COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Yumeng Lian,Yi Wang,Dun Zhang,Likun Xu
Developing a stable and reusable material for antibacterial application in an enzyme-like system is still a challenge. Herein, Mn–Co–S–Se (MnCo 2 S x Se 4–x )/Ni foam (NF) are synthesized by introducing S 2– and Se 2– in MnCo 2 O 4 /NF with a facile hydrothermal approach. With the different molar ratios of S/Se, the surface morphology of MnCo 2 S x Se 4–x /NF shows different growth and the catalytic activity also presents regular changes. MnCo 2 S 3.1 Se 0.9 /NF possesses a high enzyme-like ability with higher V max than natural horseradish peroxidase . Due to the outstanding peroxidase-like activity, MnCo 2 S 3.1 Se 0.9 /NF also exhibits broad-spectrum bactericidal performance towards Escherichia coli and Staphylococcus aureus which stems from the formation of ·O 2 – from H 2 O 2 . In the reutilization experiment, the enzyme-like activity keeps a stable value after 25 cyclic tests and the bactericidal performance is still stable after 10 cyclic tests, proving that MnCo 2 S 3.1 Se 0.9 /NF possesses relative stability and reusability. This research showed the great prospect of new energy and environmental catalysis.
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高影响因子
CHEMISTRY OF MATERIALS
·
2020
·
IF 9.567
Huanhuan Jia,Xinmiao Liang,Tao An,Linfeng Peng,Jiwen Feng,Jia Xie
Finding sodium solid electrolytes (SSEs) with good performance is key to building all-solid-state sodium batteries. In the development of solid electrolytes, halogen doping has been shown to be an effective approach. However, it has rarely been applied to chalcogenide-based SSEs, possibly because of strict structure constraints. In this work, the strategy of halogen doping is successfully demonstrated on Na3.67[Sn0.67Si0.33]0.67P0.33S4, a novel SSE with high structural tolerance. The halogen-doped samples formulated as Na3.57[Sn0.67Si0.33]0.67P0.33S3.9X0.1 (X = Cl, Br, and I) exhibit higher ionic conductivities and lower activation energies than the pristine sample. Na3.57[Sn0.67Si0.33]0.67P0.33S3.9I0.1, the I-doped sample, has the highest ambient ionic conductivity of 1.08 mS cm–1 and the lowest activation energy of 0.24 eV. Structure analysis indicates that the high electronegativity of Cl atoms plays an important role in improving the conduction of Na+ ions in Cl-doped samples. The large atomic radius and high polarizability of I are more important factors to accelerate the transportation of Na+ ions in the I-doped counterpart. Furthermore, the all-solid-state sodium batteries assembled with Na3.57[Sn0.67Si0.33]0.67P0.33S3.9I0.1 as solid electrolytes show decent cyclic stability at 30 °C with a current density of 0.15 A g–1. This work systematically manifests the effect of halogen doping in SSEs, providing a versatile method to develop novel SSEs.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Bo Wang,Yanhong Liu,Jinhui Hao,Junbo Zhong,Furong Yu,Kewei Zhang,Hao Shen,Baodong Mao
Earth-abundant metal sulfides attracts large attention in recent years for hydrogen production via electrocatalytic water splitting. However, most works have been limited to the acidic condition, whereas the hydrogen evolution reaction (HER) in alkaline condition has rarely been discussed. Here we present an effective strategy for the growing of Co-Mo-S catalysts on carbon cloth via the controllable incorporation of cobalt into MoS 2 with L-cysteine and phosphomolybdic acid to achieve the synergistic interaction of CoS 2 and MoS 2 . The optimized Co-Mo-S catalysts (Co:Mo=1:2) showed a largely improved HER activity with an overpotential of 92 mV at current density of 10 mA cm -2 and Tafel slope of 82 mV dec -1 . The origin of the activity enhancement was investigated through a series of characterizations, where the synergetic effect of the intrinsic fast HER kinetics of metallic CoS 2 and the high active surface area of MoS 2 plays a crucial role. With appropriate amount of cobalt, the Co-Mo-S catalysts show a relatively uniform distribution on the carbon cloth to ensure the large surface area, whereas excessive cobalt results in the formation of the large CoS 2 particles with low HER activity from the low active surface area. Further electrochemical measurements demonstrated that the combination of larger exchange current density of CoS 2 and the high electrochemical double–layer capacitance (proportional to the active surface area) of MoS 2 together contributed to the HER activity enhancement of the Co-Mo-S catalysts. The Co-Mo-S/CC catalysts also show robust stability in alkaline solution. Our work provides a more profound understanding and an interesting view for the design of efficient ternary transition metal sulfide HER catalysts in alkaline condition by synergetic optimization of the intrinsic HER kinetics and the electrochemical active surface area.
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高影响因子
ACS Applied Materials & Interfaces
·
2014
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IF 5.9
Pei Yu Xu,Ke Zhou,Guang Lu Han,Qiu Gen Zhang,Ai Mei Zhu,Qing Lin Liu
Two kinds of novel multiblock poly(arylene ether sulfone)s were synthesized via block copolycondensation of telechelic oligomers as a starting material for the preparation of anion-exchange membranes (AEMs). The as-synthesized copolymers have extremely similar main chains. The difference is that the benzylmethyl groups for one are located on the fluorene–sulfone segments and they are located on the isopropylidene–sulfone segments for the other. The benzylmethyl moieties served as precursors to cationic sites and were brominated using N-bromosuccinimide (NBS) and then quaternized with N,N,N′,N′-tetramethyl-1,6-diaminohexane (TMHDA). Controlled bromination and quaternization at specific positions of the benzylmethy-containing fluorene–sulfone segments and isopropylidene–sulfone segments can be achieved. 1H NMR spectroscopy, Fourier transform infrared spectroscopy, and gel permeation chromatography were used to characterize the as-synthesized copolymers. Distinct microphase separation in the as-prepared AEMs was observed using small-angle X-ray scattering and transmission electron microscopy. The AEM containing fluorene–sulfone segments (IEC = 1.89 meq·g–1) showed higher ionic conductivity and methanol permeability than that containing isopropylidene–sulfone segments (IEC = 2.03 meq·g–1). Moreover, the former showed better alkaline stability than the latter.
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高影响因子
DALTON TRANSACTIONS
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2017
·Vol. 46
·期 9
·2778-2784
·
IF 4.029
Guang-mao Li,Qiong Liu,Kui Wu,Zhi-hua Yang,Shi-lie Pan
In view of their inherent defects for commercial infrared nonlinear optical (IR NLO) materials, exploration for new IR NLO materials with excellent performance is an imperative and meaningful work. Herein, we report the successful design and synthesis of two metal-mixed chalcogenides containing divalent cations with d10 electronic configuration: Na2CdGe2S6 and Na2CdGe2Se6. Both of them crystallize in the polar Cc space group and exhibit three-dimensional tunnel structures constructed by the CdQ4 tetrahedra and ∞[GeQ3]n chains with Na+ located in the tunnels. Furthermore, an interesting space group transformation between the monoclinic (Cc) and tetragonal (I4/mcm) systems from Na2CdGe2Se6 to Na2ZnGe2Se6 was discovered, which may arise from the different connection types of their building blocks (more flexible corner-sharing type in Cc while tightly edge-sharing type in I4/mcm). Remarkably, they exhibit type-I phase-matching abilities and large second harmonic generation (SHG) responses (0.8 and 2 times that of benchmark AgGaS2 at 2.09 μm fundamental light). Notably, Na2CdGe2S6 satisfies the essential requirements (coexistence of large NLO response and high laser damage threshold) as one excellent IR NLO material. The structure–property relationship has also been investigated through theoretical calculations and the results indicate that the origin of their NLO effects can be attributed to CdQ4 and GeQ4 units.
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Journal of Biobased Materials and Bioenergy
·
2022
·Vol. 16
·期 3
·367-373
·
IF 0.687
Zhang Yingwei,Wang Chunhua,Yi Yong,Wang Wenzhi,Yang Jun,Lou Yibo,Li Jianlin
Three diimide diacid (DIDA) monomers possessing different rigid groups (phenyl, biphenyl and diphenyl ether group) between two imide rings were prepared through the dehydration cyclization reaction of 11-aminoundecanoic acid and aromatic dianhydride. These DIDA monomers were polymerized
with 1,10-diaminodecane to produce bio-based poly(amide imide)s (PAIs) by the ecofriendly and low-cost two-step polymerization method. All the PAIs have high thermal stabilities, and their initial thermal decomposition temperatures are above 400 °C at 5% weight loss. When the rigid group
between two imide rings is changed from phenyl to diphenyl ether group, the glass transition temperature of PAI shows a decreasing trend from 54.7 °C to 42.4 °C, the tensile strength also reduces from 62.4 MPa to 49.5 MPa, but elongation at break increases from 3.7% to 6.8%. Moreover,
the PAI with phenyl group between two imide rings is a semicrystalline polymer, while the PAI with biphenyl or diphenyl ether group is an amorphous polymer. It is a viable way to regulate the properties of PAIs by changing the structure of rigid group between two imide rings. Such bio-based
PAIs with high thermal stabilities, low glass transition temperatures and good mechanical strength will provide great promise for their wider applications.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Fanghui Wang,Qian Zhang,Zenghua Liu,Mingxiu Hou,Zhenjiang Li,Jie Liu,Rongfang Wang,Lei Wang
The development of Li-S battery has been seriously hindered by the shuttle effect of polysulfides and the mechanical instability of the sulfur electrode during cycling. Constructing strong-affinity oxide hosts is an effective way to anchor the polysulfides . And then the oxide hosts with sulfur active materials need additional binder to adhere them to the current collector, and they also possess poor ability to suppress the volume change of sulfur cathode. Herein, a bifunctional lithium polysilicate (Li 2 O·nSiO 2 , LSO) as highly efficient adhesion agent and anchoring host has been exploited for long-lifespan Li-S battery. Like other oxide hosts, density functional theory (DFT) calculations reveal that LSO also displays strong chemisorption effect towards polysulfides. Specially, the LSO shows impressive adhesive property and mechanical strength , which make it act as a robust binder to improve the mechanical stability of the sulfur electrode. The sulfur cathode with LSO as the highly efficient adhesion agent and anchoring host can give an excellent cycling stability with ∼ 0.076 % capacity decay per cycle at 0.5C for 500 cycles. This work lights a new way to improve the chemical and mechanical stability of sulfur cathodes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Liying Sun,Xuesong He,Bin Liu,Shuming Zhang,Zheng Xiang,Xin Wang,Yang Wang
The development of materials with dual adsorption/photocatalytic functions for the removal of difficult-to-degrade organics is a very promising and challenging strategy. In this paper, a novel S-scheme heterojunction photocatalyst, InVO 4 /ZnIn 2 S 4 , was successfully synthesized with a unique hierarchical structure, which provides plenty of accessible adsorption/photocatalytic sites with a high light-harvesting rate (by multiple reflections). The experimental results show that optimized InVO 4 /ZnIn 2 S 4 (5-IV/ZIS) has superior removal performance, whose adsorption-photocatalytic synergistic removal of tetracycline (TET) can reach 69.31 % after 15 min and 90.69 % after 45 min. Based on the analysis of the mechanism, the excellent removal performance can be attributed to the adsorption of the target onto the material by hydrogen bonding, followed by the degradation of the adsorbed target by active substances ( h + > O 2 •− > e - > 1 O 2 > • OH) generated by the S-scheme heterojunction. In addition, the possible pathways for the photocatalytic removal of TET on 5-IV/ZIS were investigated by HPLC-MS analysis. T.E.S.T. and E. coli inhibition experiments demonstrated a significant reduction in the toxicity of TET after the photocatalytic reaction. In conclusion, the novel multifunctional photocatalyst 5-IV/ZIS prepared in this study can be used for the efficient treatment of organic compounds in wastewater with a bright application prospect.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Lihong Tan,Xinhe Wu,Jiachao Xu,Mahmoud Sayed,Guohong Wang
The construction of crystalline/amorphous g-C 3 N 4 homojunctions presents a versatile strategy to obtain all-organic homojunction photocatalysts with better interface matching and lower interface charge carrier movement resistance for optimized photocatalytic activity. However, the process entails a complex multi-step workup, which compromises its feasibility. To overcome this challenge, this work provided an innovative Na 2 CO 3 -induced crystallinity modulation strategy to construct a Na-doped crystalline/amorphous g-C 3 N 4 S-scheme homojunction photocatalyst in a single step. The approach involves the initial pre-assembling of melamine and cyanuric acid molecules, and subsequent introduction of Na 2 CO 3 before the calcination. Na 2 CO 3 plays key roles to induce in-situ crystallinity modulation during the calcination and as a source for Na-doping. The prepared g-C 3 N 4 S-scheme homojunction photocatalyst demonstrated a prominent H 2 O 2 -production rate of 444.6 μmol·L –1 ·h –1 , which is 6.1-fold higher than that of bulk g-C 3 N 4 . The enhanced activity was attributed to the synergistic effect of charge carrier separation induced by the S-scheme homojunction system, and the optimized interfacial H 2 O 2 generation kinetics. The latter was fostered by the Na-doping. This study provides an innovative approach for the one-step construction of g-C 3 N 4 S-scheme homojunction and its integration in photocatalytic applications.
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高影响因子
Theranostics
·
2020
·
IF 8.579
Ping Liu,Yidan Wang,Yang Liu,Fengping Tan,Jining Li,Nan Li
To a large extent, the dense extracellular matrix (ECM), which tightly connects tumor cells to arm the tumor into an intractable fortress, significantly decreases the nanoparticles delivery efficacy and overall performance in cancer treatments. Therefore, it is necessary to transform the dense stroma of solid tumors to loose state, which could realize deep penetration of nanomedicine and enhance cancer treatment effects. Here, we fabricated a protein-free collagen nanosweeper, triphenylphosphonium bromide (TPP) coated and S-nitrosothiols loaded mini-sized Au@silica nanorod (Au@SiO 2 -SNO/PEG/TPP, GSNP-TPP), to clear the transport barriers of nanoparticles as well as elevate enhanced permeability and retention (EPR) effect, thus alleviating the diffusion resistance and realizing further penetration of nanoparticles. Methods: By modifying the Au@silica with thermo-sensitive S-nitrosothiols, the carrier could release the nitric oxide (NO) due to the surface overheat as well as perform photothermal therapy (PTT) under near-infrared (NIR) laser irradiation. The level of collagen depletion was observed via western blotting and immunofluorescent staining. In addition, the dual-imaging and antitumor efficiency of GSNP-TPPs were evaluated with the HeLa tumor-bearing mouse model. Results: On one hand, the released NO could deplete collagen by activating matrix metalloproteinases (MMPs) to break collagen fibers, thus loosening the dense ECM to enhance the cellular internalization. On the other hand, with the mitochondrial-targeted effect of TPP, the diffusible NO in tumor might rapidly interact with superoxide anion (O 2 Ÿ - ) to produce highly toxic and powerful reactive nitrogen species (RNS) -- peroxynitrite (ONOO - ), which resulted in mitochondrial damage to induce cell apoptosis. With the unique properties of mini-sized gold nanorods, the formulated nanoparticles exhibited good computed tomography (CT) and multi-spectral optoacoustic tomography (MSOT) imaging effects in precisely locating and monitoring tumor. Moreover, the antitumor efficacy of GSNP-TPPs + laser group was further confirmed by ex-vivo histological analysis of tumor tissue. Conclusion: This work points out a strategy to overcome the obstacle standing in nanoparticles penetration, and opens the door of further exploitation of NO-related theranostic systems.
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DOI
PubMed
高影响因子
Drug Metabolism and Pharmacokinetics
·
2019
·
IF 1.874
Yang Zhang,Chen Su,Jinxiu Lei,Lu Chen,Haihong Hu,Su Zeng,Lushan Yu
Mandelic acid (MA) is generally used as a biomarker of the exposure of styrene , which is classified as a class of hazardous environmental pollutants, and also used as an important chiral intermediate in pharmaceutical industry. The previous studies have found the excretion of phenylglyoxylic acid (PGA) in human and rat, a metabolite of MA, was mainly from S- MA rather than R -MA. The metabolic mechanism, however, is not clear. In order to explore the possible metabolic mechanism, the enzyme types involved in the stereoselectivity metabolism of MA were firstly studied, and then human and rat long-chain 2-hydroxy-acid oxidase 2 (HAO2) were recombinantly expressed to study the metabolic profiles of S- MA and its analogues. The results indicated that HAO2 might catalyze the stereoselectivity metabolism of S- MA in rats. Human HAO2 ( h HAO2) and rat HAO2 ( r HAO2) isozymes β 1 and β 2 were successfully cloned and expressed with high purity and good enzyme activities. The enzyme kinetic profiles of these enzymes were different for S- MA and analogues. The order of catalytic efficiency for h HAO2 and r HAO2, however, was reverse. It might be relevance to the difference in active amino acid residues and loop 4 in human and rat L-2-hydroxy acid oxidase isozyme B crystal structures.
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DOI
PubMed
高影响因子
CEMENT AND CONCRETE RESEARCH
·
2025
·
IF 13.1
Haochuan Wang,Xin Liu,Chong Wang,Wei Wang,Jinxiang Hong,Pan Feng
Ultra-early mechanical properties are critical for shotcrete performance, significantly influenced by ettringite and calcium silicate hydrate (C-S-H) formed during the initial hydration stage and free water. This study investigates the individual and synergistic effects of these phases on mechanical behavior using equivalent cement pastes. In this system, cement was entirely replaced with dolomite particles of matching size distribution, with the controlled introduction of free water, ettringite, and C-S-H. The validity of these equivalent systems was confirmed through comprehensive characterization. Mechanical performance was subsequently evaluated using compression, shear, Vickers hardness and nanoindentation tests. Results revealed that free water remarkably weakened the mechanical properties, whereas both ettringite and C-S-H enhanced strength by reducing voids and reinforcing weak particle interfaces. Ettringite primarily contributed to interparticle friction, while C-S-H enhanced cohesion at interfaces including dolomite-dolomite, dolomite-ettringite and ettringite-ettringite contacts. When co-existing, C-S-H formed within the porous ettringite network, not only establishing a multi-scale filling structure but also stabilizing the dolomite-ettringite skeleton. These findings advance our understanding of the early-age mechanical development of shotcrete and highlight the potential of equivalent cement systems as robust tools for research into cementitious materials.
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