOI:10.1007/s11426-022-1272-5Xiangqian Shi, Lezhi Yi, Hexiang DengWe report the synthesis of covalent organic framework (COF) crystals with organic Lewis acid instead of the conventional use of Brønsted acid or inorganic Lewis acid. Specifically, tris(pentafluorophenyl)borane was applied for the growth of seven imine COFs: TAPB-PDA-, TAPB-2,5-DMTA-, TAPB-2,3-DMTA-, TAPT-PDA-, TAPT-2,5-DMTA-, TAPT-2,3-DMTA-COF with hcb topology and varied in functional groups, as ...
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Staggered Stacking Covalent Organic Frameworks for Boosting Cancer ImmunotherapyAdvanced Functional Materials (IF 19.924) Pub Date : 2022-04-27 ,DOI:10.1002/adfm.202201542Liang Zhang, Yao Xiao, Qi-Chao Yang, Lei-Lei Yang, Shu-Cheng Wan, Shuo Wang, Lu Zhang, Hexiang Deng, Zhi-Jun SunThe synergistic efficacy of phototherapy and cancer immunotherapy is severely restricted by both the inherent photobleaching and aggregation-caused quench (ACQ) defects of photosensitizers and the intrinsic antioxidant tumor microenvironment (TME), such as hypoxia and overexpressed glutathione (GSH). To address these issues, a novel porphyrin-based staggered stacking covalent organic framework (COF) ...
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Laser driven conversion of MOFs to rare earth metal oxide nanoparticlesAPL Materials (IF 6.635) Pub Date : 2022-04-18 ,DOI:10.1063/5.0085497Xinyu Dou, Jin Liu, Xuan Gong, Haoqing Jiang, Hexiang Deng
We report the production of ultrafine rare earth metal oxide nanoparticles from metal–organic frameworks (MOFs) using lasers, exemplified by the conversion of three Tb-MOFs composed of three different linkers, such as C4H4O4 (H2Fum), C27H18O6 (H3BTB), and C24H15O6N3 (H3TATB). The size of the resulting terbium oxide nanoparticles is precisely controlled from 3 to 12 nm with a narrow distribution, which
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Determining factors in the growth of MOF single crystals unveiled by in situ interface imagingChem (IF 25.832) Pub Date : 2022-03-28 ,DOI:10.1016/j.chempr.2022.03.006Jinli Han, Xudong He, Jin Liu, Ruijian Ming, Mohan Lin, Hui Li, Xiaochun Zhou, Hexiang DengWe trace the evolution of crystal interface during the solvothermal synthesis of metal-organic frameworks (MOFs) in flow cell by in situ dark-field microscope. Precise measurement of the growth rate at specific crystal facets allows for the extraction of the key determining factors for the crystal growth of five typical MOFs, i.e., Cu-MOF-74 (1D), Co-ZIF, Cu-MOF-2-BDC, Cu-MOF-2-NDC (2D), and HKUST-1 ...
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Multivariate MOF for optimizing atmospheric water harvestingGreen Energy & Environment Pub Date : 2022-02-15 ,DOI:10.1016/j.gee.2022.02.004Ao Ma, Hengjiang Cong, Hexiang Deng
Atmospheric water harvesting offers a powerful and promising solution to address the problem of global freshwater scarcity. In the past decade, significant progress has been achieved in utilizing hydrolytically stable metal–organic frameworks as recyclable water-sorbent materials under low relative humidity, especially in those arid areas. Recently, Yaghi's group has employed a combined crystallographic
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Engineering Multienzyme-Mimicking Covalent Organic Frameworks as Pyroptosis Inducers for Boosting Antitumor ImmunityAdvanced Materials (IF 32.086) Pub Date : 2021-12-16 ,DOI:10.1002/adma.202108174Liang Zhang, Qi-Chao Yang, Shuo Wang, Yao Xiao, Shu-Cheng Wan, Hexiang Deng, Zhi-Jun SunThe engineering of a series of multienzyme-mimicking covalent organic frameworks (COFs), COF-909-Cu, COF-909-Fe, and COF-909-Ni, as pyroptosis inducers, remodeling the tumor microenvironment to boost cancer immunotherapy, is reported. Mechanistic studies reveal that these COFs can serve as hydrogen peroxide (H2O2) homeostasis disruptors to elevate intracellular H2O2 levels, and they not only exhibit ...
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Long excited state lifetime of thermally activated delayed fluorescent photosensitizer integrated into Metal-organic framework enables efficient CO2 photoreductionChemical Engineering Journal (IF 16.744) Pub Date : 2021-12-01 ,DOI:10.1016/j.cej.2021.133897Binglin Bie, Zhuo Jiang, Jing Zhang, Hexiang Deng, Chuluo YangThe performance of metal–organic-framework-based photocatalysts were usually limited by the short lifetime of excited state and the high cost of precious metal complexes in CO2 photoreduction. To enhance the lifetime of excited state, an organic thermally activated delayed fluorescence photosensitizer was installed with the non-noble zinc node in a periodic structure named Spiro-Zn-MOF. The horizontally ...
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Uncovering growth species of multivariate MOFs in liquid phase by mass spectrometryChinese Chemical Letters (IF 8.455) Pub Date : 2021-11-18 ,DOI:10.1016/j.cclet.2021.11.035Jinli Han, Suming Chen, Xiaochun Zhou, Hexiang DengThe unveiling of MOF growth mechanism is hampered by the lack of fundamental knowledge about the very early stage of nucleation, especially the form and ratio of molecular species in the solution for crystal growth. Herein, we report the detection of growth species for a series of MOFs with mono-linker, Cu-MOF-2-BDC and Cu-MOF-2-NDC, and two linkers, MTV-MOF-2-(C4H4)x, by high resolution ESI-MS, where ...
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Enzymatic deamination of the epigenetic nucleoside N6-methyladenosine regulates gene expressionNucleic Acids Research (IF 19.16) Pub Date : 2021-11-16 ,DOI:10.1093/nar/gkab1124Zhuoran Jiang, Chao Wang, Zixin Wu, Kun Chen, Wei Yang, Hexiang Deng, Heng Song, Xiang Zhou
N6-methyladenosine (m6A) modification is the most extensively studied epigenetic modification due to its crucial role in regulating an array of biological processes. Herein, Bsu06560, formerly annotated as an adenine deaminase derived from Bacillus subtilis 168, was recognized as the first enzyme capable of metabolizing the epigenetic nucleoside N6-methyladenosine. A model of Bsu06560 was constructed
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Sequence control of metals in MOF by coordination number precoding for electrocatalytic oxygen evolutionChem Catalysis Pub Date : 2021-11-11 ,DOI:10.1016/j.checat.2021.10.007Hongnan Jia, Qi Han, Wei Luo, Hengjiang Cong, Hexiang Deng
Inorganic porous materials are prevailing in energy storage, environment remediation, and catalysis; however, it is attractive to control the spatial arrangement of heterometals in these materials with atomic accuracy. Here, we report the precise positioning of metals with identical valence, coordination number, and similar size, such as Zn (II) and Co (II), to generate an alternating sequence in a
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Two-Photon Absorption Induced Cancer Immunotherapy Using Covalent Organic Frameworks (Adv. Funct. Mater. 42/2021)Advanced Functional Materials (IF 19.924) Pub Date : 2021-10-14 ,DOI:10.1002/adfm.202170315Lei-Lei Yang, Liang Zhang, Shu-Cheng Wan, Shuo Wang, Zhi-Zhong Wu, Qi-Chao Yang, Yao Xiao, Hexiang Deng, Zhi-Jun Sun
Cancer Immunotherapy
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Three-Dimensional Covalent Organic Frameworks with Cross-Linked Pores for Efficient Cancer ImmunotherapyNano Letters (IF 12.262) Pub Date : 2021-09-15 ,DOI:10.1021/acs.nanolett.1c02050Liang Zhang, Lei-Lei Yang, Shu-Cheng Wan, Qi-Chao Yang, Yao Xiao, Hexiang Deng, Zhi-Jun SunWe report the design and synthesis of a series of three-dimensional (3D) covalent organic frameworks (COFs) as immunogenic cell death (ICD) inducers for cancer immunotherapy. Three triple-topic amine building blocks, inactive to inducing ICD, were used to construct three COFs, COF-607, COF-608, and COF-609, with outstanding ICD eliciting efficiency. Mechanism studies revealed that after linking these ...
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Two-Photon Absorption Induced Cancer Immunotherapy Using Covalent Organic FrameworksAdvanced Functional Materials (IF 19.924) Pub Date : 2021-06-21 ,DOI:10.1002/adfm.202103056Lei-Lei Yang, Liang Zhang, Shu-Cheng Wan, Shuo Wang, Zhi-Zhong Wu, Qi-Chao Yang, Yao Xiao, Hexiang Deng, Zhi-Jun SunImmune checkpoint blockade therapy is revolutionizing the traditional treatment model of multiple tumor types, but remains ineffective for a large subset of patients. Photodynamic therapy (PDT) has been shown to induce cancer cell death and provoke an immune response, and may represent a potential strategy to synergize with immune checkpoint blockade therapy. However, the limited tissue penetration ...
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Structures suggest an approach for converting weak self-peptide tumor antigens into superagonists for CD8 T cells in cancer [Immunology and Inflammation]Proceedings of the National Academy of Sciences of the United States of America (IF 12.779) Pub Date : 2021-06-08 ,DOI:10.1073/pnas.2100588118Pengcheng Wei, Kimberly R. Jordan, Jonathan D. Buhrman, Jun Lei, Hexiang Deng, Philippa Marrack, Shaodong Dai, John W. Kappler, Jill E. Slansky, Lei Yin
Tumors frequently express unmutated self-tumor–associated antigens (self-TAAs). However, trial results using self-TAAs as vaccine targets against cancer are mixed, often attributed to deletion of T cells with high-affinity receptors (TCRs) for self-TAAs during T cell development. Mutating these weak self-TAAs to produce higher affinity, effective vaccines is challenging, since the mutations may not
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25 Years of Reticular ChemistryAngewandte Chemie International Edition (IF 16.823) Pub Date : 2021-03-29 ,DOI:10.1002/anie.202101644Ralph Freund, Stefano Canossa, Seth M. Cohen, Wei Yan, Hexiang Deng, Vincent Guillerm, Mohamed Eddaoudi, David G. Madden, David Fairen-Jimenez, Hao Lyu, Lauren K. Macreadie, Zhe Ji, Yuanyuan Zhang, Bo Wang, Frederik Haase, Christof Wöll, Orysia Zaremba, Jacopo Andreo, Stefan Wuttke, Christian S. DiercksReticular chemistry translates the precision and expertise of organic and inorganic synthesis to the solid state. The most profound innovation of the field has been the elaboration of design strategies for the synthesis of extended crystalline solids through strong directional bonds. This Review highlights the classes of reticular materials, their functionalization, and the introduction of complexity ...
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Immune-based mutation classification enables neoantigen prioritization and immune feature discovery in cancer immunotherapybioRxiv - Cancer Biology Pub Date : 2021-01-27 ,DOI:10.1101/700732Peng Bai, Yongzheng Li, Qiuping Zhou, Jiaqi Xia, Peng-Cheng Wei, Hexiang Deng, Min Wu, Sanny K. Chan, John W Kappler, Yu Zhou, Eric Tran, Philippa Marrack, Lei Yin
Genetic mutations lead to the production of mutated proteins from which peptides are presented to T cells as cancer neoantigens. Evidence suggests that T cells that target neoantigens are the main mediators of effective cancer immunotherapies. Although algorithms have been used to predict neoantigens, only a minority are immunogenic. The factors that influence neoantigen immunogenicity are not completely
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Covalent organic frameworks for optical applicationsAggregate Pub Date : 2021-1-22 ,DOI:10.1002/agt2.24Liang Zhang, Lezhi Yi, Zhi-Jun Sun, Hexiang Deng*
In this review, we focus on the impact from geometric arrangement of molecular building blocks within COF backbone, which is closely associated with the optical property. Specifically, three critical structure factors, the connection, orientation and alignment (C, O and A) are extracted to facilitate the understanding of influence from microscopic structure features to their optical behaviors at macroscopic
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Publisher Correction: Filling metal–organic framework mesopores with TiO 2 for CO 2 photoreductionNature (IF 69.504) Pub Date : 2021-01-19 ,DOI:10.1038/s41586-020-03101-xZhuo Jiang, Xiaohui Xu, Yanhang Ma, Hae Sung Cho, Deng Ding, Chao Wang, Jie Wu, Peter Oleynikov, Mei Jia, Jun Cheng, Yi Zhou, Osamu Terasaki, Tianyou Peng, Ling Zan, Hexiang Deng
A Correction to this paper has been published: https://doi.org/10.1038/s41586-020-03101-x
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Immune-based mutation classification enables neoantigen prioritization and immune feature discovery in cancer immunotherapyOncoImmunology (IF 7.723) Pub Date : 2021-01-15 ,DOI:10.1080/2162402x.2020.1868130Peng Bai, Yongzheng Li, Qiuping Zhou, Jiaqi Xia, Peng-Cheng Wei, Hexiang Deng, Min Wu, Sanny K. Chan, John W. Kappler, Yu Zhou, Eric Tran, Philippa Marrack, Lei Yin
ABSTRACT Genetic mutations lead to the production of mutated proteins from which peptides are presented to T cells as cancer neoantigens. Evidence suggests that T cells that target neoantigens are the main mediators of effective cancer immunotherapies. Although algorithms have been used to predict neoantigens, only a minority are immunogenic. The factors that influence neoantigen immunogenicity are
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Reticular chemistry at the atomic, molecular, and framework scalesNano Research (IF 10.269) Pub Date : 2020-11-28 ,DOI:10.1007/s12274-020-3226-6Yue-Biao Zhang,Qiaowei Li,Hexiang Deng
1 School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China 2 Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China 3 Key Laboratory of Biomedical Polymers, Ministry of Education, College of Chemistry and
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A laser metallurgy route for the batch preparation of mm-scale 3D silver/graphite heteronanoclusters in airNanoscale (IF 8.307) Pub Date : 2020-11-04 ,DOI:10.1039/d0nr06806cMeng-Yue Gao, Hao-Qing Jiang, Fang-Yuan Han, He-Xiang Deng, Ji-Ming Hu, Ai-Guo ShenWe report a batch preparation of mm-scale 3D Ag hetero-nanoclusters which exhibit an excellent surface plasmon resonance ability via facile laser metallurgy. Under laser irradiation, the porous AgI-based coordination network crystals were instantly converted into 3D graphite-encapsulated Ag hetero-nanoclusters with uniform sizes and gaps in several seconds. The obtained hetero-nanoclusters exhibited ...
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Filling metal–organic framework mesopores with TiO2 for CO2 photoreductionNature (IF 69.504) Pub Date : 2020-09-09 ,DOI:10.1038/s41586-020-2738-2Zhuo Jiang, Xiaohui Xu, Yanhang Ma, Hae Sung Cho, Deng Ding, Chao Wang, Jie Wu, Peter Oleynikov, Mei Jia, Jun Cheng, Yi Zhou, Osamu Terasaki, Tianyou Peng, Ling Zan, Hexiang DengMetal–organic frameworks (MOFs) 1 – 3 are known for their specific interactions with gas molecules 4 , 5 ; this, combined with their rich and ordered porosity, makes them promising candidates for the photocatalytic conversion of gas molecules to useful products 6 . However, attempts to use MOFs or MOF-based composites for CO 2 photoreduction 6 – 13 usually result in far lower CO 2 conversion efficiency ...
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Molecular Vises for Precisely Positioning Ligands near Catalytic Metal Centers in Metal-Organic FrameworkJournal of the American Chemical Society (IF 16.383) Pub Date : 2020-08-21 ,DOI:10.1021/jacs.0c07450Wei Yan, Shenhui Li, Tao Yang, Yucong Xia, Xinrui Zhang, Chao Wang, Zier Yan, Feng Deng, Qianghui Zhou, Hexiang DengWe report the construction of molecular vise by pairing a tritopic phenylphosphrous (III) linker and a monotopic link-er in opposite position within metal-organic framework. The angle between these linkers at metal sites is fixed upon change of functionality in the monotopic linker, while the distance between them is precisely tuned. Such distance within molecular vise is accurately measured by 1H-31P ...
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Structures and Structural Evolution of Sublayer Surfaces of Metal-Organic Frameworks.Angewandte Chemie International Edition (IF 16.823) Pub Date : 2020-08-14 ,DOI:10.1002/anie.202008100Xiaocang Han,Pan Liu,Fang Lin,Wenqian Chen,Ruichun Luo,Qi Han,Zhuo Jiang,Xiaodong Wang,Shuangxi Song,Kolan Madhav Reddy,Hexiang Deng,Mingwei ChenThe structural characterization of sublayer surfaces of MIL‐101 is reported by low‐dose spherical aberration‐corrected high‐resolution transmission electron microscopy (HRTEM). The state‐of‐the‐art microscopy directly images atomic/molecular configurations in thin crystals from charge density projections, and uncovers the structures of sublayer surfaces and their evolution to stable surfaces regulated ...
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Anisotropic reticular chemistryNature Reviews Materials (IF 76.679) Pub Date : 2020-08-13 ,DOI:10.1038/s41578-020-0225-xWentao Xu, Binbin Tu, Qi Liu, Yufei Shu, Cong-Cong Liang, Christian S. Diercks, Omar M. Yaghi, Yue-Biao Zhang, Hexiang Deng, Qiaowei LiReticular chemistry has been focused on making simple structures in which a few kinds of components are linked to make crystals such as metal–organic frameworks (MOFs). While this chemistry has grown into a large field, a more extensive area with fascinating directions is emerging through the introduction of multiplicity and variation into the components of MOFs. When the MOF backbone is composed of ...
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Hyperpolarized Xe NMR signal advancement by metal-organic framework entrapment in aqueous solution.Proceedings of the National Academy of Sciences of the United States of America (IF 12.779) Pub Date : 2020-07-28 ,DOI:10.1073/pnas.2004121117Qingbin Zeng,Binglin Bie,Qianni Guo,Yaping Yuan,Qi Han,Xiaocang Han,Mingwei Chen,Xu Zhang,Yunhuang Yang,Maili Liu,Pan Liu,Hexiang Deng,Xin ZhouWe report hyperpolarized Xe signal advancement by metal-organic framework (MOF) entrapment (Hyper-SAME) in aqueous solution. The 129Xe NMR signal is drastically promoted by entrapping the Xe into the pores of MOFs. The chemical shift of entrapped 129Xe is clearly distinguishable from that of free 129Xe in water, due to the surface and pore environment of MOFs. The influences from the crystal size of ...
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Reticulation of 2D Semiconductors by Metal–Organic Approach for Efficient Hydrogen EvolutionACS Sustainable Chemistry & Engineering (IF 9.224) Pub Date : 2020-05-28 ,DOI:10.1021/acssuschemeng.0c02805Hongmei Dai, Jiao Sun, Yi Zhou, Zirui Zhou, Wei Luo, Guangfeng Wei, Hexiang DengWe report a universal approach to synthesize a series of three-dimensional (3D) metal–organic constructs by linking 2D metal dichalcogenides with organic amine molecules [p-phenylenediamine (PPDA), biphenyl diamine (BPDA), tetra(4-aminophenyl) methane) (TPMA)]. Accurate interlayer distances, ranging from 0.61 to 1.7 nm, are dialed-in by the organic components in 3D constructs of MoS2, MoSe2, and WS2 ...
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