INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Zongwei Hao,Ailong Hu,Juntao Cheng,Zhenni Ma,Zhaofeng Li,Jiali Lv,Huajian Xu,Huifang Ge,Hongyan Wang,Zhenyu Yu,Zhongwen Xie,Yiqun Du
The digestibility of starch-based foods is receiving increased attention. To date, the full understanding of how including L-theanine (THE) can modify the structural and digestive properties of starch has not been fully achieved. Here, we investigated the multi-scale structure and digestibility of maize starch (MS) regulated by THE in ultrasound field and the molecular interactions . Ultrasound disrupted the structure of starch granules and opened the molecular chains of starch, promoting increased THE binding and producing more low-order or disordered crystal structures. In this case, the aggregation of starch molecules, especially amylose , was reduced, leading to increased mobility of the systems. As a result, the apparent viscosity, G', and G" were significantly decreased, which retarded the starch regeneration. Density functional theory calculations indicated that there were mainly non-covalent interactions between THE and MS, such as hydrogen bonding and van der Waals forces. These interactions were the main factors contributing to the decrease in the short-range ordering, the helical structure, and the enthalpy change (ΔH) of MS. Interestingly, the rapidly digestible starch (RDS) content of THE modified MS (MS-THE-30) decreased by 17.89 %, while the resistant starch increased to 26.65 %. These results provide new strategies for the safe production of resistant starch.
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DOI
PubMed
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2025
·
IF 4.6
Ahsan Nazir,Ameena Tur Rasool,Chuntao Chen,Bianjing Sun,Dongping Sun
In this study, a NiO-PbBiO 2 Br photocatalyst was developed by a simple chemical precipitation approach followed by a hydrothermal process to eliminate tetracycline (TC). The resultant materials were assessed utilizing diverse characterization techniques. Compared with pure PbBiO 2 Br (49.5 %) and NiO (56.8 %), the NiO-PbBiO 2 Br composite exhibited superior photocatalytic effectiveness for removing TC under visible light and achieved a remarkable 98.4 % elimination of TC within 70 min (conditions: [TC] = 10 mg/L, pH 7 and [catalyst] = 1 g/L). The reaction rate constant (K) values are in the following order: NiO-PbBiO 2 Br (0.0591 min −1 ) > NiO (0.0119 min −1 ) > PbBiO 2 Br (0.0097 min −1 ). The markedly improved photocatalytic efficiency of NiO-PbBiO 2 Br can be ascribed to the expanded light absorption and the establishment of p-n heterojunction amid NiO and PbBiO 2 Br. The effects of several important factors, e.g. TC concentration, pH, catalyst dosage, and different water sources, were thoroughly investigated. Cycle tests were performed to confirm the stability and reusability of NiO-PbBiO 2 Br. Furthermore, electron spin resonance (ESR) and radical scavenging studies verified that the species •O 2 − , h + , and •OH play a key role in removing TC. The susceptible active regions of TC and the probable TC degradation routes were examined through density functional theory (DFT) calculations and high-performance liquid chromatography (HPLC) analyses. Thus, this work presents a new methodology for creating a photocatalyst with enhanced photocatalytic effectiveness for removing organic pollutants in water.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Cong Wan,Jianwen Zhang,Honglei Zhang,Min Liu,Yiming Li,Zijun Yan,Chengheng Pang,Tao Wu
The catalytic reduction of CO₂ into valuable chemicals and fuels is a promising strategy for mitigating global carbon emissions. This study explores the synergistic co-reduction of CO₂ and H₂O using nanoscale zero-valent iron (NZVI) as a dual-function catalyst. Under light irradiation at 300 °C, the CO₂ reduction rate increased by more than 10-fold compared to dark conditions, demonstrating significant photothermal synergy. The study reveals that NZVI undergoes a phase transformation, where Fe₃O₄ functions as a photocatalyst while Fe 0 serves as an electron donor, enabling a unique dual-functionality that facilitates efficient electron transfer. The addition of 10 vol% H₂ stabilizes the reaction, leading to a higher and more consistent CO yield. When investigating the simultaneous reduction of CO₂ and H₂O, we discovered competitive adsorption and reaction pathways that significantly influence product distribution. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations revealed three distinct mechanistic pathways for CO₂ conversion: direct C O bond cleavage, a carboxylate-mediated pathway and bicarbonate-mediated pathway, with the carboxylate and bicarbonate pathways being uniquely promoted by H and OH from H₂O dissociation. The addition of H₂O into the CO₂ and H₂ reaction significantly enhanced CH₄ generation due to the extra H source from H₂O dissociation. These findings offer valuable insights into the competitive mechanistic pathways of CO₂-H₂O co-reduction and contribute to the design of more efficient iron-based catalysts for sustainable CO₂ conversion and water splitting in energy and environmental applications.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Si Duan,Yuanhua Lin,Guihong Lan,Yudi Jing,Mohd Talha
Antibiotic pollution and resistance spread pose urgent environmental risks, compounded by coexisting multiple antibiotics. To address this, this study aims to enhance the adsorption of typical antibiotics (tetracycline, TC; ciprofloxacin, CIP) through structural and functional modulation of metal-organic frameworks (MOFs). Focusing on MIL-101(Fe), a series of NH 2 -MIL-101(Fe) materials with tunable amination degrees were prepared via a mixed-ligand strategy, which involves adjusting the molar ratio of terephthalic acid (H 2 BDC) to 2-amino terephthalic acid (NH 2 -H 2 BDC). This strategy breaks through the limitations of traditional single-ligand systems. Results revealed that the NH 2 -MIL-101(Fe)-3 (H 2 BDC: NH 2 -H 2 BDC = 1:3) exhibited remarkable adsorption performance in both single and binary systems. The maximum adsorption capacities for TC and CIP reached 827.75 mg/g and 806.26 mg/g, respectively, representing significant increases of 46.34 % and 52.44 % compared to pristine MIL-101(Fe). Although the adsorption capacities decreased in the competitive binary system, they still achieved 641.17 mg/g and 588.43 mg/g for TC and CIP, respectively, outperforming most reported adsorbents. Additionally, NH 2 -MIL-101(Fe)-3 demonstrated robust tolerance to interference from inorganic ions and natural organic matter, along with excellent cyclic regeneration performance. FTIR, XPS, and density functional theory (DFT) calculations clarified mechanisms: -NH 2 groups enhanced the material's polarity and hydrophilicity, facilitating hydrogen bonding; Fe 3 + -antibiotic chelation dominated, supplemented by π-π stacking and pore-filling effects. This multi-mechanism synergy, quantified by DFT-derived binding energies (coordination > hydrogen bonding > π-π interactions). Overall, this study underscores the potential of mixed-ligand functionalized MOFs in addressing complex pollution systems, providing a theoretical foundation for high-performance adsorbent design and antibiotic pollution control.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Ran Zhang,Liye Zhu,Xuan Liu,Jiayin Zhu,Yan Zhao
Owing to the increasing energy demands, direct small-molecule fuel cells, such as ethanol and formate fuel cells, have attracted great attention. During the operation of the fuel cell, noble metal catalysts are widely used to accelerate the reaction kinetics by alloying with other materials. However, there are a few facile methods for improving elemental metal catalytic activity. In this work, the defect-rich palladium (Pd) aerogels are acquired by laser ablating technology, which can significantly improve the intrinsic activity of Pd elementary catalysts through introducing defects and lattice strain. The electrochemical results show that the mass and specific activities of the obtained Pd aerogel for the formate oxidation reaction are 2.26 and 1.99 times higher than those of the commercial Pd/C. The excellent activity and stability of the Pd aerogel for ethanol oxidation reaction have also been demonstrated. The effect of the compressive strain is further investigated by density functional theory (DFT) calculations. It has been found that the compressive strain weakens the adsorption strength of the intermediates, which can facilitate the desorption of toxic specifics. The laser-assisted synthesis of defect-rich aerogel paves a way in optimizing the structure of the elemental metal catalysts and improving their intrinsic catalytic activity.
研究领域:
材料科学
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电化学
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催化
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燃料电池
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Yuan He,Liangjie Wang,Zhan Chen,Xia Huang,Xiaomao Wang,Xiaoyuan Zhang,Xianghua Wen
In the present study, MnMe oxide (Me = Fe, Co, Ce) were in situ embedded on the surface and inside micropores of membranes by redox reaction to fabricate novel catalytic ceramic membranes . The synergistic effect of membrane filtration and catalytic ozonation were evaluated towards atrazine degradation. MnCe-CM owned the best performance with 99.99% atrazine removal in 40 min among four catalytic membranes because of the oxygen vacancies created by Ce 3+ /Ce 4+ and Mn 2+ /Mn 3+ . MnCe-CM was subsequently chosen to explore the optimized operating conditions with a finding of ozone concentration 0.8 mg/min and pH 7. As the catalysts were successfully embedded on the surface and inside the micro-pores of MnCe-CM, the catalytic ozonation took place both on the surface and inside micropores. The reactions on the surface and inside micropores were proved very effective considering that the high specific surface provided sufficient reaction sites while the confined space facilitated the contact between •OH and the reactants. In addition, atrazine degradation pathways were proposed based on the identified byproducts. The reaction sites and the biotoxicity evaluation were calculated by density function theory (DFT) and Toxicity Estimation Software Tool (T.E.S.T), respectively. The present study provides a novel MnCe-CM with dual functions of filtration and catalytic ozonation and outlines the synergistic effect of separation and catalytic ozonation.
研究领域:
环境科学
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催化
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水处理
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高影响因子
RARE METALS
·
2024
·Vol. 43
·期 4
·1513-1523
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IF 9.6
Zhang Ze-Yu,Wang Hai-Bin,Zhang Fei-Fei,Li Jing-Wei,Hu Xin-Zhuo,Yan Si-Wei,Bai Yi-Ming,Zhang Xun,Shen Gu-Rong,Yin Peng-Fei,Yang Jing,Dong Cun-Ku,Mao Jing,Liu Hui,Du Xi-Wen
Electrocatalysis of CO 2 reduction reaction is an effective way to convert CO 2 into high value-added products, but the selectivity of Cu-based catalysts for C 2+ products needs to be improved due to the high energy barrier of C–C coupling. Therefore, a viable catalyst design strategy to decrease energy barrier of C–C coupling should be put forward. Here, a nanocavity-enriched CuPd single atom alloy (CuPd SAA) catalyst is designed to promote C–C coupling process. The faradaic efficiency of CuPd SAA for ethylene and C 2+ reaches 75.6% and 85.7% at − 0.7 V versus reversible hydrogen electrode (RHE), respectively. Based on the results given by in situ characterization, the porous hollow structure dramatically increases the ratio of the linear-bond *CO, thus enhancing the faradaic efficiency for ethylene. Density functional theory (DFT) calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C–C coupling, further improving the faradaic efficiency. This work provides a new idea for designing catalyst with high selectivity for ethylene. Graphical abstract
研究领域:
材料科学
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化学
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电化学
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催化
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
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IF 11.2
Haoyuan Zheng,Yuxiao Jia,Chen Jin,Hang Che,Chia-TseLee,Guang Liu,Li Wang,Yuyuan Zhao,Shixuan He,Haizhen Liu,Xinhua Wang,Yifeng Yu,Mi Yan
The magnesium based metal hydrogen storage composite system Mg(NH 2 ) 2 -2LiH has a theoretical hydrogen storage capacity of 5.6 wt.% and is a promising hydrogen storage material for vehicles. However, its application is limited due to serious thermodynamic and kinetic barriers. Introducing efficient catalysts is an effective method to improve the hydrogen storage performance of Mg(NH 2 ) 2 -2LiH. This article investigates for the first time the use of nano rare earth oxide CeO 2 (∼44.5 nm) as an efficient modifier, achieving comprehensive regulation of the hydrogen storage performance of Mg(NH 2 ) 2 -2LiH composite system through oxygen vacancy driven catalysis. The modification mechanism of nano CeO 2 is also systematically studied using density functional theory (DFT) calculations and experimental results. Research has shown that the comprehensive hydrogen storage performance of the Mg(NH 2 ) 2 -2LiH-5 wt.% CeO 2 composite system is optimal, with high hydrogen absorption and desorption kinetics and reversible performance. The initial hydrogen absorption and desorption temperatures of the composite system were significantly reduced from 110/130°C to 65/80°C, and the release of by-product ammonia was significantly inhibited. Under the conditions of 170°C/50 min and 180°C/100 min, 4.37 wt.% of hydrogen can be rapidly absorbed and released. After 10 cycles of hydrogen release, the hydrogen cycle retention rate increased from 85% to nearly 100%. Further mechanistic studies have shown that the nano CeO 2− x generated in situ during hydrogen evolution can effectively weaken the Mg–N and N–H bonds of Mg(NH 2 ) 2 , exhibiting good catalytic effects. Meanwhile, oxygen vacancies provide a fast pathway for the diffusion of hydrogen atoms in the composite system. In addition, nano CeO 2− x can effectively inhibit the polycrystalline transformation of the hydrogen evolving product Li 2 MgN 2 H 2 in the system at high temperatures, reducing the difficulty of re-hydrogenation of the system. This study provides an innovative perspective for the efficient modification of magnesium based metal hydrogen storage composite materials using rare earth based catalysts, and also provides a reference for regulating the comprehensive hydrogen storage performance of hydrogen storage materials using rare earth catalysts with oxygen vacancies.
研究领域:
材料科学
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催化
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氢气存储
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纳米技术
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DOI
高影响因子
ChemPlusChem
·
2020
·Vol. 85
·期 3
·503-509
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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.
研究领域:
材料科学
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无机化学
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理论化学
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DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2022
·Vol. 105
·期 10
·6370-6383
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IF 4.186
Yu Gao,Liang Huang,Zhaoming Tong,Jianghao Liu,Qi Zhang,Haijun Zhang,Quanli Jia,Shaowei Zhang
A theoretical calculation combined with experiment was used to study high-entropy (Hf 0.2 Ti 0.2 Mo 0.2 Ta 0.2 Nb 0.2 )B 2 (HEB-HfTiMoTaNb). The theoretical calculation suggested HEB-HfTiMoTaNb could be stable over a wide temperature range. Then, a novel solvothermal/molten salt-assisted borothermal reduction method was proposed to efficiently pre-disperse transitional metal atoms in a precursor and synthesize (Hf 0.2 Ti 0.2 Mo 0.2 Ta 0.2 Nb 0.2 )B 2 nanoscale powders at 1573 K for 6 h, which is nearly 300 K lower than previous reports. The characterization results indicated that the as-synthesized nanoscale HEB-HfTiMoTaNb powder was hexagonal single-phase with homogeneous elements distribution and uniform size, and the oxygen content of the particles is 0.97 wt%. Simultaneously, the mechanical properties, anisotropic nature, and thermal properties of HEB-HfTiMoTaNb were investigated by density functional theory (DFT) calculations. The Cannikin's law was adopted to explain the improvement of comprehensive mechanical properties. In addition, a significant reduction of thermal conductivity was observed for HEB-HfTiMoTaNb and it only was 1/15 of the value of HfB 2 . This work suggests a reliable technique for synthesis of nanosized HEB powders and discovery of high-entropy materials under the guidance of first-principle theory.
研究领域:
材料科学
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物理化学
·
理论物理
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Hongbing Wang,Yifei Yang,Linsen Zhou,Jun Chen,Linan Lin,Xinchun Mao,Wei Cui,Yunxi Yao
The reactive interfacial sites upon supported catalysts provide an alternative pathway to enable the reactants activation in an energetically favorable mode, thus decreasing the energy barrier and promoting the catalytic efficiency. By virtue of structural characterization, in-situ spectroscopic analysis, kinetic assessments and density functional theory (DFT) calculations, supported Pt/TiN catalysts are systematically studied to interrogate H 2 O activation on the Pt-TiN interfacial sites and its catalytic function during the low-temperature water gas shift (WGS). It is found that the partially oxygen-covered TiN surface is highly efficient for H 2 O activation by oxygen-assisted dissociation with an energy barrier of 0.41 eV, much less than that on metallic Pt surface. The formed hydroxyls binding on Ti sites, observed by in-situ X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption (TPD), could readily react with the adjacent CO adsorbed on Pt clusters with the reaction energy barrier of 0.43 eV to attain the individual catalytic cycle. Benefiting from the enhanced H 2 O activation, the catalytic turnover rate of CO-H 2 O reaction on Pt/TiN is 3.8 and 20.3 times higher than that on traditional Pt/TiO 2 and Pt/SiO 2 at 403 K, respectively. The interfacial reactive sites are the origin of low-temperature WGS on Pt/TiN catalysts.
研究领域:
催化
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材料科学
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化学工程
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表面化学
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·Vol. 43
·期 45
·20712-20720
·
IF 4.229
Biyao Jin,Yiqi Li,Lianhua Zhao
Bimetallic PdV/C nanoparticles have been synthesized by phase-transfer method for catalyzing the oxygen reduction reaction (ORR) in alkaline electrolytes . PdV/C nanoparticles with different V contents are spherical with a mean diameter of 3–4 nm, and the addition of V expands the lattice parameter of Pd as shown by XRD . XPS analysis indicated the binding energy of Pd 0 3d peak increased by ca. 1 eV. Density functional theory (DFT) calculations results shows d-band center of Pd down-shift after V-doping. Based on the electrocatalytic results, introducing V can improve the catalytic activity for ORR, methanol crossover tolerance and stability. Especially, Pd 4 V/C shows higher initial potential (E onset = 1.027 V), excellent methanol crossover tolerance (98.03% retained) and long-term stability (81.30% retained), which are comparable with Pt/C JM . This work provides a new method of synthesizing PdV/C nanoparticles , which have the potential to be used as the cathode electrocatalysts for fuel cells.
研究领域:
材料科学
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电化学
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纳米催化
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能源材料
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燃料电池
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物理化学
·
表面科学
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高影响因子
危险品化学品经营许可证（带存储）