Nature Communications
·
2022
·Vol. 13
·期 1
·1-13
·
IF 17.694
Li Bang Lin,Luo Jun Jiang,Zou Hao Lin,Zhang Qing-Meng,Zhao Liu-Bin,Qian Hang,Luo Hong Qun,Leong David Tai,Li Nian Bing
The transfer of the concept of chirality from molecules to synthesized nanomaterials has attracted attention amongst multidisciplinary teams. Here we demonstrate heterogeneous nucleation and anisotropic accumulation of Au nanoparticles on multilayer MoS 2 planes to form chiroptically functional nanomaterials. Thiol amino acids with chiral conformations modulate asymmetric growth of gold nanoarchitectures on seeds of highly faceted Au/MoS 2 heterostructures. Consequently, dendritic plasmonic nanocrystals with partial chiral morphologies are synthesized. The chirality of dendritic nanocrystals inherited from cysteine molecules refers to the structural characteristics and includes specific recognition of enantiomeric molecules. With integration of the intrinsic photothermal properties and inherited enantioselective characteristics, dendritic Au/MoS 2 heterostructures exhibit chirality-dependent release of antimicrobial drugs from hydrogel substrates when activated by exogenous infrared irradiation. A three-in-one strategy involving synthesis of chiral dendritic heterostructures, enantioselective recognition, and controlled drug release system is presented, which improves nanomaterial synthetic technology and enhances our understanding of crucial chirality information.
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高影响因子
CELLULOSE
·
2022
·Vol. 30
·期 2
·1103-1115
·
IF 6.123
Wang Weiming,Wu Yuming,Yi Jie,Yang Yuhan,Shen Meiling,Yang Zhihui,Peng Shuai,Min Xue,Yang Xixian,Xiong Jun,Li Ming
Solar vapor production is considered an effective and environmentally friendly method of reducing freshwater shortages. However, designing an affordable solar evaporator with a simple method is still a challenge. Herein, motivated by the transpiration of plants, a full cattail leaf-based solar evaporator has been developed. In this solar evaporator, the photothermal membrane has been exploited by simply cross-linking the carbonized cattail leaf and the fibers from the alkali-treated cattail leaf with sodium alginate. The original cattail leaf with its square water transport channels and inherent hydrophilicity is employed to pump the bottom water to the upper photothermal membrane. Thanks to the synergistic effect between the photothermal membrane and the cattail leaf-based water transporter, the full cattail leaf-derived solar evaporator acquires an evaporation rate of 1.46 kg m –2 h –1 with a solar thermal efficiency of 87.48% under 1-solar (1 kW m –2 ). Fifteen-cycle experiments indicate that this solar evaporator has excellent stability. Outdoor experiments demonstrate that the full cattail leaf-based solar evaporator can effectively desalinate seawater and purify dyeing wastewater. Moreover, the total cost of the chemicals applied to manufacture 1 m 2 of cattail leaf-based photothermal membrane is approximately 3.1 dollars. This strategy is expected to turn freely available biomass into a potentially valuable solar evaporator with a simple cross-linking method and an affordable price that offers a promising future for alleviating the global freshwater crisis. Graphical abstract
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GENOME BIOLOGY
·
2022
·Vol. 23
·期 1
·1-29
·
IF 17.906
Li Conghui,Yin Zhinang,Xiao Ruijing,Huang Beili,Cui Yali,Wang Honghong,Xiang Ying,Wang Lingrui,Lei Lingyu,Ye Jiaqin,Li Tianyu,Zhong Youquan,Guo Fangteng,Xia Yuchen,Fang Pingping,Liang Kaiwei
Background G-quadruplexes (G4s) are unique noncanonical nucleic acid secondary structures, which have been proposed to physically interact with transcription factors and chromatin remodelers to regulate cell type-specific transcriptome and shape chromatin landscapes.Results Based on the direct interaction between G4 and natural porphyrins, we establish genome-wide approaches to profile where the iron-liganded porphyrin hemin can bind in the chromatin. Hemin promotes genome-wide G4 formation, impairs transcription initiation, and alters chromatin landscapes, including decreased H3K27ac and H3K4me3 modifications at promoters. Interestingly, G4 status is not involved in the canonical hemin-BACH1-NRF2-mediated enhancer activation process, highlighting an unprecedented G4-dependent mechanism for metabolic regulation of transcription. Furthermore, hemin treatment induces specific gene expression profiles in hepatocytes, underscoring the in vivo potential for metabolic control of gene transcription by porphyrins.Conclusion sThese studies demonstrate that G4 functions as a sensor for natural porphyrin metabolites in cells, revealing a G4-dependent mechanism for metabolic regulation of gene transcription and chromatin landscapes, which will deepen our knowledge of G4 biology and the contribution of cellular metabolites to gene regulation.
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JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 58
·期 1
·170-185
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IF 4.682
Zang Yu,Gao Shan,Jing Boyu,Sun Hong,Wang Jianjun,Liu Jiao,Miao Fengjuan,Xu Liang
Four kinds of conjugated microporous polymers (CMPs) with imine structures were synthesized by a Sonogashira coupling reaction followed by a postreaction between aldehydes and amines. Palladium nanoparticles (Pd NPs) were successfully supported on the CMPs to prepare Pd/CMP heterogeneous catalysts and were used to catalyze the Suzuki–Miyaura coupling reaction. The number of aromatic nuclei and nitrogen atoms in the CMPs highly affects Pd loading. In the Suzuki–Miyaura coupling reaction, the Pd/CMP with good Pd NPs dispersibility and appropriate Pd content (Pd/CMP-NA) exhibited the highest catalytic efficiency with 100% conversion and 95.4% yield which can be used for many substrates. The Pd/CMP-NA heterogeneous catalyst was easy to recover and still exhibited good catalytic efficiency after 5 cycles. To further understand the catalytic mechanism of Pd/CMP-NA on the Suzuki–Miyaura coupling reaction, we proposed a rational catalytic cycle. This paper provides an idea for the structural design of CMPs used for Suzuki–Miyaura catalytic reaction.
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POLYMER BULLETIN
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2022
·Vol. 80
·期 11
·12065-12077
·
IF 2.843
Xing Yunliang,Zhang Yuan,He Xianru
Developing of high-performance thermosets with outstanding thermal properties has attracted increasing attention. Herein, a combined strategy, acetylene modification and copolymerization with bismaleimide, has been utilized for a novel bio-based tri-functional benzoxazine monomer. The monomer (RES-pa) was successfully synthesized using biomass resources, resveratrol, as raw material. Three systems with different ratios (RES-pa: bismaleimide = 1:0, 1:1, 1:2) were designed. The thermal derived polymerization of three systems was monitored by DSC and in situ FT-IR. Thermal stability of derived thermosets was systemically investigated in detail by dynamic mechanical analysis (DMA) and thermogravimetric analysis (TGA). Specially, poly(RES-pa- co -DDM-BMI-1/1) is found to show a high T g value of 374 °C and Td 10 of 387 °C. Promisingly, the combined strategy used in the work may grant efficient way for design and preparation of high-performance thermosets.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Zhu Yiming,Wang Jiaao,Koketsu Toshinari,Kroschel Matthias,Chen Jin-Ming,Hsu Su-Yang,Henkelman Graeme,Hu Zhiwei,Strasser Peter,Ma Jiwei
Designing active and stable electrocatalysts with economic efficiency for acidic oxygen evolution reaction is essential for developing proton exchange membrane water electrolyzers. Herein, we report on a cobalt oxide incorporated with iridium single atoms (Ir-Co 3 O 4 ), prepared by a mechanochemical approach. Operando X-ray absorption spectroscopy reveals that Ir atoms are partially oxidized to active Ir >4+ during the reaction, meanwhile Ir and Co atoms with their bridged electrophilic O ligands acting as active sites, are jointly responsible for the enhanced performance. Theoretical calculations further disclose the isolated Ir atoms can effectively boost the electronic conductivity and optimize the energy barrier. As a result, Ir-Co 3 O 4 exhibits significantly higher mass activity and turnover frequency than those of benchmark IrO 2 in acidic conditions. Moreover, the catalyst preparation can be easily scaled up to gram-level per batch. The present approach highlights the concept of constructing single noble metal atoms incorporated cost-effective metal oxides catalysts for practical applications.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 58
·期 1
·211-229
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IF 4.682
Wang Chenxu,Ding Jiawei,Gong Chuangchuang,Chen Tong,Zhang Yijing,Song Kai,Shi Chunsheng,He Fang
In order to tackle the electromagnetic pollution caused by the application of electromagnetic wave (EMW) in wireless communication, military industry, and other fields, broadband EMW absorption materials are urgently needed. To achieve this goal, emerging methods resort to constructing multivariate synergistic composites with unique morphology to enhance EMW absorption through diverse loss mechanisms and prominent structural advantage. Herein, a spatially tuned confinement pyrolysis strategy is proposed to design pomegranate-like MnO@NC absorption material. Unique hierarchical structure and more scattering sites are accessed via well-designed one-shell multiple cores nanostructure. N-doped carbon acts as an interwoven conductive network and restricts the movement of EMW in the shell, while nano-MnO acts as an impedance matching phase and interferes with the continuity of EMW. Moreover, the intercalation of dispersed MnO also amplifies the contribution of interfacial effect to EMW absorption, which can be verified by the calculation of the surface work function. The optimized composite possesses a maximum absorption bandwidth of 6.51 GHz at 2.4 mm and its maximum reflection loss reaches − 58.4 dB ( d = 2.3 mm). The synthesis of pomegranate-like composite provides a new direction for fabricating advanced carbonate-based EMW absorbers which are toward practical application. Graphical abstract
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高影响因子
MICROCHIMICA ACTA
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2022
·Vol. 190
·期 1
·1-9
·
IF 6.408
Ma Yao,Zhao Liping,Li Linsen,Zhu Chao,Qu Feng
A new type of aptamer-functionalized pH-responsive polymer-modified magnetic nanoparticles (ApMNPs) is introduced for specific enrichment and sensitive determination of lactoferrin (Lf) in complex matrixes. In the construction, Fe 3 O 4 @3-(Triethoxysilyl)propylmethacrylate@poly(4-Vinyl-1, 3-dioxolan-2-one-acrylic acid) (Fe 3 O 4 @MPS@p(VEC-AA)) were synthesized as pH-responsive polymer-modified magnetic nanoparticles (pMNPs) through free radical polymerization to increase the tunable interaction. Lf-binding aptamers were conjugated onto pMNPs through the reaction of amino-group in aptamer and epoxide-group in VEC, innovatively applied to prepare Lf-ApMNPs. On the basis of the synergistic effect of specific affinity of aptamer on Lf and tunable hydrophobic/hydrophilic property of pH-responsive polymer, Lf-ApMNPs presented good selectivity toward Lf, excellent adsorption capacity (as high as 233.9 mg g −1 ), as well as good recoveries in the range 93.6–99.6% in Lf-related nutrition samples. Significantly, the introduction of pH-responsive monomer (AA) effectively regulated the adsorption–desorption process of Lf, with the function similar to a switch. Moreover, the good performances of Ct-ApMNPs toward α-Chymotrypsin showed that ApMNPs exhibited universality to other proteins through easily changing the binding aptamer, thereby offering a facile and efficient approach for specific enrichment and sensitive determination of targets in real biological samples. Graphical Abstract
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高影响因子
CELLULOSE
·
2022
·Vol. 30
·期 3
·1533-1542
·
IF 6.123
Lou Jiayu,Wang Meiyi,Liu Yang,Wang Huashan
T 1 –T 2 multi-modality submicron particles were widely used in clinic imaging, biochemical analysis and biosensor. Here, we prepared a new magnetic submicron particle through the spatial-gap of cellulose nanocrystal (CNC) dispersion as a template.The obtained submicron particles were ellipsoid and had a better magnetic response and relaxation effects. By varying the Fe(acac) 3 to Gd(acac) 3 ratio, it was possible to tune the surface morphology, crystal structure and T 1 –T 2 relaxation effect. More importantly, the pre-drying and burning process had influence on the polycrystalline growth process of Fe(acac) 3 and Gd(acac) 3 mixture, and the slow removal process for the CNC template could endow the compounds with different relaxation effects. By using the spatial-gap of the cellulose nanocrystal dispersion as a template makes it possible to fabricate T 1 –T 2 multi-modality crystalline submicron particles directly and is promising for preparing other CNC-templating based functional materials.
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Nano Research
·
2022
·Vol. 16
·期 6
·8405-8410
·
IF 10.269
Cao Renfei,Cui Yangfeng,Huang Gang,Liu Wanqiang,Liu Jianwei,Zhang Xinbo
Li-O 2 batteries with extremely high specific energy density have been regarded as a kind of promising successor to current Li-ion batteries. However, the high charge overpotential for the decomposition of Li 2 O 2 discharge product reduces the energy efficiency and triggers a series of side reactions that cause the Li-O 2 batteries to have a limited lifetime. Herein, Co-doped C 3 N 4 (Co-C 3 N 4 ) photocatalysts were designed by an in situ thermal evaporation method to take advantage of the photo-assisted charging technology to conquer the shortcomings of Li-O 2 batteries encountered in the charge process. Different from the commonly used photocatalysts, the Co-C 3 N 4 photocatalysts perform well no matter with and without illumination, owing to the Co doping induced conductivity and electrocatalytic ability enhancement. This makes the Co-C 3 N 4 reduce the charge and discharge overpotentials and improve the cycling performance of Li-O 2 batteries (from 20 to 106 cycles) without illumination. While introducing illumination, the performance can be further improved: Charge voltage reduces to 3.3 V, and the energy efficiency increases to 84.84%, indicating that the Co-C 3 N 4 could behave as a suitable photocathode for Li-O 2 batteries. Besides, the low charge voltage and the continuous illumination together weaken the corrosion of the Li anode, making the long-term high-efficiency operation of Li-O 2 batteries no longer just extravagant hope.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-20
·
IF 16.6
Zhou Songlei,Huang Yukun,Chen Yu,Liu Yipu,Xie Laozhi,You Yang,Tong Shiqiang,Xu Jianpei,Jiang Gan,Song Qingxiang,Mei Ni,Ma Fenfen,Gao Xiaoling,Chen Hongzhuan,Chen Jun
The limited benefits of immunotherapy against glioblastoma (GBM) is closely related to the paucity of T cells in brain tumor bed. Both systemic and local immunosuppression contribute to the deficiency of tumor-infiltrating T cells. However, the current studies focus heavily on the local immunosuppressive tumor microenvironment but not on the co-existence of systemic immunosuppression. Here, we develop a nanostructure named Nano-reshaper to co-encapsulate lymphopenia alleviating agent cannabidiol and lymphocyte recruiting cytokine LIGHT. The results show that Nano-reshaper increases the number of systemic T cells and improves local T-cell recruitment condition, thus greatly increasing T-cell infiltration. When combined with immune checkpoint inhibitor, this therapeutic modality achieves 83.3% long-term survivors without recurrence in GBM models in male mice. Collectively, this work unveils that simultaneous reprogramming of systemic and local immune function is critical for T-cell based immunotherapy and provides a clinically translatable option for combating brain tumors.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 6
·2619-2633
·
IF 4.5
Yang Lei,Liu Duan,Luo Jianhong
The new polypyrrole tin boratophosphate (PTB) material has been synthesized for the first time in this work. A series of characterization analyses of the PTB by FTIR, XRD, TGA, SEM, TEM and EA have proved that PTB is amorphous ion nanocomposites, which shows that the PTB has excellent chemical stability in complex acidic and organic environments and commendable selectivity for Pb 2+ as well. The adsorption mechanism of the PTB adsorption process was studied in detail from the aspects of thermodynamics, kinetic and adsorption isotherm. It is proved that the adsorption kinetic model conforms to the quasi second-order kinetic model, while the adsorption isotherm is consistent with the Langmuir model. It is also proved that the adsorption of Pb 2+ ions by the PTB is spontaneous endothermic process. In conclusion, the PTB cation exchange material synthesized in this paper has a good application prospect in the removal of Pb 2+ from industrial and domestic sewage.
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