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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Free-standing nanoporous NiMnFeMo alloy: An efficient non-precious metal electrocatalyst for water splitting

Hao Liu,Cong Xi,Jinghua Xin,Guoliang Zhang,Shaofei Zhang,Zhijia Zhang,Qin Huang,Jianxin Li,Hui Liu,Jianli Kang

Although significant progresses have been achieved recently in developing efficient catalysts for electrochemical water splitting, high performance catalysts toward hydrogen evolution and oxygen evolution in alkaline electrolyte at high current density (≧1000 mA cm −2 ) have been seldom realized. Herein, we report a flexible and free-standing nanoporous NiMnFeMo alloy (np-NiMnFeMo) with ultrahigh catalytic activity as both anode and cathode even at high current density. The nanoporous NiMnFeMo alloy can deliver as high as 1000 mA cm −2 at an overpotential of only 290 mV for hydrogen evolution reaction and 570 mV for oxygen evolution reaction. DFT calculations indicate that the ultrahigh HER activity of the catalyst is originated from the synergetic effect of the solid solution elements, where Ni atoms act as water dissociation center in the np-NiMnFeMo and the other metals (Mn, Fe and Mo) regulate the electronic structure and provide superior adsorption properties towards hydrogen. More importantly, the electrolyzer, assembled using the np-alloys as both cathode and anode for full water splitting, shows excellent stability.

✓ 已验证 DOI 高影响因子
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Nature Communications · 2021 ·Vol. 12 ·期 1 ·1-9 · IF 14.919

Sea urchin-like microstructure pressure sensors with an ultra-broad range and high sensitivity

Wang Xiu-man,Tao Lu-qi,Yuan Min,Wang Ze-ping,Yu Jiabing,Xie Dingli,Luo Feng,Chen Xianping,Wong ChingPing

Sensitivity and pressure range are two significant parameters of pressure sensors. Existing pressure sensors have difficulty achieving both high sensitivity and a wide pressure range. Therefore, we propose a new pressure sensor with a ternary nanocomposite Fe 2 O 3 /C@SnO 2 . The sea urchin-like Fe 2 O 3 structure promotes signal transduction and protects Fe 2 O 3 needles from mechanical breaking, while the acetylene carbon black improves the conductivity of Fe 2 O 3 . Moreover, one part of the SnO 2 nanoparticles adheres to the surfaces of Fe 2 O 3 needles and forms Fe 2 O 3 /SnO 2 heterostructures, while its other part disperses into the carbon layer to form SnO 2 @C structure. Collectively, the synergistic effects of the three structures (Fe 2 O 3 /C, Fe 2 O 3 /SnO 2 and SnO 2 @C) improves on the limited pressure response range of a single structure. The experimental results demonstrate that the Fe 2 O 3 /C@SnO 2 pressure sensor exhibits high sensitivity (680 kPa −1 ), fast response (10 ms), broad range (up to 150 kPa), and good reproducibility (over 3500 cycles under a pressure of 110 kPa), implying that the new pressure sensor has wide application prospects especially in wearable electronic devices and health monitoring.

✓ 已验证 DOI 高影响因子
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-8 · IF 14.7

Quantifying the conductivity of a single polyene chain by lifting with an STM tip

You Sifan,Yu Cuiju,Gao Yixuan,Li Xuechao,Peng Guyue,Niu Kaifeng,Xi Jiahao,Xu Chaojie,Du Shixuan,Li Xingxing,Yang Jinlong,Chi Lifeng

Conjugated polymers are promising candidates for molecular wires in nanoelectronics, with flexibility in mechanics, stability in chemistry and variety in electrical conductivity. Polyene, as a segment of polyacetylene, is a typical conjugated polymer with straightforward structure and wide-range adjustable conductance. To obtain atomic scale understanding of charge transfer in polyene, we have measured the conductance of a single polyene-based molecular chain via lifting it up with scanning tunneling microscopy tip. Different from semiconducting characters in pristine polyene (polyacetylene), high conductance and low decay constant are obtained, along with an electronic state around Fermi level and characteristic vibrational mode. These observed phenomena result from pinned molecular orbital owing to molecule-electrode coupling at the interface, and weakened bond length alternation due to electron-phonon coupling inside single molecular chain. Our findings emphasize the interfacial characteristics in molecular junctions and promising properties of polyene, with single molecular conductance as a vital tool for bringing insights into the design and construction of nanodevices.

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Journal of Materials Chemistry A · 2024 ·Vol. 12 ·期 45 ·31500-31507 · IF 10.7

An ultrathin phase-inversion induced co-assembly separator for high-performance lithium-metal batteries

Yuying Wang,Fanjun Guo,Mengzhen Zhou,Qian Wu,Tao You,Zhengxiang Zhong,Jiankun Yang,Li Liu,Yudong Huang,Mingqiang Wang

Lithium metal batteries (LMBs) have been regarded as promising electrochemical energy storage systems due to the high theoretical specific capacity of metallic lithium. However, the uncontrolled growth of lithium dendrites, stemming from uneven lithium deposition, poses a significant challenge to their practical implementation. To tackle this issue, an ultra-thin composite separator, consisting of octamethacryloyloxy sesquioxane (MA–POSS), methacryloyloxy trimethoxysilane grafted holey graphene oxide (MPS–HGO), and aramid nanofibers (ANF), was prepared through a combination of phase transition-induced co-assembly and in situ polymerization techniques. Experiments indicate that the composite separator, with a thickness of only 3.8 μm, exhibits exceptional mechanical properties, specifically a tensile strength of 104 ± 5.1 MPa and a modulus of 3.23 ± 0.2 GPa, due to extensive hydrogen bonding and π–π interactions between the HGO sheets and ANF. Furthermore, benefiting from the synergistic effect of the abundant pores in MPS–HGO and the inhibition of stacking through the copolymerization of MPS–HGO and MA–POSS, the composite separator also demonstrates good electrolyte infiltration and a high lithium-ion transport number (tLi+ = 0.87), which not only acts as a physical obstacle but also efficiently regulates Li-ion transport to hinder irregular dendritic growth. The simultaneous regulation of Li-ion transport and mitigation of dendrite growth resulted in a long cycle life for Li|Li cells without dendrite deposition after 1500 cycles at a high current density of 5 mA cm−2. Moreover, the LiFePO4 (LFP)|Li battery with the composite separator displayed a capacity of 154 mA h g−1, a coulombic efficiency of 99%, and a high capacity retention of 99.6% after 250 cycles at 0.5C (85.7% after 1000 cycles at 2C). This work provides a promising new approach to fabricating high-performance lithium battery separators.

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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Soft Artificial Muscle of Poly(vinyl chloride) Gel with an Imperceptible Liquid Metal Electrode

Meng-Ting Xu,Yu Zhu,Chang Wei,Lei Liu,Zicai Zhu,Zhen-Hua Tang,Yuan-Qing Li,Shao-Yun Fu

Electrodes with high electrical conductivity, yet good flexibility and mechanical compliance, are critical for electroactive artificial muscles. Herein, a promising liquid metal (LM) electrode is proposed by transforming eutectic gallium–indium (EGaIn) LM with high surface tension into paste-like LM with solid Ga2O3 shells. The developed compliant LM electrode not only shows high conductivity and negligible additional stiffness but also displays excellent electrical stability during cyclic actuation. Based on the LM electrode, the poly(vinyl chloride) gel (PVCG) artificial muscle developed exhibits the maximum actuation strain of 18.7% at a low electric field strength of 9 V μm–1 and maintains excellent durability without obvious performance attenuation after 10,000 s. A comparison shows that the as-developed PVCG artificial muscle is superior over that based on widely used carbon electrodes. Moreover, an artificial upper limb and crawling worm were manufactured to explore the great potential of PVCG artificial muscle in the robotic field. In addition, the practical application demonstration of the PVCG artificial muscle in the biomimetics field is also successfully fulfilled through the design of reasonable structures. Due to its easy fabrication, excellent electrical conductivity, and high mechanical compliance, the newly developed LM electrode is promising for high-performance PVCG artificial muscles in bionic robots.

✓ 已验证 DOI PubMed 高影响因子
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NANOTECHNOLOGY · 2017 ·Vol. 28 ·期 36 ·365503 · IF 3.44

Fe2Ni2N nanosheet array: an efficient non-noble-metal electrocatalyst for non-enzymatic glucose sensing

Chao You,Rui Dai,Xiaoqin Cao,Yuyao Ji,Fengli Qu,Zhiang Liu,Gu Du,Abdullah M Asiri,Xiaoli Xiong,Xuping Sun,Ke Huang

It is very important to develop enhanced electrochemical sensing platforms for molecular detection and non-noble-metal nanoarray architecture, as electrochemical catalyst electrodes have attracted great attention due to their large specific surface area and easy accessibility to target molecules. In this paper, we demonstrate that an Fe2Ni2N nanosheet array grown on Ti mesh (Fe2Ni2N NS/TM) shows high electrocatalytic activity toward glucose electrooxidation in alkaline medium. As an electrochemical glucose sensor, such an Fe2Ni2N NS/TM catalyst electrode demonstrates superior sensing performance with a short response time of less than 5 s, a wide linear range of 0.05 μM–1.5 mM, a low detection limit of 0.038 μM (S/N = 3), a high sensitivity of 6250 μA mM−1 cm−2, as well as high selectivity and long-term stability.

✓ 已验证 DOI 高影响因子
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MACROMOLECULAR RAPID COMMUNICATIONS · 2024 ·Vol. 45 ·期 13 ·2300737 · IF 4.2

An Intrinsic Photothermal Supramolecular Hydrogel with Robust Mechanical Strength and NIR-Responsive Shape Memory

Ruyue Wang,Xingxing Chen,Yilong Cheng,Zicheng Ding,Xiaoqing Ming,Yanfeng Zhang

Near-infrared (NIR)-triggered shape memory hydrogels with promising mechanical strength hold immense potential in the field of biomedical applications and soft actuators. However, the optical and mechanical properties of currently reported hydrogels usually suffer from limited solubility and dispersion of commonly used photothermal additives in hydrogels, thus restricting their practical implementations. Here,, a set of NIR-responsive shape memory hydrogels synthesized by polyaddition of diisocyanate-terminated poly(ethylene glycol), imidazolidinyl urea (IU), and p -benzoquinone dioxime (BQDO) is reported. The introduction of IU, a hydrogen bond reinforcing factor, significantly enhances the mechanical properties of the hydrogels, allowing for their tunable ranges of the ultimate tensile strength (0.4–2.5 MPa), elongation at break (210–450%), and Young's modulus (190–850 kPa). The unique hydrogels exhibit an intrinsic photothermal effect because of the covalently incorporated photothermal moiety (BQDO), and the photothermal supramolecular hydrogel shows controllable shape memory capabilities characterized by rapid recovery speed and high recovery ratio (>90%). This design provides new possibilities for applying shape memory hydrogels in the field of soft actuators.

✓ 已验证 DOI 高影响因子
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-13 · IF 14.7

An efficient C-glycoside production platform enabled by rationally tuning the chemoselectivity of glycosyltransferases

Li Min,Zhou Yang,Wen Zexing,Ni Qian,Zhou Ziqin,Liu Yiling,Zhou Qiang,Jia Zongchao,Guo Bin,Ma Yuanhong,Chen Bo,Zhang Zhi-Min,Wang Jian-bo

Despite the broad potential applications of C -glycosides, facile synthetic methods remain scarce. Transforming glycosyltransferases with promiscuous or natural O -specific chemoselectivity to C -glycosyltransferases is challenging. Here, we employ rational directed evolution of the glycosyltransferase MiCGT to generate MiCGT-QDP and MiCGT-ATD mutants which either enhance C- glycosylation or switch to O -glycosylation, respectively. Structural analysis and computational simulations reveal that substrate binding mode govern C -/ O -glycosylation selectivity. Notably, directed evolution and mechanism analysis pinpoint the crucial residues dictating the binding mode, enabling the rational design of four enzymes with superior non-inherent chemoselectivity, despite limited sequence homology. Moreover, our best mutants undergo testing with 34 substrates, demonstrating superb chemoselectivities, regioselectivities, and activities. Remarkably, three C -glycosides and an O -glycoside are produced on a gram scale, demonstrating practical utility. This work establishes a highly selective platform for diverse glycosides, and offers a practical strategy for creating various types of glycosylation platforms to access pharmaceutically and medicinally interesting products.

✓ 已验证 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

2D black phosphorus dotted with silver nanoparticles: An excellent lubricant additive for tribological applications

Gongbin Tang,Fenghua Su,Xing Xu,Paul K. Chu

Black phosphorus (BP) is a new two-dimensional (2D) material with attractive nanoscale chemical and physical properties. Herein, black phosphorus dotted with silver nanoparticles (Ag/BP) was synthesized via a facile and in-suit chemical reduction approach without reductant. The tribological properties of as-prepared Ag/BP nanocomposite as lubricant additive in poly-alpha-olefin (PAO6) based oil were investigated by a ball-on-disc tribometer. The results demonstrate that the oil dispersed with trace amount of Ag/BP nanoadditives shows excellent lubricating performance for the steel/steel contact. The friction coefficient and wear rate of the oil dispersed with 0.075 wt% Ag/BP nanoadditives are reduced by 73.4% and 92.0% respectively, as compared to the based PAO6 oil. The possible friction-reducing and anti-wear mechanisms of Ag/BP nanoadditives in oil are illustrated by analyzing the wear scar surfaces. During scratching, the Ag/BP nanomaterials serves not only as a friction-reducing and anti-wear additive, but also as a catalyst to decompose the based PAO oil for forming a carbon-based tribofilm under ambient condition that further reduces the friction and wear. The findings here provide a novel insight into the design of lubricant additive incorporated in base oil and suggests a new potential application of black phosphorus in lubrication and tribology.

✓ 已验证 DOI 高影响因子
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MATERIALS LETTERS · 2021 · IF 3.423

An ultra-strong, ultra-stiff and anti-freezing hydrogel based on poly(vinyl alcohol)

Min Huang,Huan Shi,Ning Wei,Chunhui Luo,Faliang Luo

Polyvinyl alcohol (PVA) hydrogels have drawn enormous attention but are severely limited on account of poor mechanical properties at subzero temperatures. Here, we propose a simple method to tackle this problem by incorporating chain entanglements of PVA chains and coordination bonds between Al 3+ ions and –OH groups via air-drying and soaking in Al 2 (SO 4 ) 3 solution. The multiple dynamic interactions worked in tandem to achieve outstanding mechanical performance (41.0 MPa of fracture stress and 49.9 MJ/m 3 of toughness). Meanwhile, the introduction of ions endowed the PVA hydrogel with excellent anti-freezing property (36.9 MPa of fracture stress and 51.4 MJ/m 3 of toughness at −20 ℃), superior to most anti-freezing gels at subzero temperatures. The facile synthesis and superior properties might expand the application of PVA hydrogels.

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Nanoscale · 2019 ·Vol. 11 ·期 43 ·20942-20948 · IF 6.97

Anomalous variable-temperature photoluminescence of CsPbBr3 perovskite quantum dots embedded into an organic solid

Fei Tang,Zhicheng Su,Honggang Ye,Ye Zhu,Jiyan Dai,Shijie Xu

All-inorganic lead halide perovskite quantum dots (PQDs) of CsPbBr3 were synthesized at room temperature via a facile solution-based procedure. The cubic phase structure of the synthesized PQDs was judiciously identified through examining high-resolution transmission electron microscopy (TEM) images, selected area electronic diffraction (SAED) patterns and scanning TEM images of the PQDs. Variable-temperature photoluminescence (PL) spectra of the CsPbBr3 PQDs randomly embedded into a frozen solid of methylbenzene were measured in the temperature range of 5–180 K. It is found that both the linewidth and peak position of the measured PL spectra are abnormally almost temperature independent in the temperature range of interest. Some competing mechanisms, such as a competition between the bandgap blue shift induced by thermal lattice expansion and red shift induced by thermal escaping of localized excitons, and a competition between lineshape broadening by phonon scattering and narrowing by thermal escaping of localized excitons, are proposed to interpret the phenomena. Good agreement between the theoretical fitting and the experimental data leads to a state-of-the-art understanding of the temperature-dependent luminescence of the CsPbBr3 PQDs in a solid matrix.

✓ 已验证 DOI 高影响因子
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ChemSusChem · 2020 ·Vol. 13 ·期 16 ·4151-4158 · IF 7.962

Oxidative Esterification of 5-Hydroxymethylfurfural with an N-doped Carbon-supported CoCu Bimetallic Catalyst

Huai Liu,Ning Ding,Junnan Wei,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Huayu Fang,Tianyuan Li,Lu Lin

Graphical No base needed : N-doped carbon-supported CoCu bimetallic catalyst with enhanced O 2 activation ability and basicity is demonstrated as an effective catalyst for the oxidative esterification of 5-hydroxymethylfurfural. The introduction of Cu significantly enhances the catalytic activity, resulting in a high furan-2,5-dimethylcarboxylate yield and an impressive formation rate, paving the way for the efficient and green synthesis of sustainable bio-based polymer monomers. The direct fabrication of furan-2,5-dimethylcarboxylate (FDMC), a promising renewable monomer, from biomass-derived 5-hydroxymethylfurfural (HMF) is a cutting-edge process. In this contribution, an elaborately designed N-doped carbon-supported CoCu bimetallic catalyst (Co x Cu y -NC; x / y= 9:1, 7:3, 4:6, which represents the designed molar ratio of Co and Cu in the catalyst), which could offer a desirable FDMC yield of 95 % under mild and base-free conditions (Co 7 Cu 3 -NC, 2 bar O 2 , 80 °C, 4 h) is described for the oxidative esterification of HMF. Notably, an FDMC formation rate of 6.1 mol FDMC mol Co −1 h −1 was achieved over Co 7 Cu 3 -NC, which represents the highest catalytic efficiency so far among Co-based catalytic systems. It has been demonstrated that Cu-doping in Co 7 Cu 3 -NC catalyst brings about more active sites (Co-N x species) with stronger molecular oxygen activation ability. The increase of surface N content of Co 7 Cu 3 -NC also improves basicity of the catalyst, which favors the hydrogen abstraction process during the HMF oxidative esterification reaction. These findings may pave an efficient and green way for the synthesis of sustainable bio-based polymer monomers.

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