CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Chunjie Liu,Jing Wang,Hua Huang,Luyang Li,Liang Chen,Haiyan Zhang
Separation materials have focused on porous particles with a microporous structure and a large specific surface area. However, for specific separation processes such as biomacromolecules, cell fermentation liquid, or high viscosity liquids, large pores can substantially reduce mass transfer resistance and enhance mass transfer efficiency. Therefore, a more detailed investigation is required to develop a simple method for obtaining super-macroporous particles. In this work, we presented a strategy that combined gas-shearing and sulfolane freeze casting to obtain poly (methyl methacrylate) (PMMA)-based cryogel particles with a tunable size (476–1873 μm) and polarity (contact angle of 135°–0°). The cryogel particles had a micron-scale porous structure (16.8–46.8 μm), and the volume shrinkage effect during sulfolane crystallization formed unique surface single pores (93.7–294.6 μm) and an internal hollow structure (218.4–615.6 μm). Cryogel particles with high porosity (>75 %) and good hydrophobicity had a high absorption capacity for organic solvents and oils (>15 g g −1 ). Meanwhile, the cryogel particles exhibited a column effect that was 1.3–3.9 times greater than that of the macroporous resin, along with superior adsorption kinetics. This study provides a novel strategy for obtaining super-macroporous particles with tunable particle size and composition, achieving efficient separation in special systems.
研究领域:
生物分离工程
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材料科学
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化学工程
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高分子材料
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吸附分离技术
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产品关联
DOI
高影响因子
Carbon Capture Science & Technology
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2025
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IF 10.5
Zeyou Meng,Xin Ye,Xiao Sun,Jiahao Li,Nan Wang,Zhen Wang,Gang Xie
To address the two major challenges of low active site utilization and amine loss in traditional amine-functionalized CO 2 adsorbent, this study proposed a synergistic strategy of “hierarchical pore channels-polarity regulation”. Using hierarchical mesoporous silica (HMS) as the support, a dual-functional modification approach combining aminopropyltrimethoxysilane (APTMS) and butyltrimethoxysilane (BTMS) grafting with tetraethylenepentamine (TEPA) impregnation was employed to construct an efficient CO 2 adsorption system with dual active sites. APTMS and BTMS were alternately grafted onto the HMS via siloxane bonds, resulting in a structure with varying polarities. The strong polarity of TEPA interacts simultaneously with the terminal groups of APTMS and BTMS, facilitating the uniform dispersion of TEPA within the material. The optimized HMS-AB-70T adsorbent exhibited a dynamic CO 2 adsorption capacity of 5.34 mmol g −1 at 70°C, with a reduction of 9.8% in adsorption capacity after 10 cycles. In a humid environment, its performance was further enhanced to 5.89 mmol g −1 . The CO 2 adsorption mechanism was revealed by in situ infrared spectroscopy and kinetic analysis, involving the formation of carbamate and bicarbonate species. By adjusting the hydrophilic-lipophilic balance of the P123 template, a hierarchical mesoporous structure of HMS (∼6 nm and ∼10 nm) was successfully achieved, promoting rapid mass transfer and providing abundant adsorption sites. This strategy offers a novel molecular-level approach for the design of efficient and stable CO 2 adsorbents.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Jialin Li,Xuzhou Tian,Chunlei Xia,Yuting Duan,Yi-nan Sun,Binghui Liu,Liming Wu,Chunyu Ru,Shi-Tong Zhang,Chengji Zhao
The approach to constructing proton transport channels via direct adjustments, including hydrophilia and analytical acid concentration in hydrophilic domains, has been proved to be circumscribed when encouraging the flatter hydrophilic–hydrophobic microphase separation structures and reducing conductivity activation energy. Here, we propose a constructive solution by regulating the polarity of hydrophobic domains, which indirectly varies the aggregation and connection of hydrophilic ion clusters during membrane formation, enabling orderly self-assembly and homogeneously distributed microphase structures. Accordingly, a series of comb-shaped polymers were synthesized with diversified optimization, and more uniformly distributed ion cluster lattices were subsequently observed using high-resolution transmission electron microscopy. Simultaneously, combining with density functional theory calculations, we analyzed the mechanism of membrane degradations caused by hydroxyl radical attacks. Experimental results demonstrated that, facilitated by proper molecule polarity, beneficial changes of bond dissociation energy could extend the membrane lifetime more than the protection from side chains near ether bonds, which were deemed to reduce the probability of attacks by the steric effect. With the optimal strategy chosen among various trials, the maximum power density of direct methanol fuel cell and H2/air proton exchange membrane fuel cell was enhanced to 95 and 485 mW cm–2, respectively.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
Journal of the American Chemical Society
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2025
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IF 15.6
Shaochong Cao,Tianlin Zhou,Yongshuai Liu,Wenyi Lu,Aiwen Zhang,Shan He,Pengshu Yi,Longli Ma,Zhu Liu,Fengkai Zuo,Liang Cao,Zhouhong Ren,Mingxin Ye,Huayi Fang,Jianfeng Shen
Aqueous zinc batteries are promising energy storage systems, but face significant challenges, including zinc dendrite growth, electrochemical corrosion, and poor reversibility for large-scale applications. Herein, we design a defective fluorinated covalent organic framework (FCOF) with localized high polarity based on a truncated monomer strategy. Controllable defect design in the FCOF framework produces polar amino groups with enhanced Zn2+ trapping ability. Meanwhile, an additional transport pathway was formed at the well-designed defect sites, which reduced the migration energy barriers. The Zn2+ diffusion coefficient of the optimal defective FCOF separators (FCOF-30, with 30% defect content) was calculated to be 9.83 × 10–10 cm s–1 (2 times higher than FCOF). At 10 mA cm–2 (5 mAh cm–2), the symmetric cell using FCOF-30 exhibited excellent Zn2+ deposition/stripping behavior with 1200 h cycling stability. This defect engineering concept provided in-depth insights into the ion transport regulation for the electrochemical energy storage applications.
研究领域:
材料科学
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电化学
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能源存储
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纳米材料
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界面科学
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功能材料
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2025
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IF 5.5
Yu Zhou,Chuanping Li,Yulong Zhou,Changyong Hu,Guan Yang,Xiandong Zhu
The rational design of catalytic materials featuring high specific surface area, precise compositional control, and ordered porosity is crucial for enhancing the performance of electrochemical sensors. Two-dimensional conductive metal–organic frameworks (2D c-MOFs) have garnered significant attention as promising candidates for sensing applications due to their intrinsic electrical conductivity, crystalline structural uniformity, and robust chemical stability. In this study, we demonstrate precise morphological control of M3(HITP)2 (M = Co, Ni) arrays on carbon cloth (CC) via solvent polarity-modulated hydrothermal synthesis. By tailoring reaction conditions, we obtained distinct nanostructures: vertically aligned nanorod arrays (Ni3(HITP)2/CC-0.3) and interconnected nanosheet networks (Co3(HITP)2/CC-3). The Ni3(HITP)2/CC-0.3 sensor exhibited remarkable ascorbic acid (AA) detection capabilities, achieving an ultrawide linear range (0–4.0 mmol·L–1) and a submicromolar detection limit (0.25 μmol·L–1). Additionally, the sensor demonstrated rapid response, outstanding selectivity, and stable performance over 30 days. This work provides a versatile platform for engineering MOF-based electrochemical sensors in the ultrasensitive detection of biomolecules.
研究领域:
电化学传感器
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纳米材料
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金属-有机框架
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生物传感
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分析化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Weimeng Cai,Haojie Du,Erju Wang,Yuting Qiang,Kunhong Hu,Jianhua Guo
The synthesis of value-added chemicals from renewable biomass is becoming increasingly important in the transition to a sustainable and low-carbon energy system. Herein, we demonstrate a solvent-polarity modulation strategy to engineer biomass-derived Cu-MOF using 2,5-furandicarboxylic acid (FDCA) as a renewable ligand, where tailored β/α ratios via Kamlet-Taft parameters balance nucleation-growth kinetics to optimize textural properties. Pyrolyzed Cu-MOF at 500 °C under a nitrogen atmosphere yield the Cu/C catalysts, which were subsequently employed in the selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). Among the various solvents used, the Cu-MOF precursor synthesized in a mixed solvent of methanol and N, N-dimethylformamide (DMF) demonstrated the highest catalytic performance, outperforming those synthesized in other solvents. This highlights the significant impact of solvent selection on the structure of Cu-MOF, which in turn affects their hydrogenation activity. Advanced characterization confirming that the uniform Cu dispersion (confirmed by HRTEM mapping) and Cu⁰/Cu⁺ electronic synergy (via Cu Auger analysis) enhanced hydrogenation performance. Additionally, the biomass-derived catalysts exhibited excellent durability. Overall, this research provides a promising approach to develop highly efficient catalysts using renewable ligands and demonstrates the potential of regulating catalyst properties through the strategic selection of solvents, as informed by Kamlet-Taft parameters.
研究领域:
催化化学
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绿色化学
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材料科学
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可再生能源
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化学合成
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产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
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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.
研究领域:
电化学
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材料科学
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催化化学
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纳米技术
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理论化学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）