ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shiqiang Liu,Bin Wang,Shihang Jin,Lin Zhang,Zhizhou Yang,Yue Wu,Sheng Gao
Silicone resins, known for their exceptional properties across various industries, are traditionally nonreprocessable due to their permanent cross-linked networks. Herein, we propose a method to turn a disadvantage into an advantage by converting silanol (Si–OH) groups─adverse factors for thermal stability─into dynamic Si–O–Ph bonds, thereby endowing silicone resin with reprocessability. Polysiloxane oligomers with benzoxazine side groups (PBTS) were formed via hydrolysis–condensation reactions between monofunctional benzoxazine-containing siloxane (P-mdes) monomers and triethoxymethylsilane (MTES). The curing behaviors of PBTS are analyzed using DSC and FTIR, confirming the formation of silicone resin-based covalent adaptive networks (CANs) through the introduction of dynamic Si–O–Ph bonds. The resulting silicone resin-based CANs exhibit reprocessability and significantly improved mechanical and thermal properties. The tensile strength of the original silicone resin-based CANs reaches 23.34 MPa, and even after five cycles of reprocessing, the strength remains at 22.98 MPa, demonstrating excellent mechanical retention. The Tg and Td5 of the silicone resin-based CANs reach up to 132 °C, 424 °C, and 425 °C in nitrogen or air atmospheres, respectively. Notably, the reprocessed samples maintain excellent heat resistance and thermal stability even after five reprocessing cycles, with Tg and Td5 values around 130 and 380 °C.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Zhang Xiuxiu,Zhang Yuhao,Protsenko Bogdan O.,Soldatov Mikhail A.,Zhang Jing,Yang Chenyu,Bo Shuowen,Wang Huijuan,Chen Xin,Wang Chao,Cheng Weiren,Liu Qinghua
The development of non-iridium-based oxygen evolution reaction (OER) catalysts is crucial for proton exchange membrane water electrolysis (PEMWE), but hydrogen production remains a great challenge because of sluggish OER kinetics and severe catalyst dissolution. Here, we present a 4 f -induced covalent polarity modulation strategy for the construction of 4 f -orbital-modified RuO 2 (4 f -RuO 2 ) nanocatalysts with tunable Ru–O polarity. We find that the OER activity of 4 f -RuO 2 shows a volcano shape as a function of the polarity of Ru–O bond. Consequently, the best 4 f -Nd-RuO 2 catalyst possesses an ultra-low overpotential of 214 mV at 10 mA cm −2 and robust electrochemical stability in 0.1 M HClO 4 . Theoretical calculations coupled with in situ synchrotron infrared and X-ray absorption spectroscopy analyses reveal that the modulation of Ru–O polarity in RuO 2 by the valence f − p − d gradient orbital coupling can modify the adsorption energy of the reaction intermediates and suppress the participation of lattice oxygen to avoid over-oxidation of Ru, which can thus serve as an effective descriptor for fine tuning the activity and durability of acidic OER nanocatalysts.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Jie Huang,Xue Fan,Fei Yan,Jiyang Liu
Herein, we develop a simple electrochemical sensor based on the confinement effect of vertically ordered mesoporous silica film (VMSF) and the o-phenanthroline (Phen) chelating agent for ultrasensitive determination of ferrous ions (Fe2+). Fe(Phen)32+ obtained from the chelation between Fe2+ and Phen, shows higher electrochemical activity and larger geometric dimensions compared with free Fe2+, which could be effectively preconcentrated into the inner nanochannels of VMSF through spatial and electrostatic confinement effects. Differing from the conventional anodic stripping voltammetry, Fe(Phen)32+ could be enriched by convenient mechanical stirring and further detected by VMSF-modified indium tin oxide (VMSF/ITO), achieving an outstanding detection performance in terms of a linear range (1.0 nM–13.0 μM) and a limit of detection (LOD, 0.66 nM). Moreover, the established electrochemical sensor can accurately measure total iron and distinguish between different valence states (Fe2+ or Fe3+) with the help of reducing agents. Thanks to the outstanding antifouling ability of VMSF, the sensing platform consisting of VMSF/ITO and Phen chelating agent enables the precise determination of Fe2+ in complex real samples including tap water, pond water, FeSO4 tablets, and even colored samples, which can avoid the tedious sample pretreatment process and be applied in a wide range of scenarios.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Jin Liu,Yuyao Chen,Yue Shi,Bin Song,Jing Wang,Chong Zhang,Dan Zhang,Yuanyuan Feng
The development of hydrogen evolution reaction (HER) catalysts that combine high activity with high current density stability is an important step in promoting the scale-up preparation of green hydrogen in anion exchange membrane water electrolyzer (AEMWE). In this paper, we propose an asymmetrical “Nd−O–Ru” bridge active sites strategy in the rapid construction of rare earth metal oxides (M x O y , M = Nd, Ce) and ruthenium heterojunctions (M x O y @Ru/CNT, CNT stands for carbon nanotube) catalysts by a solvent-free microwave method. Experiments show that the catalyst exhibits excellent HER performance in alkaline media: driving 10 mA cm −2 and 1000 mA cm −2 only requires ultra-low overpotentials of 20 mV and 363 mV, and operates stably for 100 h at 1000 mA cm −2 . The combination of in situ Raman spectroscopy and theory calculations reveals that the p orbital of oxygen at the interface acts as an electronic bridge to mediate the coupling of the f orbital of Nd to the d orbital of Ru through “Nd−O–Ru” bridge enhancing the adsorption of water molecules while synergistically optimizing the free energy of hydrogen adsorption (ΔG H∗ ) and accelerating the kinetics of hydrolysis dissociation. Integrating this catalyst into the AEMWE yields current densities of 500 and 1000 mA cm −2 at voltages of 1.665 V and 1.806 V, respectively, thus offering a novel material design paradigm for industrial-scale water electrolysis. This study opens a new path for rational design of efficient energy conversion catalysts through orbital coupling engineering.
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THERMOCHIMICA ACTA
·
2025
·
IF 3.5
Yuxin Yang,Chunhua Lou,Huixiao Wang,Jingjing Yu
In this study, dicyandiamide (DCD) was modified with o-aminoacetophenone to synthesize a new curing agent for epoxy resin (EP), called o-acetylphenylguanidine (o-APG). The experimental results showed that the yield of o-APG could reach 85.79% under the optimal ratio. The structure of o-APG was characterized via Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction analysis, and nuclear magnetic resonance spectroscopy. The result deduced that the compatibility of o-APG with EP was significantly improved because reacted to form the group. The curing kinetics of the reaction of EP cured with o-APG was investigated via differential scanning calorimetry (DSC) by using the methods of Kissinger, Ozawa, Starink, and Friedman. The DSC analysis result showed that curing temperature was reduced by about 50 °C compared with the DCD-cured EP.
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
·
2024
·Vol. 149
·期 10
·4491-4503
·
IF 3
Chen Yongjia,Zhao Yilin,Hua Min,Pan Xuhai,Jiang Huichun,Jiang Juncheng
We investigated the inhibition of thermal runaway of styrene polymerization by DNPB. DNBP is an inhibitor in styrene polymerization reaction. Polymerization is one of eighteen hazardous processes. Styrene polymerization reaction is characterized by high heat production and fast reaction rate. Firstly, differential scanning calorimetry (DSC) and adiabatic calorimetry (ARC) were chosen to study the effect of different mass of DNBP on thermal behavior in non-isothermal and adiabatic environments. Secondly, exploring the inhibitory effect of DNBP at different runaway temperatures using an oil bath reactor. The results showed that when DNBP was at 0.80%, effective inhibition was obtained at different runaway temperatures. Finally, GC/MS and Gauss16 were used to infer the mechanism of inhibition in terms of macroscopic products and microscopic instabilities. The results showed that the products of the oil bath reactor experiments were related to the mass of DNBP, and when DNBP was 0.80%, the products increased and the main reaction was inhibited. Finally, it was deduced that the nitro group undergoes a possible path of direct addition reaction with the styrene radical before bond breaking.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zichen Song,Xinxin Zhang,Jianqiu Zhu,Xiaolei Wang,Wenqian Wang,Xiangbo Ma,Jiantao Fu,Jian-Qiang Wang,Guiling Wang,Zhiyu Ren,Honggang Fu
While copper complexes intrinsically provide Cu sites for electrocatalytic CO 2 reduction (ECR), their efficacy toward multicarbon products (C 2+ ) remains fundamentally limited by the operational instability of reactive Cu valence states and the inability to synchronously optimize *CO intermediate generation and C-C coupling within symmetric coordination environments. Herein, we judiciously design a single-crystal N, O co-coordinated copper complex (Cu(ICA) 2 ) featuring asymmetric N 2 -Cu-O 2 centers that precisely modulate the electronic structure and local adsorption environment. The Cu-N bonds stabilize partially reduced Cu δ⁺ sites while weakening Cu-O interactions, thus balancing structural integrity with catalytic reactivity. This asymmetric dual-site coordination concurrently hosts distinct *CO intermediates (atop-adsorbed *CO at Cu sites and bridge-adsorbed *CO at Cu-N sites), enabling cooperative C-C coupling into C 2 products. The catalyst achieves a record 69.2 % Faradaic efficiency for C 2 products at 400 mA cm −2 and 57.4 % for C 2 H 4 at 500 mA cm −2 in 1.0 M KOH, rivaling the state-of-the-art Cu-based complexes. In situ characterization and DFT calculations mechanistically corroborate that bridge-adsorbed *CO at Cu-N sites drives energetically favorable hydrogenation and C-C coupling pathways. This work establishes a coordination-asymmetry design principle for constructing robust molecular catalysts capable of efficient CO 2 -to-C 2+ conversion.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 31
·2203095
·
IF 19.924
Lin Li,Ruonan Xu,Long Zhang,Ziqi Zhang,Meng Yang,Di Liu,Xinlin Yan,Aijun Zhou
The severe parasitic interface reaction and dendrite growth retard the practical applications of all-solid-state (ASS) Na batteries with sulfide solid electrolytes (SEs). Here, a novel composite SE is proposed, with a high ionic conductivity, composed of Na 3 SbS 4 (NSS) and oxysulfide glass. The study reveals that the P 2 S 7- a O a and PS 4- a O a units in oxysulfide play various roles: The former is deoxidized to release free O ions, which reacts with the anode via migrating to form oxides, favoring an improved interface stability. The latter is highly stable upon cycling, thereby maintaining an ion transport network. Meanwhile, NSS acts as a dendrite predator via reacting with penetrated Na. These advantages enable the resulting ASS Na battery with superior long-term cycling performance at a high current density at room temperature, one of the best results so far. This discovery sheds light on innovative advanced SE materials through an oxysulfide-based composite design.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Mengyang Xu,Bingqing Chang,Jinze Li,Huiqin Wang,Pengwei Huo
The assembly of different Metal organic framework (MOFs) into hybrid heterostructures has proven to be a promising strategy that can effectively break through the limited regulatory capacity of single metal sites. Here, an S-scheme heterostructure (Fe 3 Ni-MOF) based on homologous ligands (1,4-phthalic acid) of ultra-thin Ni-MOF and Fe-MOF nanoparticles with directional electron transport channels, was developed and used it for photoreduction of CO 2 . Under the S-scheme electric field mechanism, the photogenerated carrier can achieve efficient directional separation through Fe–O–Ni atomic bond, which significantly reduces the energy barrier of the rate-determining step. Results show that the performance of Fe 3 Ni-MOF (63.5 μmol g –1 ) was 20 and 3.2 times higher than that of Ni-MOF and Fe-MOF, respectively, and exhibits excellent CO selectivity (96.4%) and stability. Transmission electron microscopy and atomic force microscopy revealed the two-molecular-layers structure of Ni-MOF and the micro-assembly structure of Fe 3 Ni-MOF, which can shorten the electron transport distance and increase the molecular mass transfer rate. X-ray photoelectron spectroscopy, electron spin resonance and electron density difference calculations reveal that interfacial electric fields and atomic bonds work together to promote directional carrier separation, resulting in the accumulation of holes on Ni-MOF and electrons on Fe-MOF. The Gibbs free energy calculation and in-situ Fourier transformed infrared spectroscopy validate that the micro-assembled S-scheme heterostructures with directional electron transport channels can significantly reduce the activation energy barrier of the reaction. This study not only proves the feasibility of constructing MOFs S-scheme heterostructures using homologous ligands, but also provides a new way to overcome the limitations of monometallic MOFs. This strategy is expected to open up a new avenue to design efficient photocatalysts.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2024
·
IF 5.7
Lichun Guo,Mengqing Zhang,Ying Fei,Wei Zhao
This study examines the inhibitory effects of a range of sweeteners on α-glucosidase. Our findings revealed that only one natural sweetener, namely, glycyrrhetinic acid 3-O-mono-beta-d-glucuronide (GAMG), derived from licorice, exhibited a mixed-type inhibition against α-glucosidase with a IC50 value of 0.73 ± 0.05 mg/mL. The fluorescence intensity of α-glucosidase was quenched by GAMG in the formation of an α-glucosidase–GAMG complex. GAMG has been shown to induce conformational changes in α-glucosidase, likely through hydrogen bonding, van der Waals force, and alkyl–alkyl interactions with amino acid residues, including Arg 281, Leu 283, Trp 376, Asp 404, Asp 443, Trp 481, Asp 518, Phe 525, Ala 555, and Asp 616. Additional animal validation experiments demonstrated that GAMG slowed starch digestion, thereby attenuating the postprandial glycemic response. Taken together, these findings provide evidence that GAMG is a natural sweetener with potent inhibitory activity that selectively targets α-glucosidase. This study supports the use of GAMG as a natural sweetener, which holds a high biological value and may be beneficial for managing postprandial hyperglycemia.
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APL Materials
·
2024
·Vol. 12
·期 4
·
IF 5.3
Lin Jia,Wang Shuai,Jin Hua,Cui Shuyuan,Wang Rongwen,Yang Yihang,Huang Guimei,Wang Jinhuo
The preparation of ceramic materials with complex porous structures through photopolymerization-based 3D printing requires the development of stable and printable slurries. In this study, zirconium acetylacetonate was incorporated into the thiol vinyl organosilicon prepolymer to create a photosensitive Si–Zr–O–C slurry. Regarding the natural bone structures and the Tyson polygon principle, a gradient pore structure was designed and then printed using a digital light processing 3D printer. After printing, the effects of sintering temperatures on the phase composition and structure of Si–Zr–O–C ceramics were systematically investigated. Subsequently, a comparative analysis of structure and properties was performed on sintered samples with different zirconium acetylacetonate contents. The results revealed that the sample containing 30 wt. % zirconium acetylacetonate exhibited a higher compressive strength of 9.70 ± 0.28 MPa and a lower room temperature thermal conductivity of 0.528 W m −1 K −1 . This study confirmed the significant potential of using 3D printing technology to prepare Si–Zr–O–C precursor ceramics with a porous structure.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Liying Huang,Di Zhang,Nitong Bu,Yuanbo Zhong,Pingping Tan,Huanglong Lin,Jie Pang,Ruojun Mu
In this work, pullulan (PUL) nanofibrous films incorporated with water-in-oil emulsions (PE) were prepared by microfluidic blowing spinning (MBS). The microstructures of nanofibers were characterized by scanning electron microscopy (SEM), fourier transform infrared (FT-IR), and X-ray diffraction (XRD). With the addition of W/O emulsions, the thermal stability, mechanical, and water barrier properties of PUL nanofibers were improved. Increases in emulsion content significantly affected the antioxidant and antimicrobial properties of nanofibrous films. ABTS and DPPH free radical scavenging rates increased from 10.26 % and 8.57 % to 60.66 % and 57.54 %, respectively. The inhibition zone of PE nanofibers against E. coli and S. aureus increased from 11.00 to 20.00 and from 15.67 to 21.17 mm, respectively. In addition, we investigated the freshness effectiveness of PE nanofibrous films on fresh-cut apples. PE nanofibrous films significantly maintained the firmness, and reduced the weight loss and browning index of the fresh-cut apple, throughout the 4 days of storage. Thus, the PE nanofibrous films exhibited good potential to prolong the shelf life of fresh-cut fruit and promote the development of active food packaging.
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