Nature Communications
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2021
·Vol. 12
·期 1
·1-9
·
IF 14.919
Lin Zirui,Shi Hua-Yu,Lin Lu,Yang Xianpeng,Wu Wanlong,Sun Xiaoqi
Rechargeable aqueous zinc-organic batteries are promising energy storage systems with low-cost aqueous electrolyte and zinc metal anode. The electrochemical properties can be systematically adjusted with molecular design on organic cathode materials. Herein, we use a symmetric small molecule quinone cathode, tetraamino-p-benzoquinone (TABQ), with desirable functional groups to protonate and accomplish dominated proton insertion from weakly acidic zinc electrolyte. The hydrogen bonding network formed with carbonyl and amino groups on the TABQ molecules allows facile proton conduction through the Grotthuss-type mechanism. It guarantees activation energies below 300 meV for charge transfer and proton diffusion. The TABQ cathode delivers a high capacity of 303 mAh g −1 at 0.1 A g −1 in a zinc-organic battery. With the increase of current density to 5 A g −1 , 213 mAh g −1 capacity is still preserved with stable cycling for 1000 times. Our work proposes an effective approach towards high performance organic electrode materials.
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Nature Protocols
·
2021
·Vol. 16
·期 7
·3522-3546
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IF 13.491
Liu Jia,He Hui,Xie Dan,Wen Yanrong,Liu Zhen
Cellular heterogeneity is pervasive and of paramount importance in biology. Single-cell analysis techniques are indispensable for understanding the heterogeneity and functions of cells. Low-copy-number proteins (fewer than 1,000 molecules per cell) perform multiple crucial functions such as gene expression, cellular metabolism and cell signaling. The expression level of low-copy-number proteins of individual cells provides key information for the in-depth understanding of biological processes and diseases. However, the quantitative analysis of low-copy-number proteins in a single cell still remains challenging. To overcome this, we developed an approach called single-cell plasmonic immunosandwich assay (scPISA) for the quantitative measurement of low-copy-number proteins in single living cells. scPISA combines in vivo microextraction for specific enrichment of target proteins from cells and a state-of-the-art technique called plasmon-enhanced Raman scattering for ultrasensitive detection of low-copy-number proteins. Plasmon-enhanced Raman scattering detection relies on the plasmonic coupling effect (hot-spot) between silver-based plasmonic nanotags and a gold-based extraction microprobe, which dramatically enhances the signal intensity of the surface-enhanced Raman scattering of the nanotags and thereby enables sensitivity at the single-molecule level. scPISA is a straightforward and minimally invasive technique, taking only ~6–15 min (from in vivo extraction to Raman spectrum readout). It is generally applicable to all freely floating intracellular proteins provided that appropriate antibodies or alternatives (for example, molecularly imprinted polymers or aptamers) are available. The entire protocol takes ~4–7 d to complete, including material fabrication, single-cell manipulation, protein labeling, signal acquisition and data analysis.
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Nano-Micro Letters
·
2021
·Vol. 13
·期 1
·1-21
·
IF 16.419
Xiang Zhen,Shi Yuyang,Zhu Xiaojie,Cai Lei,Lu Wei
AbstractSection
Abstract
High-performance electromagnetic wave absorption and electromagnetic interference (EMI) shielding materials with multifunctional characters have attracted extensive scientific and technological interest, but they remain a huge challenge. Here, we reported an electrostatic assembly approach for fabricating 2D/1D/0D construction of Ti 3 C 2 T x /carbon nanotubes/Co nanoparticles (Ti 3 C 2 T x /CNTs/Co) nanocomposites with an excellent electromagnetic wave absorption, EMI shielding efficiency, flexibility, hydrophobicity, and photothermal conversion performance. As expected, a strong reflection loss of -85.8 dB and an ultrathin thickness of 1.4 mm were achieved. Meanwhile, the high EMI shielding efficiency reached 110.1 dB. The excellent electromagnetic wave absorption and shielding performances were originated from the charge carriers, electric/magnetic dipole polarization, interfacial polarization, natural resonance, and multiple internal reflections. Moreover, a thin layer of polydimethylsiloxane rendered the hydrophilic hierarchical Ti 3 C 2 T x /CNTs/Co hydrophobic, which can prevent the degradation/oxidation of the MXene in high humidity condition. Interestingly, the Ti 3 C 2 T x /CNTs/Co film exhibited a remarkable photothermal conversion performance with high thermal cycle stability and tenability. Thus, the multifunctional Ti 3 C 2 T x /CNTs/Co nanocomposites possessing a unique blend of outstanding electromagnetic wave absorption and EMI shielding, light-driven heating performance, and flexible water-resistant features were highly promising for the next-generation intelligent electromagnetic attenuation system.
AbstractSection
Highlights
The 2D/1D/0D Ti 3 C 2 T x /carbon nanotubes/Co nanocomposite is successfully synthesized via an electrostatic assembly.
Nanocomposites exhibit an excellent electromagnetic wave absorption and a remarkable electromagnetic interference shielding efficiency.
The flexible, waterproof, and photothermal conversion performances are achieved.
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Nano Research
·
2021
·Vol. 15
·期 2
·1027-1038
·
IF 8.897
Ouyang Zhaofeng,Cui Songbo,Yu Houyong,Xu Dewen,Wang Chuang,Tang Dongping,Tam Kam Chiu
Flexible wearable electronics were developed for applications such as electronic skins, human-machine interactions, healthcare monitoring, and anti-infection therapy. But conventional materials showed impermeability, single sensing ability, and no designated therapy, which hindered their applications. Thus it was still a great challenge to develop electronic devices with multifunctional sensing properties and self-driven anti-infection therapy. Herein, flexible and breathable on-skin electronic devices for multifunctional fabric based sensing and self-driven designated anti-infection therapy were prepared successfully with cellulose nanocrystals/iron(III) ion/polyvinyl alcohol (CNC/Fe 3+ /PVA) composite. The resultant composite films possessed robust mechanical performances, outstanding conductivity, and distinguished breathability (3.03 kg/(m 2 ·d)), which benefited from the multiple interactions of weak hydrogen bonds and Fe 3+ chelation and synergistic effects among CNC, polyaniline (PANI), and PVA. Surprisingly, the film could be assembled as a multifunctional sensor to actively monitor real-time physical and infection related signals such as temperature, moisture, pH, NH 3 , and human movements even at sweat states. More importantly, this multifunctional device could act as a self-driven therapist to eliminate bacterial by the release of Fe 3+ , which was driven by the damage of metal coordination Fe-O bonds due to the high temperature caused by infection at wound sites. Thus, the composite films had potential versatile applications in electronic skins, smart wound dressings, human-machine interactions, and self-driven anti-infection therapy.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 7
·1-13
·
IF 5.833
Wang Xiao-han,Li Wei,Jiang Hong-xin,Chen Yan,Gao Rong-zhi,Tang An-na,Kong De-ming
A heteropore covalent organic framework (COF)-based composite membrane material was prepared and proved to have a satisfactory effect on the pretreatment of vegetable samples. The composite membrane was fabricated by in situ growth of a dual-pore COF on the surface of polydopamine (PDA)-aminated non-woven (NW) fabric. Due to the difference in the strength of the interaction between the phytochromes/COF and the pesticides/COF, the removal of phytochromes and the recovery of pesticides can be achieved by adjusting the composition of the solution. Through a simple immersion or filtration operation, NW@PDA@COF composite membrane can quickly and almost completely remove interfering phytochromes in the samples. The recovery of pesticides was determined by HPLC-MS/MS, and the recovery efficiencies were 72.3~101.7% and 67.3~106.7% for immersion and filtration modes of five different vegetable samples, respectively; the RSD is between 1.1 and 19% ( n = 3). The limits of detection and quantification for the 13 pesticides investigated were 0.08 μg·L −1 and 0.23 μg·L −1 , respectively. A wide linear range of 1~1000 μg·L −1 was observed with R 2 values from 0.9774 to 0.9998. The membrane can be repeatedly used for at least 10 times by using a facile elution treatment. Compared to other commonly used sample pretreatment materials, heteropore COF-based composite membrane is superior in terms of sorbent amount, treatment time, operation simplicity, and material reusability. Graphical abstract
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ACTA PHARMACOLOGICA SINICA
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2021
·Vol. 43
·期 4
·1059-1071
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IF 6.15
Pan Hong,Shi Fu-guo,Fang Chao,Shi Jing-shan
Dendrobine is the main sesquiterpene alkaloid of Dendrobium nobile Lindl, which exhibits potent neuroprotective activity. However, its metabolism and disposition are little known. In this study, we investigated the metabolic characteristics of dendrobine in vitro and in rats. The metabolic stability and temporal profile of metabolites formation of dendrobine were assayed in human/rat liver microsomal and S9 fractions. Dendrobine metabolites were separated and identified mainly by UPLC-Q/Orbitrap MS. After oral administration of dendrobine (50 mg/kg) to rats, the accumulative excretion rate of dendrobine in feces, urine, and bile was 0.27%, 0.52%, and 0.031%, respectively, and low systematic exposure of dendrobine (AUC 0–∞ = 629.2 ± 56.4 ng·h/mL) was observed. We demonstrated that the elimination of dendrobine was very rapid in liver microsomal incubation (the in vitro elimination t 1/2 in rat and human liver microsomes was 1.35 and 5.61 min, respectively). Dendrobine underwent rapid and extensive metabolism; cytochrome P450, especially CYP3A4, CYP2B6, and CYP2C19, were mainly responsible for its metabolism. Aldehyde dehydrogenase, alcohol dehydrogenase and aldehyde oxidase were involved in the formation of carboxylic acid metabolites. By the aid of in-source fragmentation screening, hydrogen/deuterium exchange experiment, post-acquisition processing software, and available reference standards, 50 metabolites were identified and characterized in liver microsomal incubation and in rats. The major metabolic pathways of dendrobine were N -demethylation, N -oxidation, and dehydrogenation, followed by hydroxylation and glucuronidation. Collectively, the metabolic fate of dendrobine elucidated in this study not only yields benefits for its subsequent metabolism study but also facilitates to better understanding the mode of action of dendrobine and evaluating the pharmacologic efficiency of the high exposure metabolites.
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Journal of Bionic Engineering
·
2021
·Vol. 18
·期 3
·559-573
·
IF 2.682
Zhang Ruilong,Zhou Zhiping,Wang Yi,Dai Xiaohui,Chen Li,Dai Jiangdong
Mimicry of nature drives the development of bionic materials. Bionic superhydrophobic materials are a kind of high-efficiency materials to handle oil spills and water pollution. However, the stability of surface coatings of the superhydrophobic materials remains a challenge. Herein, a new category of self-assembly bionic superhydrophobic surface coating was prepared via one-step condensation/copolymerization of vinyltriethoxysilane (VTES) and divinylbenzene (DVB), which realized the close combination of covalent bonds between organic ( e.g. DVB) and inorganic matter ( e.g. VTES), and avoided the swelling of polydivinylbenzene (PDVB) in the process of collection of oil from water. This organic-inorganic hybrid polymer could self-assembly deposit on the surface of sponge even other substrates. For example, P(VTES-DVB)-SiO 2 /MS obtained by assembling P(VTES-DVB)-SiO 2 on the surface of Melamine Sponge (MS) exhibited superhydrophobicity with a Water Contact Angle (WCA) of 157.3°, the optimal adsorption capacity of 77 g·g −1 − 136 g·g −1 for diverse oils, and an excellent separation efficiency of 99.3%. Besides, the excellent acid and alkali resistance of P(VTES-DVB)-SiO 2 /MS suggested the potential value in practical oil-water separation. P(VTES-DVB)-SiO 2 showed the outstanding hydrophobic performance by using as coating on different substrates. This work provided a new idea about the stable combination of organic and inorganic matter in the surface modification.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2021
·Vol. 32
·期 16
·21297-21307
·
IF 2.478
Cao Yong,Luo Penghui,Xu Yang,Zhang Cong,Tian Chang,You Yuanqi,Tian Meiling,Wang Liqiong,Zhou Shenggang
In this paper, a hydrothermal synthesis method synthesized a foamed nickel (NF)-supported Ag-doped Ag 2 S@MoS 2 hydrogen evolution catalyst. Silver doping can improve the conductivity of MoS 2 , thereby improving the hydrogen evolution activity of MoS 2 . Compared with a single MoS 2 , the Ag 2 S@MoS 2 electrode has a larger specific surface area and has many highly catalytic S edges. In 1 M KOH, the overpotential of Ag 2 S@Ag 0.33 MoS 2 /NF electrode at 10 mA cm −2 is approximately 188 mV. Comparing with the overpotential of NF (391 mV) and MoS 2 /NF (290 mV), it is much lower. Further changing the amount of silver added, the overpotential of Ag 2 S@Ag 0.5 MoS 2 /NF is further reduced to 165 mV at a current density of 10 mA cm −2 . When the voltage is 0.35 V, the current densities of Ag 2 S@Ag 0.33 MoS 2 /NF (42.45 mA cm −2 ) and Ag 2 S@Ag 0.5 MoS 2 /NF (55.5 mA cm −2 ) are higher than those of NF (4.91 mA cm −2 ) and MoS 2 /NF (20.51 mA cm −2 ).
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Advanced Fiber Materials
·
2021
·Vol. 4
·期 1
·108-118
·
IF 0
Li Jianwei,Zhang Xuanning,Lu Yuyan,Linghu Keliang,Wang Chen,Ma Zhonglei,He Xinhai
The separator with excellent mechanical and thermal properties are highly required for lithium ion batteries (LIBs). Therefore, it is crucial to develop novel nanofibrous membranes with enhanced mechanical strength and thermal stability. In this work, the fluorinated polyimide (FPI) was synthesized and blended with polyvinylidene fluoride (PVDF) to fabricate composite nanofibrous membranes (CNMs) via electrospinning method. Benefiting from the introduction of aromatic FPI, the prepared PVDF/FPI nanofibrous membranes were endowed with enhanced mechanical strength and thermal stability. When the FPI content increased from 0 to 30 wt%, the tensile strength of composite nanofibrous membranes enhanced from 1.57 to 2.30 MPa. Moreover, there are almost no dimensional shrinkage for the CNM-30 containing 30 wt% FPI after heat treatment at 160 °C for 1 h. Furthermore, the prepared CNMs show improved electrochemical performances in comparison with neat PVDF and commercial Celgard membranes. The electrolyte uptake and ionic conductivity of the CNMs could reach to 522.4% and 1.14 ms·cm −1 , respectively. The prepared CNMs could provide an innovative and promising approach for the development and design of high-performance separators.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 15
·20295-20305
·
IF 2.478
Zhao Yaxin,Liu Dan,Yan Zhuqing,Zhang Zhidong,Zheng Yongqiu,Zhang Yanjun,Xue Chenyang
In recent years, the demand for wearable devices has promoted the research of flexible thermoelectric generators. Herein, this work reports a facile method to prepare the flexible Ag 2 Se/polyvinyl pyrrolidone (PVP) composite films. The Ag 2 Se nanorods are synthesized by the template method and then mixed with PVP solution to form the composite film optimized by the content of Ag 2 Se. The maximum power factor of the film is 16.18 µW m −1 K −2 at 320 K, and the thermoelectric generator (TEG) has an output voltage and power of 5.49 mV and 55.57 nW at a temperature difference of 40 K, respectively. Moreover, the Ag 2 Se/PVP film has good flexibility and can withstand multiple bending, the electrical conductivity reaching 89.8% and 76 % at 500 and 1000, respectively. PVP has an excellent protective capabilities effect so that the TE performance can remain stable in 40 days, and then the electrical conductivity only drops to 89 % of the initial value at 50 days. This work provides an effective method for preparing wearable thermoelectric devices, which can be extended to other composite materials.
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Science China-Life Sciences
·
2021
·Vol. 65
·期 3
·561-571
·
IF 6.038
He Meng,Lin Jie,Akakuru Ozioma Udochukwu,Xu Xiawei,Li Yanying,Cao Yi,Xu Yanping,Wu Aiguo
The detection of circulating tumor cells (CTCs) is a crucial tool for early cancer diagnosis, prognosis, and postoperative evaluation. However, detection sensitivity remains a major challenge because CTCs are extremely rare in peripheral blood. To effectively detect CTCs, octahedral Ag 2 O nanoparticles (NPs) with high dispersibility, good biocompatibility, remarkable surface-enhanced Raman scattering (SERS) enhancement, and obvious enhancement selectivity are designed as an SERS platform. Ag 2 O NPs with many oxygen vacancy defects are successfully synthesized, which exhibit an ultra-high SERS enhancement factor (1.98×10 6 ) for 4-mercaptopyridine molecules. The remarkable SERS activity of octahedral Ag 2 O NPs is derived from the synergistic effect of the surface defect-promoted photo-induced charge transfer (PICT) process and strong vibration coupling resonance in the Ag 2 O-molecule SERS complex, greatly amplifying the molecular Raman scattering cross-section. The promoted PICT process is confirmed using ultraviolet-visible (UV-Vis) absorption spectroscopy, demonstrating that obvious PICT resonance occurs in Ag 2 O SERS system under visible light. An additional growth step of SERS bioprobe is proposed by modifying the Raman signal molecules and functional biological molecules on Ag 2 O NPs for CTC detection. The Ag 2 O-based SERS bioprobe exhibits excellent detection specificity for different cancer cells in rabbit blood. Importantly, the high-sensitivity Ag 2 O-based SERS bioprobe satisfies the requirement for rare CTC detection in the peripheral blood of cancer patients, and the detection limit can reach 1 cell per mL. To our knowledge, this study is the first time that a semiconductor SERS substrate has been successfully utilized in CTC detection. This work provides new insights into CTC detection and the development of novel semiconductor-based SERS platforms for cancer diagnosis.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-10
·
IF 14.919
Liu Gongquan,Zhao Yi-Lei,He Fangyuan,Zhang Peng,Ouyang Xingyu,Tang Hongzhi,Xu Ping
Biodegradation of aromatic and heterocyclic compounds requires an oxidative ring cleavage enzymatic step. Extensive biochemical research has yielded mechanistic insights about catabolism of aromatic substrates; yet much less is known about the reaction mechanisms underlying the cleavage of heterocyclic compounds such as pyridine-ring-containing ones like 2,5-hydroxy-pyridine (DHP). 2,5-Dihydroxypyridine dioxygenase (NicX) from Pseudomonas putida KT2440 uses a mononuclear nonheme Fe(II) to catalyze the oxidative pyridine ring cleavage reaction by transforming DHP into N -formylmaleamic acid (NFM). Herein, we report a crystal structure for the resting form of NicX, as well as a complex structure wherein DHP and NFM are trapped in different subunits. The resting state structure displays an octahedral coordination for Fe(II) with two histidine residues (His 265 and His 318 ), a serine residue (Ser 302 ), a carboxylate ligand (Asp 320 ), and two water molecules. DHP does not bind as a ligand to Fe(II), yet its interactions with Leu 104 and His 105 function to guide and stabilize the substrate to the appropriate position to initiate the reaction. Additionally, combined structural and computational analyses lend support to an apical dioxygen catalytic mechanism. Our study thus deepens understanding of non-heme Fe(II) dioxygenases.
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