ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Linsen Li,Zhuwei Yang,Hui Xiong,Ming Ma,Riguang Zhang,Zhao Jiang
The NECZ/12H-NECZ (N-ethylcarbazole/dodecahydro-N-ethylcarbazole) system is one of the commercially promising liquid organic hydrogen carriers (LOHCs). However, the dehydrogenation reaction of 12H-NECZ is still the bottleneck of the whole hydrogen storage and release process, possessing a relatively low hydrogen release rate. In this study, one kind of C3N4 (carbon nitride) mesoporous nanosheet material with abundant N vacancies was fabricated by the thermal treatment of trace S-doped C3N4, and a series of Pd-based catalysts were prepared by the impregnation reduction method. The Pd/S0.03-C3N4-Nv550 (treated by S-doped and N) catalyst with abundant N vacancies showcases the most outstanding catalytic performance, achieving a 5.41 wt % hydrogen release amount as well as 81.09% NECZ selectivity at 90 min. Combined with the experimental and computational results, the presence of trace S does not lead to structural collapse of the material and interestingly induces the generation of high concentrations of N vacancies. The N vacancies greatly facilitate the dispersion of loaded metals, offering more active sites; meanwhile, the existence of N vacancy weakens the electronic localization of C3N4 carriers, modulates the electronic structure of active metal Pd, and promotes the activation of reactants and intermediates. What is more, the Pd/S0.03-C3N4-Nv550 catalyst shows excellent stability during long-term cycle tests. It provides some reference values for the design of LOHC dehydrogenation catalysts.
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FLUID PHASE EQUILIBRIA
·
2024
·
IF 2.8
Tao Jia,Weixue Jiang,Jia Yu
The compressed liquid densities of n -pentane(1) + n -dodecane(2) binary mixtures were measured using a high pressure vibrating-tube densimeter at temperatures from 283 K to 363 K, pressures up to 100 MPa, and five different compositions ( x 1 = 0.3778, 0.6230, 0.7968, 0.9051, and 1). The densities of binary mixtures were correlated using the modified Tait equation, and the absolute average deviations of the experimental and calculated values were 0.010 %, 0.019 %, 0.016 %, 0.025 %, and 0.017 %, respectively. In addition, the isothermal compressibility and the isobaric thermal expansivity were calculated from the obtained densities.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Ming-Yang He,Pin-Xi Wang,Jun-Qing Ye,Wen-Wen Chen,Jun-Feng Qian,Qun Chen
The development of highly active catalysts for the direct synthesis of N,N’-diphenylurea (DPU) from CO 2 and aniline is crucial yet has faced significant challenges. This study introduces a metal oxide composite catalyst, Cu x Fe 0.5 Ce 0.5 , synthesized via a one-step co-precipitation method. This catalyst features both acidic and basic active sites that synergistically catalyze the conversion of CO 2 and aniline into DPU with high efficiency. It achieved an aniline conversion rate of up to 33.0 % and an exceptional DPU selectivity of 99.9 %. Comprehensive characterizations confirmed that the catalyst possesses well-defined morphology, controlled size, optimized pore structure, and robust acid-base properties, along with abundant oxygen vacancies. Specifically, CuFe components function as Lewis base sites, effectively activating CO 2 molecules, while Ce 3+/4+ species serve as Lewis acid sites, facilitating the adsorption and activation of aniline to form key intermediates. Importantly, the presence of oxygen vacancies enhances electronic interactions between CeO 2 and metals, increasing metal electron density and providing critical active sites for CO 2 adsorption and activation, thus promoting the efficient catalytic reaction progression. Moreover, the catalyst demonstrates excellent reusability, maintaining approximately 95 % of its catalytic efficiency after five cycles. This work provides an innovative approach to developing efficient catalysts for the valorization of CO 2 into higher value-added chemicals.
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CHEMICAL PHYSICS
·
2025
·
IF 2.4
Wenchao Ma,Na Du,Wanguo Hou
Prediction of surface tension and surface composition of multicomponent liquid mixtures remains challenging. A predictive model, called the “surface aggregation adsorption” (SAA) model, was proposed recently, but its applicability needs to be examined, especially for the monophasic solutions containing immiscible components. In this work, the surface tensions of binary and ternary solutions consisting of isopropanol ( i PrOH), water, and n -decane (DA) or n -tetradecane (TDA) were determined. Based on the SAA model, the model parameters of the binary ( i PrOH–water or DA or TDA) solutions were first estimated, and then used to predict the surface tension and composition of the ternary ( i PrOH–water–DA or TDA) solutions. The predicted surface tension values for the ternary solutions are well consistent with their experimental ones. Importantly, the so-obtained information on surface compositions can provide a better understanding of the surface adsorption behavior.
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LANGMUIR
·
2025
·
IF 3.9
Ke-Xin Zhang,Ye Hong,Lu Wang,Ting Chen,Dong Wang
Halogen bonding interactions are crucial in the design of 2D supramolecular assemblies. In this study, we introduce the N-oxide moiety as a halogen-bonding acceptor for the formation of 2D coassemblies. The monomers 4,4’-bipyridine N,N’-dioxide (BPYD) and 1,3,5-trifluoro-2,4,6-triiodobenzene (1,3,5-TFTIB) coassemble into well-ordered, close-packed nanoarchitectures on HOPG surfaces. BPYD forms both halogen and hydrogen bonds with 1,3,5-TFTIB, resulting in pentameric structural units. At high concentrations, these units pack into dense ordered structures. When octanoic or nonanoic acid is used as a solvent, the formation of a 3-component linear structure with the interdigitated solvent molecules between the linear-arranged pentameric units is observed at low concentrations of reactants.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2015
·
IF 4.152
Wei Wei,Xiaoliang Qi,Yucheng Liu,Junjian Li,Xinyu Hu,Gancheng Zuo,Jianfa Zhang,Wei Dong
Salecan is a water-soluble microbial polysaccharide produced by Agrobacterium sp. ZX09, a salt-tolerant strain isolated from a soil sample in our laboratory. Previous work inspired us salecan is a good candidate to fabricate hydrogels. Poly( N , N -diethylacrylamide) is one type of thermo sensitive polymer which is not investigated extremely as poly( N -isopropylacrylamide). Here, we report a novel pH-thermo dual responsive hydrogel based on salecan and poly( N , N -diethylacrylamide-co-methacrylic acid) semi-interpenetrating polymer networks (semi-IPNs). The physicochemical property of this hydrogel was investigated by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and thermogravimetric analyses (TGA), rheological test and Scanning Electron Microscopy (SEM). It was interesting that the storage modulus (G′) and pore size of the hydrogel could be tuned by adjusting the content of salecan and crosslinker. The pH-thermo dual responsive property was demonstrated by swelling behavior test: the swelling ratio of the hydrogel decreased continuously as the temperature increased from 25 °C to 37 °C, while it was pH-dependent as well. Especially, when exposed to a higher temperature (37 °C) and acidic environment (pH 4.0), drug-loaded hydrogel would have a quick release. Finally, the cytotoxicity of drug-free hydrogels was investigated on A549 and HepG2 cells, results showed that it was non-toxic while the DOX released from hydrogels had comparable cytotoxicity with respect to free DOX. In conclusion, the novel salecan/poly( N , N -diethylacrylamide-co-methacrylic acid) semi-interpenetrating polymer network hydrogels were pH-thermo dual responsive and may be a promising candidate for drug delivery system.
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Advanced Science
·
2024
·
IF 14.3
Wei Shi,Hui Li,Jing Chen,Yern Chee Ching,Cheng Hock Chuah,Chengsheng Xu,Moran Liu,Jinyong Zhang,Kuan Yong Ching,Yongsheng Liang,Guanglin Li,Wei Tang
Hydrogels present attractive opportunities as flexible sensors due to their soft nature and tunable physicochemical properties. Despite significant advances, practical application of hydrogel-based sensor is limited by the lack of general routes to fabricate materials with combination of mechanical, conductive, and biological properties. Here, a multi-functional hydrogel sensor is reported by in situ polymerizing of acrylamide (AM) with N,N′-bis(acryloyl)cystamine (BA) dynamic crosslinked silver-modified polydopamine (PDA) nanoparticles, namely PAM/BA-Ag@PDA. Compared with traditional polyacrylamide (PAM) hydrogel, the BA-Ag@PDA nanoparticles provide both high-functionality crosslinks and multiple interactions within PAM networks, thereby endowing the optimized PAM/BA-Ag@PDA hydrogel with significantly enhanced tensile/compressive strength (349.80 kPa at 383.57% tensile strain, 263.08 kPa at 90% compressive strain), lower hysteresis (5.2%), improved conductivity (2.51 S m −1 ) and excellent near-infrared (NIR) light-triggered self-healing ability. As a strain sensor, the PAM/BA-Ag@PDA hydrogel shows a good sensitivity (gauge factor of 1.86), rapid response time (138 ms), and high stability. Owing to abundant reactive groups in PDA, the PAM/BA-Ag@PDA hydrogel exhibits inherent tissue adhesiveness and antioxidant, along with a synergistic antibacterial effect by PDA and Ag. Toward practical applications, the PAM/BA-Ag@PDA hydrogel can conformally adhere to skin and monitor subtle activities and large-scale movements with excellent reliability, demonstrating its promising applications as wearable sensors for healthcare.
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ChemPlusChem
·
2020
·Vol. 85
·期 3
·503-509
·
IF 2.753
Meng-Yao Chao,Jing Chen,Xiao-Yu Wu,Rui-Yao Wang,Pei-Pei Wang,Lifeng Ding,David J. Young,Wen-Hua Zhang
Graphical Flexible friend : A metal–organic framework sustained by a Cd 5 cluster shows flexible behavior and coordination preference toward electron-deficient rather than electron-rich pyridyl ligands. Density functional theory calculations offer binding energies of the electron-deficient 4-pyridinealdehyde (1.09 eV) and 4-acetylpyridine (1.36 eV) to the flanking Cd centers, and are larger than those of the electron-rich ligands, such as 4-iodopyridine (0.32 eV) and 4,4′-bipyridine (0.61 eV). A cationic three-dimensional (3D) metal-organic framework (MOF) sustained by an N , N ′-diethylformamide (DEF)-solvated zigzag-shaped Cd 5 cluster secondary building unit (SBU), [Et 2 NH 2 ] 2 [Cd 5 (BTB) 4 (DEF) 2 ] ⋅ 4.75DEF ( 1 a , H 3 BTB=benzene-1,3,5-tribenzoic acid) shows flexible framework behavior and undergoes solvate exchange with CHCl 3 to yield [Et 2 NH 2 ] 2 [Cd 5 (BTB) 4 (DEF) 2 ] ⋅ x CHCl 3 ( 1 b ) accompanied by changes to pore sizes and shapes. Unexpectedly, the DEF solvates coordinated to the central Cd 2+ could not be replaced by strongly donor pyridyl and dipyridyl ligands. Additionally, more electron-deficient pyridyls preferentially coordinated to the flanking Cd 2+ of the Cd 5 SBU, as exemplified by [Et 2 NH 2 ] 2 [Cd 5 (BTB) 4 (DEF) 2 (PyCHO) 2 ] ⋅ x Sol ( 2 a , PyCHO=4-pyridinealdehyde) and [Et 2 NH 2 ] 2 [Cd 5 (BTB) 4 (DEF) 2 (PyAc) 2 ] ⋅ x Sol ( 2 b , PyAc=4-acetylpyridine). Density functional theory (DFT) calculations were used to understand these counterintuitive observations.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Xiao Ma,Xue Zhao,Jianshe Huang,Litai Sun,Qun Li,Xiurong Yang
Herein, we develop a novel method to synthesize evenly dispersed fine Co nanoparticles (CoNPs) (particle size of ∼42 nm) encapsulated in a N-doped porous carbon matrix (NPCM) with superficial N-doped porous carbon nanofibers (NPCNF) (denoted as Co@NPCM/CNF-850) as an oxygen reduction reaction (ORR) electrocatalyst. Such an electrocatalyst is the direct pyrolysis product of the novel pine needle-like ZIF-67-based metal-organic framework nanowire array (MOFNWA) prepared using an inorganic cobalt carbonate hydroxide (Co(CO3)0.5(OH)·0.11H2O) nanowire array as a linear sacrificial template, which is totally different from the traditional method, that is, using inorganic salts to synthesize MOF particles. Because of the high dispersibility of the effective fine N-doped carbon-wrapped CoNPs (rather than the overlarge CoNP aggregates); the unique linear MOF-derived assemblies, which are beneficial to electronic transmission; the high degree of graphitization, which is attributed to the superficial NPCNF and carbon layers wrapping the CoNPs; as well as the high porosity, our catalyst showed remarkable ORR activity (Eonset of 1.033 V vs the reversible hydrogen electrode) in alkaline solution. Besides, our catalyst revealed excellent stability and tolerance of methanol. Furthermore, on the basis of the X-ray absorption near-edge structure, extended X-ray absorption fine structure, and linear sweep voltammetry data, we first provided proof that a catalyst devoid of obvious Co–Nx can have superior ORR activity.
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JOURNAL OF CHROMATOGRAPHY A
·
2019
·
IF 3.858
Shuaihua Wang,Xianxiu Li,Yan Sun
Ion exchangers of high binding capacity and uptake rate are desired for high performance purification of proteins by ion exchange chromatography. For this purpose, we have herein developed a new anion exchanger by grafting N,N - Dimethylaminopropyl acrylamide (DMAPAA) onto Sepharose FF by atom transfer radical polymerization. Six DMAPAA-grafted Sepharose FF resins of the same grafting density but different chain lengths (ionic capacities, ICs) were prepared, and named as FF-pDMAPAA n ( n denotes IC value, 65–831 mmol/L). Bovine serum albumin (BSA) adsorption and its chromatography were studied to evaluate the anion exchange resins. It was found that the equilibrium protein adsorption capacity ( q m ) increased rapidly from 91 mg/mL at IC = 65 mmol/L till reaching a peak value (368 mg/mL) at IC = 458 mmol/L and then decreased slightly with further increasing IC (chain length) to 831 mmol/L. The uptake rate, D e / D 0 , defined as the ratio of effective diffusion coefficient ( D e ) to free diffusivity of the protein ( D 0 ), also presented similar changes as a function of IC. Namely, D e / D 0 increased from 0.25 to 2.45 in the IC range of 65 to 458 mmol/L, kept almost unchanged from 458 to 573 mmol/L and then decreased slightly with further increase of IC to 831 mmol/L. Therefore, FF-pDMAPAA458 presented the best performance of the six resins for BSA adsorption, possessing very high q m and D e / D 0 values (368 mg/mL and 2.45, respectively). The resin was thus extensively characterized in the effect of ionic strength and column chromatography. The q m and D e / D 0 of FF-pDMAPAA458 were much higher than other anion exchangers reported in literatures and kept over 230 mg/mL and 2.3, respectively, at salt concentrations up to 100 mmol/L. Therefore, the dynamic binding capacity of the FF-pDMAPAA458 column was remarkably higher than Q Sepharose FF and other two typical polymer-grafted anion exchangers reported in literatures in the salt concentration range, and kept as high as 180–220 mg/mL in the superficial flow velocity rang of 150–1350 cm/h. Taken together, the results demonstrated that FF-pDMAPAA resins of appropriate ionic capacities are promising for high-performance protein chromatography.
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Materials Science & Engineering C-Materials for Biological Applications
·
2020
·
IF 5.88
Zhimei Wei,Qingyu Lin,Jie Yang,Shengru Long,Gang Zhang,Xiaojun Wang
Dual temperature- and pH-sensitive materials used as drug carriers have attracted a particularly high level of interest. However, it is limited by low sensitivity to changes in conditions because of large size and low specific surface area. In this work, novel dual temperature- and pH-sensitive poly( N -isopropylacrylamide- N -methylolacrylamide acrylic acid) (PNIPAm-NMA-AAc) ultrafine fibres were successfully prepared by radical copolymerisation, electrospinning and thermal chemical treatment. The PNIPAm-NMA-AAc ultrafine fibres were characterized by Fourier transform infrared (FTIR), proton nuclear magnetic resonance ( 1 H NMR), spectroscopy UV–visible spectroscopy, scanning electron microscopy (SEM) and cell counting kit-8 (CCK-8) assay. The uniformity and small size of PNIPAm-NMA-AAc ultrafine fibres with LCST range from 31 °C to 43 °C were used to drug carrier because of good thermal stability, no cytotoxic. Curcumin as a model drug was well distributed in PNIPAm-NMA-AAc ultrafine fibres. In addition, analysis of curcumin release at different pH values and temperatures confirmed that the PNIPAm-NMA-AAc ultrafine fibres are responsive to both temperature and pH. The maximum amount of curcumin released was 98.47% ± 1.87%. In addition, the release mechanism of curcumin-based PNIPAm-NMA-AAc ultrafine fibres was shown to conform to Fickian diffusion (r 2 ≥ 0.95). These results indicated that dual-responsive PNIPAm-NMA-AAc ultrafine fibres are promising as drug carriers.
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2016
·Vol. 16
·期 9
·9708-9715
·
IF 1.338
Guo Ruiwei,Zhong Qing,Dong Anjie,Zhang Jianhua
The success of self-template methods for fabrication of hollow silica microspheres largely depends on the stabilization of the outmost silica layer by a polymer ligand. In this study, the cationic polyelectrolyte poly(N, N-dimethylaminoethyl methacrylate) (PDMAEMA), combining
the synergistic electrostatic attractions and hydrogen bonding interactions, was found to be able to form a robust protective layer on the surface of silica spheres. The structural characteristics of obtained PDMAEMA-coated silica microspheres were detailedly characterized by Scanning Electron
Microscopy (SEM), Energy Dispersive X-ray (EDX), Dynamic Light Scattering (DLS), Fourier Transform Infrared (FTIR) and Transmission Electron Microscopy (TEM). The etching process was monitored by TEM and the shell features of prepared hollow silica nanocapsules were characterized by nitrogen
adsorption–desorption isotherm technique. The results show that the PDMAEMA protective layer not only can effectively stabilize the outmost silica layer against etching, but also actively capture the negative silicate oligomers for shell-growth, allowing more effective transformation
of silica spheres into yolkshell or hollow nanoparticles with pronounced hollow nature and well-defined mesoporous shell structure.
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