Nature Communications
·
2023
·Vol. 14
·期 1
·1-8
·
IF 16.6
Chen Biao,Huang Wenhuan,Zhang Guoqing
Pure organic room-temperature phosphorescence (RTP), particularly from guest-host doped systems, has seen exponential growth in the last several years due to their high modulation flexibility, and yet challenges remain with respect to mechanistic elucidations and advantageous applications. Here we show that by constructing guest-host doped RTP systems from chiral components, namely, chiral amino compound-modified phthalimide hosts and naphthalimide guests, a chiral-selective RTP enhancement phenomenon can be observed. For example, R -enantiomeric guests in R -enantiomeric hosts produce strong red RTP afterglow while no appreciable RTP could be observed in the S-R guest-host counterpart. An unprecedented RTP intensity difference > 10 2 folds with the ability to distinguish an enantiomeric excess of 98% could be achieved. Temperature-dependent measurements suggest that a chirality-dependent energy transfer process may be involved in the observed phenomenon, which can be harnessed to extend the RTP application to the chiral recognition of amino compounds, such as amino alcohols.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Ruiming Chen,Tingting Hu,Shu Xing,Tao Wei,Jianbin Chen,Tianduo Li,Qingfen Niu,Zhengyang Zhang,Huijun Ren,Xiaoxu Qin
Hydrazine (N 2 H 4 ) and hypochlorite (ClO − ) are extremely harmful to the public health, so it is vitally necessary to detect them in living system. Herein, we developed a new phenthiazine-thiobarbituric acid based dual-analyte responsive fluorescent sensor PT for visually distinguishing and detecting N 2 H 4 and ClO − . PT underwent N 2 H 4 /ClO − -induced C C breakage, achieving olive-drab/brilliant green fluorescence lighting-up response towards N 2 H 4 /ClO − with superb specifity, ultra-sensitivity (detection limit: 15.4 nM for N 2 H 4 , 13.7 nM for ClO − ), and ultra-fast response (N 2 H 4 : <15 s, ClO − : <20 s). The mechanisms for sensing N 2 H 4 and ClO − were investigated with support of spectral measurements and DFT investigation. Sensor based paper-strip/silica-gel device was developed for in-field supervision and on-site monitoring of gaseous and aqueous N 2 H 4 and ClO − solution. In addition, the PT was also applied for quantitatively detecting N 2 H 4 and ClO − in soil, food, plants and bio-fluids. Moreover, PT was utilized to visualize exogenous N 2 H 4 and ClO − in living plants and live-cells, demonstrating this sensor utilized as a powerful tool to detect N 2 H 4 and ClO − in biological fields.
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Reaction Chemistry & Engineering
·
2022
·Vol. 8
·期 3
·645-655
·
IF 5.2
Zhenhua Tian,Jianzhong Ma,Qiwu Liu,Hui Zhang
Amphoteric acrylic polymers are some of the commonly used leather retanning agents, and possess assistant-dyeing function in contrast to traditional anionic acrylic retanning agents. To further enhance the cationic modification degree of anionic acrylic retanning agents, various amines (dimethylamine, diethylamine, dipropylamine, diethanolamine, dicyclohexylamine and diphenylamine) with different structural characteristics were selected as raw materials to prepare amphoteric acrylic retanning agents via the Mannich reaction. Then, the obtained amphoteric acrylic retanning agents were used in leather-making, and the retanning and assistant-dyeing properties were investigated. Compared with the anionic acrylic retanning agents, all amphoteric acrylic retanning agents have better assistant-dyeing owing to the presence of amino groups. The retanning agents modified by different amines exhibit different properties. The amination degree of the acrylic polymer retanning agent modified by diethanolamine was the highest (40.8%) and had better assistant-dyeing, which was confirmed by its highest dye-uptake (87.5%) and K/S value (17.0). The tensile strength of leather retanned with diphenylamine-modified acrylic polymer was the highest (23.6 MPa). The thickening rate of the leather retanned with dipropylamine-modified acrylic polymer was the highest (23.8%). Considering these properties, the overall performance of the amphoteric acrylic polymer modified by diethanolamine was found to be the best.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 43
·2303272
·
IF 19
Si Yu Zheng,Jiahui Zhou,Mengjie Si,Shuaibing Wang,Fengbo Zhu,Ji Lin,Jimin Fu,Dong Zhang,Jintao Yang
Polyzwitterionic hydrogel is an emerging material for solar-driven water evaporation in saline environment due to its special anti-polyelectrolyte effect, which is a promising approach to co-generation of freshwater and electricity. However, the molecular impact on anti-polyelectrolyte effect remains unclear, let alone to optimize the zwitterionic structure to promote water evaporation efficiency in high-salinity brine. Herein, a molecularly engineered zwitterionic hydrogel is developed and the incorporated phenyl-methylene-imidazole motif greatly enhances the salt binding ability and strengthens anti-polyelectrolyte effect, leading to boosted hydration, improved salt tolerance, ultra-low evaporation enthalpy (almost half of traditional zwitterionic gel), and durable anti-microbial ability in brine. Besides, gradient solar-thermal network is penetrated to optimize water transport channel and heat confinement. The gel exhibits excellent evaporation rate of 3.17 kg m −2 h −1 in seawater, which is 1.6 times of that in water and such high efficiency could be maintained during 8 h continuous desalination, demonstrating outstanding salt tolerance. The high flux of ion stream can generate considerable voltage (321.3 mV) simultaneously. This work will bring new insights to the understanding of anti-polyelectrolyte effect at molecular level and promote materials design for saline water evaporation.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yue Liu,Dianlong Ge,Jijuan Zhou,Yajing Chu,Xiangxue Zheng,Li Ke,Pan Li,Yan Lu,Xue Zou,Lei Xia,Yawei Liu,Chaoqun Huang,Chengyin Shen,Yannan Chu
The investigation of volatile organic compounds (VOCs) in human metabolites has been a topic of interest as it holds the potential for the development of non-invasive technologies to screen for organ lesions in vivo. However, it remains unclear whether VOCs differ among healthy organs. Consequently, a study was conducted to analyze VOCs in ex vivo organ tissues obtained from 16 Wistar rats, comprising 12 different organs. The VOCs released from each organ tissue were detected by the headspace-solid phase microextraction-gas chromatography-mass spectrometry technique. In the untargeted analysis of 147 chromatographic peaks, the differential volatiles of rat organs were explored based on the Mann–Whitney U test and fold change (FC > 2.0) compared with other organs. It was found that there were differential VOCs in seven organs. A discussion on the possible metabolic pathways and related biomarkers of organ differential VOCs was conducted. Based on the orthogonal partial least squares discriminant analysis and receiver operating characteristic curve, we found that differential VOCs in the liver, cecum, spleen, and kidney can be used as the unique identification of the corresponding organ. In this study, differential VOCs of organs in rats were systematically reported for the first time. Profiles of VOCs produced by healthy organs can serve as a reference or baseline that may indicate the presence of disease or abnormalities in the organ’s function. Differential VOCs can be used as the fingerprint of organs, and future integration with metabolic research may contribute to the development of healthcare.
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ADVANCED MATERIALS
·
2022
·Vol. 34
·期 45
·2205028
·
IF 32.086
Yuqi Cui,Jiangjian Shi,Fanqi Meng,Bingcheng Yu,Shan Tan,Shan He,Chengyu Tan,Yiming Li,Huijue Wu,Yanhong Luo,Dongmei Li,Qingbo Meng
All-inorganic CsPbI 3 perovskite has emerged as an important photovoltaic material due to its high thermal stability and suitable bandgap for tandem devices. Currently, the cell performance of CsPbI 3 solar cells is mainly subject to a large open-circuit voltage ( V OC ) deficit. Herein, a multifunctional room-temperature molten salt, dimethylamine acetate (DMAAc) is demonstrated, which not only directly acts as a solvent for precursor solutions, but also regulates the phase conversion process of the CsPbI 3 film for high-efficiency photovoltaics. DMAAc can stabilize the DMAPbI 3 structure and eliminate the Cs 4 PbI 6 intermediate phase, which is easily spatially segregated. Meanwhile, a new homogeneous intermediate phase DMAPb(I,Ac) 3 is formed, which finally affords high-quality CsPbI 3 films. With this approach, the charge capture activity of defects in the CsPbI 3 film is significantly suppressed. Consequently, a V OC of 1.25 V and >21% power conversion efficiency are achieved, which is the record highest reported thus far. This intermediate phase-regulation strategy is believed to be applicable to other perovskite material systems.
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JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Weifeng Zhang,Guoxing Jiang,Wenwu Zou,Longhai Zhang,Shulian Li,Shengguang Qi,Xiujun Wang,Zhiming Cui,Huiyu Song,Li Du,Zhenxing Liang
The parasitic side reaction between the electrolyte and the lithium metal (Li 0 ) forms an unstable heterogeneous interphase, causing the poor reversibility of Li plating/stripping. The rational design of protection layer on Li 0 anode is imperative to inhibit side reactions and achieve fast Li + transport on the Li 0 /electrolyte interface. Herein, by firstly coordinating the bis(fluorosulfonyl)imide anion (FSI − ) to the protection layer, a layer consisting of 2D ionic vinylene-linked covalent organic frameworks (ivCOF-FSI) is proposed to stabilize the Li 0 /electrolyte interface. As demonstrated theoretically and experimentally, the triazine group in the cationic framework is identified to promote Li + de-solvation process while partial FSI − prefers to form LiF-rich interphase. Attributed to these superiorities, the ivCOF-FSI layer endows the Li 0 /electrolyte interface with high reversibility in carbonate-based electrolytes by simultaneously suppressing the side effect and achieving rapid Li + transfer. Combined with the high stability of solid-liquid interface, the LiFePO 4 full cells with ivCOF-FSI/Li anode display enhanced cyclability under a high cathode loading of 9.4 mg cm −2 and a low negative/positive capacity ratio of 5. This work provides a novel route for stabilizing the interfacial chemistry of solid-liquid interface, aiming to pave the way for the next-generation high-energy-density batteries .
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Menglan Gao,Xiaobin Liao,Jing Yu,Xinna Lin,Huan Qi,Linlu Shen,Shupo Liu,Zhimin Yang
Bromide ions (Br - ) affected non-brominated nitroso-dimethylamine (NDMA) formation during ozonation , but the mechanism is still unclear. 1,1,1′,1′-tetramethyl-4,4′-(methylene-di- p -phenylene) di-semicarbazide (TMDS) was chosen to further probe this problem. The results indicated that low levels of Br - (≤20 μM) enhanced NDMA from 3.27 to 7.56 μg/L, while its amount slightly dropped to 6.22 μg/L raising Br - to 100 μM. It was experimentally verified that intermediates 1,1-dimethylsemicarbazide (DMSC) and 1,1-dimethylhydrazine (UDMH) played important roles on promoting NDMA generation, whose contribution rates were 40.2% and 32.2%, respectively. The brominated substances with higher NDMA molar yields were detected. ∙OH reduced NDMA formation without Br - , while it played promotion role with Br - ; the corresponding contribution rates were − 26.9% and 29.2%, respectively. No matter with or without Br - , both ∙O 2 - and l O 2 brought a boost to NDMA formation, their contribution ratios were 34.9% and 58.1% without Br - , while raised significantly to 64.6% and 81.5% when Br - existed. Br - not only facilitated NDMA formation, but also benefited the degradation of TMDS. Based on the calculation results and intermediates detected, the influence mechanisms of Br - were proposed. The results would provide theoretical basis and technical guarantee for treating NDMA precursors and bromide co-existing water in the future.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 44
·2205597
·
IF 19.924
Si Yu Zheng,Jiahui Zhou,Shuaibing Wang,Yan-Jie Wang,Shanqiu Liu,Guangyan Du,Dong Zhang,Jimin Fu,Ji Lin,Zi Liang Wu,Qiang Zheng,Jintao Yang
Developing conductive underwater glue for fast sealing and in situ monitoring is critical for ocean exploration yet remains a challenge. The fluidity of glue is a double-edged sword that is favorable for molecule spreading and formation of interlocking bonding network yet also leads to leakage of conductive ions. Herein, a polymeric glue possessing good conductivity and exhibiting rapid, strong, and long-lasting underwater adhesion on diverse substrates at various harsh environments and extreme temperatures is developed. For molecular design, the nitrogen heterocyclic motif that prevails in biomolecular recognition is encoded with water-resistant benzene block in one pendant group to serve as underwater binding sites; ionic liquids (ILs) of [EMIM][BF4] is employed as the solvent for fast water exchange that triggers rapid adhesion. Simultaneously, the polymer-IL interaction is regulated, with the assistance of the theoretical calculations, to retain sufficient ILs within the adhesive for sensing. Finally, the glue is applied for underwater sealing and in situ monitoring various physical signals, while the fluorescent property is utilized for underwater labeling. This study should provide a new design strategy for the next-generation of multifunctional underwater adhesives and promote their applications.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Yan Xiao,Junhui Xu,Lei Hu,Hui Wang,Li Gao,Shiqi Peng,Mengting Di,Xiaojun Sun,Jie Liu,Xiaoming Yan,Liuping Chen,Gaohong He
Neutral aqueous organic redox flow battery (NAORFB) stands out as one of the most prospective mass energy storage options. The main limitations of large-scale storage regarding the NAORFB lie in the low Na + /Cl − conductivity of membrane in pH7 systems, which leads to a lower voltage efficiency. Herein, quaternary ammonium functionalized fluorinated poly (arylene ether) (QAFPAE-x) anion exchange membrane with hydrophilic and hydrophobic blocks was designed successfully. The results demonstrated that the grafting of quaternary ammonium and fluorine-containing block enables QAFPAE-x membrane low swelling, high Cl − conductivity, and promising chemical stability characteristics. The voltage efficiency of QAFPAE-100 membrane (93.8%–60.7%) is much higher than the AMVN membrane (88.4%–37.8%) at 20–160 mA cm −2 . Furthermore, the NAORFB with the QAFPAE-100 membrane steadily runs at 60 mA cm −2 over 1500 cycles. Therefore, the ionic highway induced excellent performance of QAFPAE-100 membrane to render this material a promising candidate for practical NAORFB applications.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2022
·Vol. 331
·期 4
·1759-1767
·
IF 1.754
Liu Yaoyang,Liu Zhibin,Zhao Chuang,Jiao Caishan,Zhang Meng,Zhou Yu,Gao Yang,Li Huibo,He Hui
In order to further study the structure-performance relationship of unsymmetrical diglycolamides. In this work, two types of unsymmetrical diglycolamides (Structure A : N,N’ -dimethyl- N,N’ -didecyl diglycoamide, L I , N,N’ -dimethyl- N,N’ -didodecyl diglycoamide, L III ; Structure B : N,N -dimethyl- N’,N’ -didecyl diglycoamide, L II , N,N -dimethyl- N’,N’ -didodecyl diglycoamide, L IV ), which are geometrical isomers each other, were synthesized, and their extraction performances in 40/60 (v/v)% n-octanol/kerosene were studied and compared. The related results reveal that the size of the alkyl substituents attached on the amide N atoms can influence the extractant performance of the extractant, and the difference in the geometric structure of extractants can lead to the differences in their extraction performances.
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Acta Biomaterialia
·
2022
·
IF 10.633
Ziting Liu,Yaozhen Yi,Lingjie Song,Yuxiang Chen,Limei Tian,Jie Zhao,Luquan Ren
Bio-inspired nanostructures have demonstrated highly efficient mechano-bactericidal performances with no risk of bacterial resistance ; however, they are prone to become contaminated with the killed bacterial debris. Herein, a biocompatible mechano-bactericidal nanopatterned surface with salt-responsive bacterial releasing behavior is developed by grafting salt-responsive polyzwitterionic (polyDVBAPS) brushes on a bio-inspired nanopattern surface. Benefiting from the salt-triggered configuration change of the grafted polymer brushes , this dual-functional surface shows high mechano-bactericidal efficiency in water (low ionic strength condition), while the dead bacterial residuals can be easily lifted by the extended polymer chains and removed from the surface in 1 M NaCl solution (high ionic strength conditions). Notably, this functionalized nanopatterned surface shows selective biocidal activity between bacterial cells sand eukaryotic cells. The biocompatibility with red blood cells (RBCs) and mammalian cells was tested in vitro. The histocompatibility and prevention of perioperative contamination activity were verified by in vivo evaluation in a rat subcutaneous implant model. This nanopatterned surface with bacterial killing and releasing activities may open new avenues for designing bio-inspired mechano-bactericidal platforms with long-term efficacy, thus presenting a facile alternative in combating perioperative-related bacterial infection. Statement of significance Bioinspired nanostructured surfaces with noticeable mechano-bactericidal activity showed great potential in moderating drug-resistance. However, the nanopatterned surfaces are prone to be contaminated by the killed bacterial debris and compromised the bactericidal performance. In this study, we provide a dual-functional antibacterial conception with both mechano-bactericidal and bacterial releasing performances not requiring external chemical bactericidal agents. Additionally, this functionalized antibacterial surface also shows selective biocidal activity between bacteria and eukaryotic cells, and the excellent biocompatibility was tested in vitro and in vivo. The new concept for the functionalized mechano-bactericidal surface here illustrated presents a facile antibiotic-free alternative in combating perioperative related bacterial infection in practical application.
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危险品化学品经营许可证（带存储）