Environmental Science-Nano
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2017
·Vol. 4
·期 12
·2395-2404
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IF 6.047
Hong-Wei Luo,Xin Zhang,Jie-Jie Chen,Han-Qing Yu,Guo-Ping Sheng
Although the existence of Fe(III) (hydr)oxide nanoparticles (NPs) in natural environments has been recently recognized, their migration and transformation, which are substantially affected by the microbial reduction process, remain unclear. In this study, hematite bioreduction and magnetite formation induced by Shewanella oneidensis MR-1, a typical metal-reducing bacterial strain, were investigated using an integrated approach that combined experiments and computational simulations at the molecular scale. High-resolution transmission electron microscopy coupled with selected area electron diffraction (SAED), Raman spectroscopy and magnetic property analyses confirmed the biogenic magnetite formation. The electron paramagnetic resonance (EPR) spectra show a decay of the EPR intensity with incubation time, implying that the biotransformation of hematite to magnetite led to concurrent changes in their contents and local structures. X-ray absorption fine spectroscopy (XAFS) identified a time-resolved structural evolution of Fe(II)/Fe(III) coordination. The octahedral configuration upon Fe(II) production was subsequently validated by DFT calculations. Microbial reductive dissolution provided various intermediate states and new chemical environments regarding Fe(II)/Fe(III) complexes, such as monodentate and bidentate coordination patterns. Bioreduction caused the breakage of iron–oxygen bonds in hematite and the concomitant formation of Fe complexing microstructures for biogenic magnetite production. All these findings reveal the underlying mechanisms for the biotransformation of Fe minerals at the molecular scale and may allow us to better understand the speciation, immobilization and bioavailability of hematite NPs in natural systems.
研究领域:
微生物学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
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2022
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IF 4.855
Teng Wang,Jiawen Zhang,Ying Cai,Lang Xu,Lingmin Yi
Molecular-scale compositional heterogeneities can slash the nonspecific interaction between proteins and surfaces, resisting surface contamination. In this work, an amphiphilic copolymer containing a soft fluorosilicone macromonomer with controllable chain length as low-surface-energy hydrophobic component and a zwitterionic monomer as hydrophilic component was prepared to establish molecular-scale compositional heterogeneities. The length of the fluorosiloxane side chains can significantly impact the surface compositional heterogeneities, thus influencing the antifouling performance of the copolymer coatings. Even under water, the coating still retains a large number of low-surface-energy fluorosilicone segments on the surface. The balance between hydrophilic and hydrophobic segments on the surface provides a better synergistic effect, which endows the copolymer coatings with excellent resistance to various proteins.
研究领域:
材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS LETTERS
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2022
·
IF 3.574
Xi Wang,Bin Wang,Yanling Yu,Mingfeng Dai,Wei Zhang,Zuowan Zhou
In this study, a multi-scale interface (molecular scale and nanoscale) strategy is proposed to modify basalt fibers (BF) to improve the mechanical strength of BF-reinforced PA6 composites. The target sample achieved a tensile strength of 225.9 MPa, which is 50.8 % and 31.8 % higher than that of the composites corresponding to unmodified BF and molecular scale modified BF, respectively. For multi-scaled interface, the molecular scale promotes the infiltration of the fiber by the resin matrix, and the nanoscale is conducive to the formation of a mechanical interlocking structure between the PA6 matrix and the fiber. It is through the above-mentioned dual effects of multi-scale interfaces that the BF-reinforced PA6 composites exhibit attractive mechanical properties.
研究领域:
材料科学
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复合材料工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
·
IF 4.2
Xuejuan Wei,Xiaopeng Chen,Linlin Wang,Xiaojie Wei,Yang Yang,Jiaqi Liang,Jiezhen Liang
Isothermal vapor–liquid equilibrium data of the binary system (−)-α-pinene + (−)-β-pinene and the quaternary system (−)-α-pinene + (−)-β-pinene + water + phenoxyacetic acid were measured at 313.2, 323.2, and 333.2 K using headspace gas chromatography. The experimental data showed that the addition of phenoxyacetic acid and water promoted the separation of (−)-α-pinene and (−)-β-pinene. The experimental data were correlated using the UNIQUAC and NRTL models. The two models showed good correlation for the binary system, whereas the UNIQUAC model gave more accuracy for the quaternary system. Moreover, the COSMO-RS model can be an efficacious method for predicting VLE data of the determined binary and quaternary systems. In addition, the optimal spatial configuration and binding energy between the molecules were obtained by DFT, and the effects on (−)-α-pinene and (−)-β-pinene with the addition of phenoxyacetic acid and water were discussed on the molecular scale.
研究领域:
化学工程
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物理化学
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热力学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zhonglei Xu,Xuejiao Zhang,Xinying Li,Hao Zha,Jun Chen
Chromium (Cr(VI)) and phosphate contaminants in wastewater pose severe threats to ecosystems and human health. To address this challenge, we engineered a novel molecular-scale organic-inorganic hybrid material (Lys-HZO) through facile integration of lysine (Lys) with hydrated zirconium oxide (HZO). The uniform anchoring of Lys within the HZO framework significantly enhances the material’s hydrophilicity, improving the accessibility of adsorption sites both internally and externally, thus overcoming the structural limitations of traditional HZO materials. The amino and hydroxyl groups in the material create a synergistic effect through multiple mechanisms, including electrostatic attraction, ligand exchange, and redox interactions, which collectively drive the adsorption process. Batch adsorption experiments showed that the material’s adsorption capacities for Cr(VI) and phosphate were 15 and 10 times higher, respectively, than those of pure HZO. Kinetic and isothermal adsorption analyses confirmed that adsorption is primarily governed by chemisorption, while thermodynamic studies indicated the adsorption process’s spontaneous and endothermic nature. In cyclic fixed-bed column experiments under competitive ion conditions, Lys-HZO demonstrated high adsorption capacity, treating 2532 bed volumes (BV) of phosphate-containing wastewater (3 mg P/L) and 726 BV of Cr(VI)-contaminated effluent (3 mg Cr(VI)/L). The treated effluent concentrations remained below regulatory limits: < 0.5 mg P/L and < 0.2 mg Cr(VI)/L, respectively. The innovative design strategy of "molecular-scale hybridization and site synergistic activation" proposed in this study not only fully unlocks the adsorption potential of HZO materials, but also provides novel insights for developing amino acid-functionalized metal oxide hybrid materials in the field of water treatment.
研究领域:
环境科学
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材料科学
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水处理技术
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纳米技术
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zirun Chen,Shaohong Liu,Luyi Chen,Junlong Huang,Bingna Zheng,Wen Huang,Shimei Li,Yuheng Lu,Ruowen Fu
Carbon aerogels have attracted increasing research interest in a wide range of potential applications owing to their unique structural features, yet the scalable preparation of carbon aerogels configured by nanoporous carbon skeletons with high surface area and precise pore structure is a great challenge. Herein, we report a molecular-scale interface engineering concept for high-throughput and scalable production of well-defined microporous carbon aerogels (MPCAs) based on simple and fast polycondensation (<8 s) of dialdehyde with silsesquioxane. Benefiting from the unique organic/inorganic hybrid molecule structure, the silsesquioxane favours the formation of molecular-scale silica templates with uniform carbon source/template interface. The resulting MPCAs exhibit 3D interconnected macroporous framework combined with well-defined micropore skeleton and large surface area. These intriguing features render MPCAs superb pore accessibility and utilization, and thus they demonstrate great promise as adsorbent materials for rapid removal (<10 s) of organic micropollutants with high uptake, and as electrocatalyst supports for incorporation of metal-nitrogen-carbon species with excellent activities.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHINESE CHEMICAL LETTERS
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2025
·
IF 8.9
Ying Li,Zelin Wu,Xiaoyu Liu,Bingkun Huang,Jing Zhang,Yanbiao Shi,Chuan-Shu He,Zhaokun Xiong,Xingxing An,Bo Lai
Extensive research has been devoted to single-atom activation of persulfates in recent years. However, mechanistic understanding of the distinct interactions between different persulfates ( i.e. , peroxymonosulfate (PMS) and peroxydisulfate (PDS)) and the coordination environments of single-atom catalysts (SACs) remains critical for advancing their practical applications. Herein, we developed a Fe-N 4 SAC exhibiting dual activation capabilities for both PMS and PDS. Intriguingly, experimental results revealed divergent activation mechanisms: PMS activation was predominantly mediated via single-site reactions generating singlet oxygen ( 1 O 2 ), whereas PDS activation proceeded through both dual-site and single-site pathways involving concurrent 1 O 2 generation and electron transfer processes. Density functional theory calculations further demonstrated that the geometric alignment between the inter-site distances of Fe-N 4 centers and the molecular dimensions of PDS serves as the key determinant for enabling the electron transfer pathway. This fundamental structure-reactivity correlation suggests that the intrinsic molecular-scale differences between PMS and PDS govern their distinct interaction mechanisms with Fe-N 4 SACs. Finally, the scale-up experiments realized nearly complete sulfamethoxazole degradation during 120 h continuous operation without obvious decline in both the Fe-N 4 /PMS and Fe-N 4 /PDS systems. This work provides fundamental insights into molecular-scale effects on persulfate activation mechanisms, establishing new design principles for SACs optimization in advanced oxidation processes.
研究领域:
催化
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环境化学
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材料科学
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物理化学
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水处理技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）