Biomaterials Science
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2024
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IF 5.8
Hang Ren,Peng Wang,Hanwen Huang,Junshen Huang,Yuheng Lu,Yanfeng Wu,Zhongyu Xie,Youchen Tang,Zhaopeng Cai,Huiyong Shen
Titanium (Ti) and its alloys have been widely employed in the treatment of orthopedics and other hard tissue diseases. However, Ti-based implants are bioinert and suffer from bacterial infections and poor osseointegration in clinical applications. Herein, we successfully modified Ti with a porous N-halaminated spermidine-containing polymeric coating (Ti-SPD-Cl) through alkali-heat treatment, surface grafting and chlorination, and it has both excellent antibacterial and osteogenic abilities to significantly enhance osseointegration. The as-obtained Ti-SPD-Cl contains abundant N–Cl groups and demonstrates effective antibacterial ability against S. aureus and E. coli. Meanwhile, due to the presence of the spermidine component and construction of a porous hydrophilic surface, Ti-SPD-Cl is also beneficial for maintaining cell membrane homeostasis and promoting cell adhesion, exhibiting good biocompatibility and osteogenic ability. The rat osteomyelitis model demonstrates that Ti-SPD-Cl can effectively suppress bacterial infection and enhance bone–implant integration. Thus, Ti-SPD-Cl shows promising clinical applicability in the prevention of orthopedic implant infections and poor osseointegration.
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Journal of Materials Chemistry C
·
2024
·Vol. 12
·期 16
·5737-5747
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IF 5.7
Naying Shan,Zihao Guan,Zhiyuan Wei,Lulu Fu,Yang Zhao,Fang Liu,Lu Chen,Yanyan Xue,Zhipeng Huang,Mark G. Humphrey,Jun Xu,Chi Zhang
A stepwise approach was implemented in this research to synthesize the covalent linkage between graphene oxide (GO) and MXene for the first time. The preparatory procedure involves the exchange of surface functional groups on MXene, followed by the covalent modification of N-terminalized MXene with GO, making a pioneering advancement in the domain of nonlinear optics. The resulting nanohybrids, labeled as f-MXene-GO, underwent fully comprehensive characterization by crystallographic, spectroscopic, and microscopic techniques. Z-scan measurements revealed that f-MXene-GO features an optimized nonlinear optical (NLO) response in both nanosecond (ns) regimes at 532 nm and femtosecond (fs) regimes at 800 nm across the visible and near-infrared spectra, surpassing its precursor and physically blended samples. The transmittance of f-MXene-GO gradually diminishes with increasing incident energy, displaying enhanced reverse saturable absorption (RSA) and optical limiting effects upon ns pulse excitation. Conversely, f-MXene-GO demonstrates promoted saturable absorption (SA) under fs laser illumination. The effective electron transfer process from MXene to the grafted GO, validated by theoretical calculations, stimulates superior NLO absorption. These findings not only elucidate the intricate relationship between the structure and the NLO response across wide spectral regions and time scales but also provide invaluable insights into the untapped potential of MXene-based materials for NLO applications.
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Journal of Physical Chemistry C
·
2024
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IF 3.3
Mingjun Xu,Zhao Jin,Meiling Xiao,Changpeng Liu,Wei Xing
Pyrolyzed iron and nitrogen codoped carbon materials (Fe–N–C) with atomically dispersed Fe-Nx sites have received extensive attention as a highly promising alternative to Pt for oxygen reduction reaction (ORR), yet there remains a considerable performance gap between them. To further improve the catalytic performance of Fe–N–C catalysts, we herein developed a microwave-assisted method to improve both the active site density (SD) and intrinsic activity, thus achieving outstanding ORR activity. The in situ generated Fe precipitation is beneficial to improve the doping efficiency of Fe and the subsequent formation of synergetic active sites, leading to increased SD. Both the X-ray absorption spectroscopy and operando Raman confirmed the copresence of atomic Fe moieties and nanoclusters, in which the nanoclusters synergically promote the activity of the single atomic sites. The enriched synergetic active sites endow the as-prepared catalyst with excellent performance by showing a current density of 42 mA cm–2 at 0.9 V in a proton exchange membrane fuel cell, approaching the DOE 2025 target. This work not only affords a highly active ORR catalyst but also provides a simple and potentially scale-up approach to Fe–N–C catalysts.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2024
·
IF 2.2
Peng Wang,Jun-Fei Gu,Zhan Chen,Hao-Yue Ma,Xing-Chuan Li,Shuai Li,Xiang-Ya Xu,Ye Yuan,Cheng Chen,Zongkui Kou
Graphical This study develops a solid-state thermal (SST) synthesis method for the one-step preparation of MOF-derived Mn x @NC catalysts. Among these, the optimal catalyst (Mn 2.5 @NC) exhibits excellent activity, remarkable stability, and good recyclability for HMF oxidation to FDCA, achieving an FDCA yield of 94 % within 4 h at room temperature and maintaining its catalytic performance for five cycles without activity decay. Transforming the bio-based 5-hydroxymethylfurfural (HMF) into its oxidation product 2,5-furandicarboxylic acid (FDCA) offers an attractive route for synthesizing bioplastic monomers. However, significant challenges remain in developing efficient and stable non-precious metal catalysts. Here, we employed a solid-state thermal synthesis (SST) method to design and synthesize a series of metal-organic framework (MOF)-derived metal-nitrogen-carbon (M@NC) materials with gradient metal contents and low metal loadings, labeled as Mn x @NC, for converting HMF into FDCA through oxidation. Further investigations revealed that the amount of metal doping significantly influenced the catalyst structure, particularly in terms of defect quantity and specific surface area. The optimal catalyst, Mn 2.5 @NC, exhibited the largest specific surface area and the highest number of defects, achieving a 94 % FDCA yield within 4 h. Experimental results demonstrated that the recovered catalyst could be reintroduced into the reaction system and maintained selectivity comparable to that of the fresh catalyst for at least five cycles. Moreover, various characterizations of both fresh and recovered catalysts confirmed the great stability of Mn 2.5 @NC. This study provides advanced insights into the effective catalytic conversion of HMF to FDCA and highlights the importance of structural design and regulation in optimizing M@NC catalysts.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Zhuocheng Wei,Bin Zhang,Rui Xu,Haoling Li,Acong Chen,Chaohai Wei,Haizhen Wu
Thiocyanate (SCN − ) is a highly toxic reducing inorganic compound commonly found in various nitrogen-rich wastewater and is also a promising electron donor for mixotrophic denitrification. However, its extent of involvement in mixotrophic denitrification under conditions of carbon limitation or excess remains unclear. In this study, five reactors were constructed to investigate the participation and microbial mechanisms of SCN − in mixotrophic denitrification under high C/N and low C/N conditions. The results showed that under low C/N conditions, SCN⁻ synergizes with organic electron donors to enhance denitrification, with mixotrophic systems exhibiting higher electron utilization efficiency and achieving 1.12 times the TN removal rate of autotrophic and heterotrophic systems combined. Under high C/N conditions, an ample supply of electron donors achieve 100% nitrate removal; however, SCN⁻ also participates in denitrification, competing with organic electron donors for NO 3 − -N, which leads to the waste of organic matter. Additionally, high-throughput sequencing revealed that under low C/N mixotrophic conditions, SCN⁻ effectively promoted the growth of SCN⁻-degrading microorganisms such as Thiobacillus , with its abundance increasing from 0% to 8.86%, approximately 1.85 times higher than under autotrophic conditions. This enhancement strengthened the sulfur and nitrogen metabolic capabilities of the microbial community, enabling the system to utilize SCN − more fully for denitrification. This study provides novel insights for reducing the addition of external organic matter to nitrogen-rich wastewater containing SCN − , offering theoretical and technical support for energy-saving and emission reduction in denitrification processes of actual industrial wastewater treatment.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
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IF 8.1
Danyang He,Liyun Cao,Jianfeng Huang,Xiaoyong Zhang,Changcong Wang,Kaikai Zhao,Koji Kajiyoshi,Liangliang Feng
Developing highly active and stably non-precious metal electrocatalysts for hydrogen production in alkaline conditions is of paramount importance to hydrogen economy. Herein, nanosheet-assembled hollow nitrogen-doped carbon nanospheres confined with ultrasmall NiSe nanoparticles (NiSe@NC) are synthesized by employing a SiO 2 template-assisted approach. As expected, the as-prepared NiSe@NC electrocatalyst delivers an overpotential of 169 mV at the current density of 10 mA/cm 2 without iR -correction, and sustains at least 80 h for continuous operation, far outperforming the NiSe-p catalyst in 1 M KOH medium toward hydrogen evolution reaction (HER). The appealing HER performance is mainly ascribed to the synergy effect between hollow nitrogen-doped carbon and highly active NiSe nanoparticles, which improves catalytically active sites, expedites electron transfer rate and optimizes the electronic structure of NiSe@NC nanomaterial. More strikingly, this study presents the feasible insights for constructing robust cost-effective electrocatalysts towards efficient HER in harsh alkaline media.
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DALTON TRANSACTIONS
·
2017
·Vol. 47
·期 1
·180-189
·
IF 4.029
Dandan Yang,Jie Dong,Baiquan Wang
A series of new pincer-type tridentate o-aryloxide-N-heterocyclic carbene nickel complexes Ni1–Ni3 were synthesized, and the molecular structure of Ni3 was confirmed by X-ray crystallography. In comparison with the above tridentate complexes, the bidentate bis(aryloxide-NHC) nickel complex Ni4 was also synthesized. On activation with either Et2AlCl or Me2AlCl, all nickel complexes showed low activity toward norbornene (NB) homopolymerization. Surprisingly, Ni1–Ni3 catalysts exhibited moderate to high activity toward the homopolymerization (up to 3.21 × 106 g PNB (mol of Ni)−1 h−1) and copolymerization of norbornene with 1-octene (up to 1.39 × 105 g polymer (mol of Ni)−1 h−1) with B(C6F5)3 as the cocatalyst even at 100 °C, showing that tridentate nickel catalysts have high thermal stability. Notably, the tridentate Ni1–Ni3 complexes showed better activities than the corresponding bidentate bis(aryloxide-NHC) nickel complex Ni4. The obtained poly(NB-co-1-octene)s were confirmed to be vinyl-addition copolymers, which exhibited high 1-octene insertion ratio (9%–17%), good thermal stability (Td > 400 °C), high molecular weight (up to 105), and narrow molecular weight distribution (PDI ≤ 1.91).
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ISRAEL JOURNAL OF CHEMISTRY
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2018
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IF 2.607
Ying Fan,Rui-Han Gao,Xin Xiao,Zhu Tao
Graphical Host-guest inclusion complexes of hymexazol with three different cucurbit[ n ]uril, cucurbit[7]uril (Q[7]), hemimethyl-substituted cucurbit[6]uril (HHMeQ[6]), and twisted cucurbit[14]uril ( t Q[14]) have been investigated by means of 1 H NMR spectroscopy, quadrupole-time of flight mass spectrometry (Q-TOF), and isothermal titration calorimetry (ITC). 1 H NMR experimental results revealed that hymexazol resides within the respective cavities of the selected Q[ n ], and mass spectrometric experimental results revealed that it interacts with these three Q[ n ] through the formation of 1 : 1 inclusion complexes. ITC experimental results indicated moderate binding constants. In vitro assays showed that the complexation of hymexazol by the Q[ n ] increased its inhibitory effect on the mycelia growth of Botrytis cinerea Pers .
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Soft Matter
·
2018
·Vol. 14
·期 10
·1789-1798
·
IF 3.709
Yaping Zhang,Jingwen Ji,Haiping Li,Na Du,Shue Song,Wanguo Hou
Nanocomposite (NC) hydrogels of positively charged layered double hydroxide (LDH) single-layer nanosheet (SLNS) cross-linked poly(N-isopropylacrylamide) (PNIPAM) were synthesized. Especially, the LDH SLNSs used here were pre-synthesized via an aqueous synthetic route without using organic solvents and modifiers. The obtained LDH/PNIPAM NC hydrogels were characterized using XRD, SEM, TEM, and DSC. The mechanical and thermoresponsive properties were determined using tensile, compression, and swelling/deswelling tests. Interestingly, different network structures are observed for the NC hydrogels along the horizontal and vertical directions; those along the horizontal direction exhibit a fine and uniform sponge-like network structure while those along the vertical direction exhibit a hierarchical layered architecture. Compared with the conventional N,N′-methylene bisacrylamide cross-linked PNIPAM hydrogel, the NC hydrogels exhibit extraordinary deformability and stretchability and obviously improved thermoresponsive swelling/deswelling characteristics. Furthermore, the fracture elongation observed here is obviously higher than those reported for negatively charged clay/PNIPAM NC hydrogels. With the increase in the LDH content from 0.8 to 2.0 wt%, the fracture strength and the compressive strength at an 85% strain increase from 23.5 to 37.2 kPa and from 0.15 to 0.57 MPa, respectively, while the fracture elongation decreases from 2689 to 2202%. The mechanism for the improved mechanical performances of the NC hydrogels is discussed. To the best of our knowledge, this is the first report on LDH/PNIPAM hydrogels. This work provides a green synthesis route for LDH-containing NC hydrogels. The new NC hydrogels may have great potential applications such as in tissue engineering, drug vehicles, and sorbents.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Jiao Li,Yalan Liu,Xiaoqian Zhu,Gang Chang,Hanping He,Xiuhua Zhang,Shengfu Wang
Electrochemical sensors now play an important role in analysis and detection of nucleic acids. In this work, we present a novel double-signal technique for electrochemically measuring the sequence and length of the d(CAG)n repeat. The double-signal technique used an electrochemical molecular beacon (a hairpin DNA labeled with ferrocene), which was directly modified on the surface of a gold electrode, while a reporter probe (a DNA sequence labeled with horseradish peroxidase) was hybridized to the target DNA. First a simple single-signal sensor was characterized in which d(CAG)n repeats were detected using a short reporter DNA strand labeled with horseradish peroxidase. To obtain a reliable signal that was dependent on repeat number, a double-signal biosensor was created in which the single strand capture DNA in single-signal sensor was replaced by an electrochemical molecular beacon labeled with ferrocene. When the hairpin DNA hybridized to the target–reporter DNA complex, it opened, resulting in a decreased ferrocene current. Both electrochemical biosensors exhibited high selectivity and sensitivity with low detection limits of 0.21 and 0.15 pM, respectively, for the detection of d(CAG)n repeats. The double-signal sensor was more accurate for the determination of repeat length, which was measured from the ratio of signals for HRP and ferrocene (H/F). A linear relationship was found between H/F and the number of repeats (n), H/F = 0.1398n + 9.89788, with a correlation coefficient of 0.974. Only 10 nM of target DNA was required for measurements based on the value of H/F in the double-signal technique. These results indicated that this new double-signal electrochemical sensor provided a reliable method for the analysis of CAG trinucleotide repeats.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Yan-Yun Meng,Qing-Da An,Zuo-Yi Xiao,Shang-Ru Zhai,Zhan Shi
Through hydrothermal synthesis and impregnation-reduction processes, a series of Pd-based nanocomposites using N-doped carbon layers coated ZrSBA-15 as the supports have been manufactured, aiming to upgrade the catalytic activity and stability of the catalysts. Pentaethylenehexamine (PEHA) was served as a nitrogen source to generate N-doped carbon (CN) layers that were pre-deposited into the acidic platelet framework ZrSBA-15, and then followed by introducing Pd 0 nanoparticles (NPs) onto it, finally leading to the formation of target composite Pd/CN-ZrSBA-15. The samples were characterized by XRD , TEM, SEM, N 2 adsorption-desorption isotherm, FTIR, XPS etc. The catalytic performance of as-prepared catalysts was evaluated by the aerobic oxidation of benzyl alcohol and the reduction of 4-NP, respectively. Duo to the platelet-like morphology with shortened channels and the modification of N-doped carbon layers, which could effectively decrease pore blocking in the process of preparation and reactions as well as enhance the metal-support interaction, the derived catalysts could afford 85% conversion of benzyl alcohol and 100% selectivity of benzaldehyde, and the conversion of 4-NP was also up to 96%. More remarkably, the catalysts could be reused at least ten times without significantly loss in catalytic activity.
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Polymers
·
2018
·Vol. 10
·期 3
·293
·
IF 2.935
Jiaxing Li,Lei Yang,Xiaoguang Fan,Fei Wang,Jing Zhang,Zhanyong Wang
Continuing efforts to develop novel smart materials are anticipated to upgrade the quality of life of humans. Thermo-responsive poly(N-isopropylacrylamide) and glucose-responsive phenylboronic acid—typical representatives—are often integrated as multi-stimuli-sensitive materials, but few are available for side-by-side comparisons with their properties. In this study, both copolymers bearingN-isopropylacrylamide (NIPAAm), with or without 3-acrylamidophenylboronic acid (AAPBA), were synthesized by free radical polymerization, and characterized by Fourier transform infrared spectrometry, nuclear magnetic resonance hydrogen spectroscopy and gel permeation chromatography. Dynamic light scattering was used to analyze and compare the responsive behaviors of the copolymers in different aqueous solutions. Atomic force microscopy was also employed to investigate the apparent morphology changes with particle sizes. The results demonstrated that the introduction of NIPAAm endowed the composite materials with thermosensitivity, whereas the addition of AAPBA lowered the molecular weight of the copolymers, intensified the intermolecular aggregation of the nanoparticles, reduced the lower critical solution temperature (LCST) of the composites, and accordingly allowed the copolymers to respond to glucose. It was also concluded that the responding of smart copolymers to operating parameters can be activated only under special conditions, and copolymer dimension and conformation were affected by inter/intramolecular interactions.Keywords:poly(N-isopropylacrylamide);phenylboronic acid;smart responsive behavior;hydrodynamic diameter;dynamic light scattering
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