INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Mengbo Wu,Qingrong Zheng
Enhancing the storage capacity of hydrogen on MOFs and making it suitable for the marine environment are crucial to its onboard application as a hydrogen storage medium. Development of the storage medium was based on the density of hydrogen contained within the storage system equipped on a typical fuel cell powered ship. The researches conducted include density functional theory (DFT) calculations and experiments, which were directed to evaluate the effect of incorporating graphene oxide (GO) on enhancing the storage performance of hydrogen on ZIF-8. DFT calculations were performed to determine adsorption energies between the GO@ZIF-8 composites and hydrogen molecules, the reduced density gradient (RDG) scatter plot and isosurface map analysis were then employed to define the interaction mechanism between the GO and ZIF-8 as well as the GO@ZIF-8 composites and hydrogen molecules. Precipitation was employed at ambient temperature to synthesize the ZIF-8 sample and GO@ZIF-8 composites, which were performed the tests further for analyzing adsorption equilibrium as well as the performances of cycling and hydro-stability. Results show that the interaction between the GO and ZIF-8 as well as the GO@ZIF-8 composites and hydrogen molecules can be ascribed to the van der Waals force, and the interaction can be enhanced by incorporating a suitable amount of GO. Within the range 0–8 wt% amount of GO incorporated, the sample added by 2 wt% GO (GO-2@ZIF-8) had a more preferable structure for hydrogen adsorption, and the isosteric heat of hydrogen adsorption on this sample is larger than that on the ZIF-8. It also shows that the incorporation brought about the enhancement on the cycling performance at 77.15 K within 0–5 MPa as well as on the hydro-stability of the sample. It suggests that the composite prepared by incorporating ZIF-8 with GO is a promising medium for on board hydrogen storage.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
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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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
LIQUID CRYSTALS
·
2023
·
IF 2.2
Ran Chen,Zihao Mao,Jiaxing Tang,Xinbing Chen,Pei Chen,Zhongwei An
Liquid crystal (LC) mixtures with high birefringence (∆n) and low rotational viscosity play an essential role for fast-response LC devices. However, high birefringence and low rotational viscosity are a pair of contradictory performance parameters. In this work, two high-∆n LC diluters are proposed to achieve a fine balance between them. These two terminal olefin diluters containing a rigid biphenyl core with a lateral fluorine substituent, a buty-3-enyl terminal group and a flexible n-alkyl chain were designed and synthesised through classical organic synthetic reactions. Meanwhile, their comprehensive properties were further evaluated in a LC mixture P02-F containing fluoro-tolane and a LC mixture P12-ISO containing isothiocyano-tolane. The results show that the biphenyl diluters 2BBF2V and 3BFB2V could effectively decrease the Tm of LC mixture P12-ISO to below −25°C, while maintain high ∆n and large Δε, which are suitable for the high-∆n LC mixtures containing isothiocyano-tolane. Furthermore, DFT calculations of molecular conformation and polarisability components were utilised to correlate the experimental findings.
研究领域:
材料科学
·
化学
·
液晶技术
·
有机合成
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高影响因子
FUEL
·
2025
·
IF 7.5
Xiaohui Wang,Zhilong Cheng,Bingrong Liu,Huiyi Liu,Xin Fang,Ruiqi Chai,Lishuang Ma,Yuchao Lyu,Jianye Fu,Xinmei Liu
Methane dehydroaromatization (MDA) was a promising technology for the synthesis of high value-added aromatics through natural gas. Fe/ZSM-5 catalysts were widely used in MDA reaction. However, its catalytic mechanism remained ambiguous. In this work, a novel one-pot strategy was developed for the preparation of Fe/ZSM-5 catalysts, which can delicately control the iron species and acidic property of Fe/ZSM-5 catalysts. In-situ DRIFTS and DFT calculation demonstrated that MDA followed a bifunctional mechanism and the second C–H bond breaking process of CH 4 was the rate-determining step, where methane underwent coupling and dehydrogenation at the iron active sites to generate intermediate species (ethylene), and Brønsted acid sites played a key role in determining the selectivity of aromatics. Moreover, CO-pulse chemisorption revealed the quantitative synergistic effect between metal active sites and Brønsted acid sites. Catalysts with highly dispersed iron oxide and proper density of Brønsted acid sites exhibited the best catalytic performance. This study elucidated the catalytic roles of iron species and Brønsted acid sites in Fe/ZSM-5 catalysts in MDA and provided guidance for the future development of highly active MDA catalysts.
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Science China-Chemistry
·
2023
·Vol. 67
·期 3
·981-989
·
IF 9.6
Guan Qitao,Shen Zhen,Tian Yiqiang,Huang Genping,Zhang Chun
The Ni-catalyzed highly selective diborylative cyclization of 1,6-enynes with diboron reagent has been developed. When pinB-Bdan was used, multiple types of boron-containing functional groups could be installed into organic molecule with great chemoselectivity and regioselectivity though this reaction. Meanwhile, if B 2 pai 2 was employed, the asymmetric diborylative cyclization could be well induced by using strategy of dynamic kinetic resolution. Importantly, the above reactions could afford desired product with 100% atomic economy, and could be compatible with different series of substituents. The studies of further transformation well illustrated that different type products could serve diverse synthetic strategy. Notably, the reaction mechanism was intensively studied by density functional theory (DFT) calculations, which could reveal the mechanism of regio- and enantio-selective control.
研究领域:
有机化学
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金属催化
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合成方法学
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计算化学
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硼化学
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 45
·30993-31002
·
IF 3.3
Siqi Dai,Xiaoyan Gan,Kegui Li,Qiang Huang,Liling Guo,Hanxing Liu
Lead-free metal halide perovskites have received widespread attention due to their composition of minimal hazardous components, excellent air stability, and long carrier lifetimes. However, the majority of the lead-free metal halide perovskites, such as Cs3Bi2Br9, have wide bandgaps, which limits their photoelectric in solar cells and optoelectronic devices. To address this issue, attempts have been made to adjust the bandgap through material alloying. Based on a solution approach, a pure phase of Cs3Bi2−xSbxBr9 crystals has been synthesized, with the alloying parameter x changing over the full range of composition. It is found that the mixed alloy has a smaller bandgap than pure Bi-based and Sb-based perovskites, with the smallest bandgap of 2.22 eV near x = 1, and there is a phenomenon of bandgap bowing throughout the alloying process. The electronic structure of Cs3Bi2−xSbxBr9 has been investigated using DFT calculations and the bandgap bowing of Cs3Bi2−xSbxBr9 is deduced to be related to the type-II band alignment between the Cs3Bi2Br9 and Cs3Sb2Br9. Owing to the mismatch of s and p orbital energies of Bi and Sb, the mixed alloy has a smaller bandgap. Our work demonstrated a method for achieving bandgap reduction and explained the phenomenon of bandgap bowing by pairing materials into type-II band alignment, which may also be found in other lead-free metal perovskites.
研究领域:
材料科学
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物理学
·
化学
·
太阳能
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高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Canyang Zhang,Guangtong Hai,Chao Chen,Yin Liang,Wei Zhao,Bolong Li,Jianghao Wang,Zhenyu Zhang,Huiping Ji,Kaige Wang,Reinout Meijboom,Jie Fu
The decarbonylation of biomass-derived fatty acids offers a green and sustainable route to high-value long-chain alkenes. Nitrogen-doped carbon-supported cobalt (Co-NC) catalysts have emerged as promising candidates for fatty acid decarbonylation, attributed to their exceptional catalytic activity and cost-effectiveness. However, identifying the active sites and elucidating the reaction mechanism remain significant challenges. To address these issues, we developed Co single-atom-rich catalysts (CoPc/MWCNT and pyrolyzed derivatives CoPc/MWCNT-X) via the impregnation of cobalt phthalocyanine onto multiwalled carbon nanotubes (MWCNTs), followed by pyrolysis. These catalysts exhibited a high stearic acid decarbonylation activity, increasing the heptadecene yield from 12.9 to 47.4%, with an alkene-to-alkane ratio of up to 4.3. Comprehensive characterization and control experiments conclusively demonstrated that Co single-atom sites serve as the active sites, while coexisting Co/CoO nanoparticles showed negligible activity and no synergistic effects. In situ DRIFTS revealed carbonyl group adsorption on Co single atoms, with DFT calculations confirming directional alkene production via C–O bond cleavage. This work establishes a facile synthetic strategy for high-performance decarbonylation catalysts and unambiguously identifies the critical single-atom active sites while enabling a profound understanding of fatty acid conversion mechanisms.
研究领域:
催化
·
绿色化学
·
材料科学
·
化学反应工程
·
表面化学
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高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 21
·11445-11453
·
IF 11.9
Yumeng Li,Yingmin Jin,Xin Zong,Xuebai Zhang,Guanshu Li,Yueping Xiong
Electrocatalytic carbon dioxide (CO2) reduction reactions (ECO2RRs) to form formate with high faradaic efficiency (FE) and production rate by renewable electricity are ideal to control CO2 concentration in the atmosphere. In this work, we successfully prepared bimetallic BixIny nanofiber (NF) catalysts with interconnected 3D network structure and controllable growth direction of crystal facets via electrospinning and the following electrochemical reduction for the first time, rendering a significantly increased InBi (200) lattice plane proportion in Bi5In5 NFs, which facilitated the improvement of intrinsic catalytic activity and formate selectivity for ECO2RR catalysts, as evidenced by crystalline characterization and DFT calculations. Consequently, the obtained Bi5In5 NFs achieve a maximum FE of 96.8% for formate and the corresponding production rate can reach 4.55 mmol h−1 cm−2, superior to most of the formate producing catalysts. This work provides a novel approach for preparing bimetallic catalyst NFs with high FE and product selectivity; moreover, the favorable productivity brings substantial application potential in industrial production.
研究领域:
材料科学
·
电化学
·
催化
·
环境科学
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高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 5
·1467-1476
·
IF 5.721
Zhuo-Qian Li,Xinxin Fu,Caiyan Gao,Jinyu Huang,Baojun Li,Yongpeng Yang,Jie Gao,Yonglong Shen,Zhikun Peng,Jing-He Yang,Zhongyi Liu
The one-step hydroalkylation of benzene to cyclohexylbenzene (CHB) needs to occur on bifunctional metal/zeolite catalysts, and introducing more acid sites to match the metal sites plays a key role in improving the matching of acid/metal sites toward the requirements of benzene hydroalkylation. Herein, we designed and constructed a Si–Al framework coating with extra acid sites outside the surface of the Pd/HBeta catalyst and obtained a zeolite-encaged Pd NP structure (Pd@HBeta). Notably, the Pd@HBeta catalysts achieved excellent catalytic performance with 44.0% CHB selectivity at about 85.0% benzene conversion, which is much higher than that of the Pd/HBeta catalyst with a CHB selectivity of 25.1% at the same benzene conversion. The remarkable increment of CHB selectivity of Pd@HBeta is mainly attributed to the extra acid sites provided by the coated Si–Al framework as well as the increase of the B/L ratio. Moreover, the adsorption capacity of benzene and cyclohexene is greatly improved after introducing extra acid sites by coating the Si–Al framework, which is beneficial for both hydrogenation and alkylation. Further DFT calculations reveal that C6H10 can easily desorb from Pd NPs and migrate to the acidic channel of HBeta in the Pd@HBeta catalyst than that in Pd/HBeta. Our work presents an elegant example of catalytic hydroalkylation selectivity regulation by coating an extra Si–Al framework to enhance the matching of acid/metal balance.
研究领域:
催化
·
化学工程
·
材料科学
·
物理化学
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高影响因子
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