APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Qiang Guo,Yu Qiao,Yonghou Xiao,Yi Pan,Yushan Li,Xu Liu,Gaohong He
Cuprous ion modified molecular sieves have been considered as promising CO adsorbents in gas separation or purification industry. However, it persists as a significant challenge to overcome the unfavorable effect of water vapor in the work environment on gas adsorption and separation. Herein, we propose a synthetic strategy using rare earth element La as an additive to form La O La coordination bonds followed by surface silanization treatment to construct a hydrophobic Si O Si barrier to significantly improve the stability of Cu + under humid atmosphere. By successively introducing La 3+ and Cu + into zeolite 5A, CuCl/LaA adsorbents were prepared via ion exchange and solid dispersion methods. And then by silanization modification using toluene as solvent and butyltrichlorosilane (BTS) as hydrophobic agent, hydrophobic CuCl/LaA-BTS adsorbents were prepared. Dynamic adsorption investigation demonstrated that the as-prepared CuCl/LaA-BTS adsorbents possessed hydrophobic surface and consequently the adsorption capacity of CO was enhanced significantly under humid atmosphere. The CO adsorption breakthrough capacity over CuCl/LaA-BTS attained 0.34 mg/g, which was 5.7 times higher than that of zeolite 5A at 40 °C, atmospheric pressure and a relative humidity of RH = 55 %. Moreover, the CO adsorption capacity of CuCl/LaA-BTS retained 0.31 mg/g after four cycle regenerations. This work provides an effective and novel route for synthesizing highly stable cuprous ion modified zeolite adsorbents.
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APPLIED SURFACE SCIENCE
·
2025
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IF 6.9
Yi Li,Shiyin Ji,Yangzhou Fan,Tao Duan,Youkui Zhang
The Haber-Bosch process for ammonia synthesis is energy-intensive and environmentally damaging, while nitrate wastewater poses risks to both the environment and human health. Utilizing electrochemical method could remove nitrate in the sewage and a part of nitrate would been reduced to ammonia provided a highly efficient approach for nitrate removal and ammonia synthesis. In this study, incorporated Cu and Co on boron-nitrogen-doped graphite (BCN) substrate with eminent conductivity synthesized BCN-CuCo catalyst. On the catalyst, Cu and Co gave rise to synergistic effect which aroused charge redistribution between Cu and Co, which facilitated the nitrate adsorption, accelerated catalytic kinetics for nitrate reduction. BCN-CuCo catalyst demonstrated eminent performance for nitrate reduction, achieving a high Faradic efficiency of 95.8 % at −0.46 V vs RHE and an impressive ammonia yield rate of 12321.6 μg h −1 mg cat -1 at −0.86 V vs RHE in 0.5 M H 2 SO 4 with 0.1 M KNO 3 . It also showed excellent performance in HNO 3 and neutral media, expanding its application scope. Ultimately, the BCN-CuCo facilitated the production of 320 mg of ammonium diuranate in a neutral medium, supporting sustainable resource utilization. This research provides an efficient strategy for ammonia synthesis and introduces a method for recycling resources from uranium and nitrate-contaminated wastewater.
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CARBON
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2025
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IF 11.6
Zhaojin Li,Zezhao Li,Chenze Di,Di Zhang,Qiujun Wang,Huilan Sun,Qujiang Sun,Fei Yuan,Ranran Li,Bo Wang
Oxygen (O) and Boron (B) heteroatom doping has emerged as a promising strategy to enhance the capacitive performance of activated carbon (AC) for supercapacitors. However, the synergistic mechanism between these heteroatoms remains ambiguous due to intertwined morphological and compositional changes during conventional doping processes. This study employs a stepwise doping methodology to independently control O and B concentrations while preserving the structural integrity of AC. Through sequential high-temperature B doping and low-temperature oxidation, dual-doped AC (AC-O-B) retains comparable specific surface area and pore structure to pristine AC. Electrochemical evaluations reveal that O-B double doping has no significant effect on the double-layer capacitance, but it greatly improves the pseudocapacitance. Mechanistic analysis demonstrates that O doping introduces abundant C-O groups and facilitating the formation of BC 2 O structures via B integration. The presence of C-O groups and BC 2 O structure not only enhance surface wettability but also optimize charge transfer kinetics and redox-active site density. This work provides critical insights into heteroatom co-doping strategies for designing high-performance carbon-based supercapacitors.
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CARBOHYDRATE POLYMERS
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2025
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IF 12.5
Shanglin Li,Yulun Wu,Yajuan Li,Longjiang Tian,Ting Zhang,Jingbo Liu,Zhiyang Du
Assembly is a natural process where molecules spontaneously form ordered structures with specific functions. In supramolecular co-assembly, interactions between surface soft patches drive structural changes, though this key aspect is often overlooked. In this study, we propose a strategy for supramolecular co-assembly mediated by surface soft patches and apply this approach to optimize the broad-spectrum antibacterial activity of lysozyme (LYS)-konjac glucomannan (KGM) supramolecular co-assembly. Surface charge distribution revealed distinct soft patches on LYS and KGM, with hydrogen bond and hydrophobic interactions between them driving supramolecular co-assembly. Characterized by a densely packed β-sheet structure, the supramolecular co-assembly exhibited excellent rheological properties and significantly enhanced antibacterial activity across a broad spectrum. Specifically, the antibacterial efficacy against Staphylococcus aureus exceeded 99.94 %, and that against Escherichia coli reached over 99.95 % in the Ca 2+ -KGM-LYS coacervate. This research sheds new light on supramolecular co-assembly mechanisms and paves the way for designing broad-spectrum antibacterial materials.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Wensheng Wei,Yuxin Wang,Guangwen Xu,Jinggang Zhao,Lei Shi
In this work, a series of multifunctional integrated heterogeneous catalysts (PS-[EIMBr-COO] 2 M, M = Fe 2+ , Co 2+ , Ni 2+ and Zn 2+ ) with abundant active sites and a dynamic swing-active architecture were successfully constructed, which were applied in catalytic cycloaddition of CO 2 and propylene oxide (PO) for efficient propylene carbonate (PC) preparation. The PS-[EIMBr-COO] 2 Co catalyst demonstrated the best catalytic activity with a 98.92 % conversion of PO, a 99.00 % selectivity towards PC, and a TOF value of 120.75 h −1 at 110 °C. The characterization techniques and theoretical simulation revealed that the excellent catalytic performance of the PS-[EIMBr-COO] 2 Co catalyst was attributed to the synergistic effect of the Lewis acid center, imidazolinium groups (Lewis base), Br − ions (nucleophilic site), and swing-active structure. The synergistic effect between active sites reduced the reaction energy barrier of the rate-determining step, and the swing-active structure in catalyst was believed to improve the contact efficiency between the active site and the reaction substrate. The synthesized PS-[EIMBr-COO] 2 Co catalyst was structurally stable and maintained its initial catalytic ability after seven cycles. Moreover, the PS-[EIMBr-COO] 2 Co catalyst shows good substrate universality for the cycloaddition reactions of epoxides. The catalyst construction strategy of functional integration and flexible active structure has high universality for cycloaddition catalyst design, and has important guiding significance for rational design of efficient heterogeneous catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Qinghai Long,Yutao Bai,Anteng Dai,Huajie Qiu,Xuanang Fu,Xiaoyun Chen,Chao Liu,Waseem Hayat,Bihong Lv,Guohua Jing,Zuoming Zhou
In this study, 2-dibutylaminoethanol imidazole ([DBAE][Im]) was developed as a novel ionic liquid for energy-efficient CO₂ capture to address key challenges, such as high energy consumption and elevated regeneration temperatures, associated with conventional amine-based absorbents. The self-extractable behavior of [DBAE][Im] facilitated reversible liquid–liquid phase separation during CO₂ absorption and desorption. The CO 2 absorption loading of the [DBAE][Im] solution (0.5 mol·L −1 ) reached 0.82 mol·mol −1 at 313.15 K, and the regeneration efficiency remained high at 87 % even after five consecutive regeneration cycles at 371.15 K. The reaction and self-extraction mechanisms were determined using carbon nuclear magnetic resonance spectroscopy and quantum chemical calculations. These analyses revealed that the significant polarity difference and weak hydrogen bonding between [DBAE][Im] and water (H₂O) induced a phase transition before CO 2 absorption. During absorption, CO 2 reacted with [DBAE][Im] to form carbamate/bicarbonate (HCO₃ − /CO₃ 2− ) species, which resulted in a homogeneous solution due to the decreased polarity of CO₂ products and the strong hydrogen bonds formed between the products and H₂O. Following thermal desorption, [DBAE][Im] separated into the upper phase, restoring its high polarity and reducing intermolecular hydrogen bonding with H₂O. Owing to its self-extraction capability, the regeneration rate of [DBAE][Im] improved significantly at 371.15 K, while the regeneration heat duty was reduced by 47 % compared to monoethanolamine. The results demonstrate that the novel aqueous [DBAE][Im] absorbent offers substantial energy savings for CO₂ capture, presenting a promising approach for advancing carbon capture technologies.
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ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Jian Zhang,Jia-Fang Xie,Jie-Jie Chen,Wen-Wei Li,Jia-Cheng E. Yang,Yu-Ming Zheng,Han-Qing Yu
Heterogeneous peroxymonosulfate (PMS) activation is of great potential for sustainably degrading antibiotics included emerging contaminants from water. However, developing synthetic metal catalysts with incompatible mass transfer and optimized metal sites to effectively enable low-levels PMS activation and antibiotics removal is challenging. Herein, a protein-like Co catalyst of spatially hierarchical hydrophilicity is synthesized by constructing flower-like Mg/Al layered double hydroxide (LDH) on super-active carbon (AC) to disperse thin-layer Co(OH) 2 along the edge of LDH. The resulting AC-LDH@Co(OH) 2 catalyst demonstrates an impressive antibiotic removal of ≈80% within 15 s and turnover frequency of 45.72 min −1 based on catalyst mass by activating 0.075 mM PMS, surpassing single-atom catalysts included reports. In a fixed-bed reactor with secondary wastewater effluent, AC-LDH@Co(OH) 2 realizes complete removal of norfloxacin for 66 h with neutral effluent pH and negligible metal leaching. Experiments combined with theoretical computations reveal that the protein-like complex not only accelerates transfer of low-levels hydrophilic PMS and hydrophobic antibiotics, but also stably confines Co sites with regulated electronic structure for multiply reactive oxygen species generation.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Wenjun Li,Jianyou Feng,Haoyu Zhang,Chengqiang Tang,Jinyan Li,Ziwei Liu,Yiqing Yang,Jiajia Wang,Kun Zhang,Songlin Zhang,Huisheng Peng,Xuemei Sun
Fiber electrochemical sensors hold great promise for wearable and implantable biomedical monitoring due to their miniature size and excellent compatibility with biological tissues. However, their application in stable and long-term monitoring, particularly in vivo, has been hindered by structural instability and inconsistent performance stemming from conventional fabrication approaches based on surface functionalization. Here, a novel co-extrusion strategy is presented to enable continuous fabrication of highly stable and performance-consistent fiber electrochemical sensors, through co-extruding sensing active materials with poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) suspension. Utilizing this strategy, a series of co-extruded fiber sensors (EFSs) tailored for versatile biochemical sensing, including hydrogen peroxide (H 2 O 2 ), ascorbic acid (AA), and glucose are developed. Benefiting from the uniform embedding of active materials within interpenetrating conductive polymer networks, the EFSs exhibited robust structural integrity and functional stability under complex dynamic conditions (e.g., cyclic bending and friction) and prolonged liquid immersion, along with highly consistent performance with deviations < 5%. Furthermore, after implantation in mice, the EFSs demonstrated stable subcutaneous monitoring of H 2 O 2 under dynamic biological environments and continuous intracerebral monitoring of AA over 14 days. This co-extrusion strategy offers a promising pathway for the scalable fabrication of high-performance fiber electrochemical sensors and other bioelectronic devices with exceptional stability and consistency.
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JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Zhaoqian Zhang,Shaopeng Xin,Qiaoxia Hu,Yunxia Hu
Proteins have emerged as promising materials to fabricate advanced separation membranes due to natural abundance, high biocompatibility, and precisely defined molecular structures. However, existing studies have primarily focused on enhancing membrane performance using proteins, with limited investigation into the mechanism of membrane-formation and structure-performance relationship of protein-based membranes. In this study, lysozyme (Lyz) and hemoglobin (BHb) were co-assembled to construct defect-free, tunable nanofiltration membranes with sub-10 nm pore sizes. The assembly behaviors in solutions, on solid substrates and on porous substrates were investigated. It is demonstrated that the membrane formation is predominantly governed by interface-induced planar growth of protein assembled nanofilms. The BHb electrostatically interacts with Lyz to tailor the pore structure of the protein assembled nanofilm, ultimately leading to the formation of programmable Lyz/BHb membranes. Furthermore, systematic optimization of key parameters including protein concentration and pH enables precise control over structure and performance of membranes. The protein membrane without defects and nanoparticles could be created by protein co-assembly with short time and multi-layer growth. The resulting Lyz/BHb membranes exhibit exceptional tunability in nanometer, with pore sizes at 1.4–6.0 nm and water permeance varying from 39 to 310 L⸱m −2 ⸱h −1 ⸱bar −1 . These protein-based membranes demonstrate high efficiency in diverse separation tasks, including protein retention, dye recovery, and antibiotic removal. This work provides a versatile and simple method for tailoring properties of protein-based membranes, offering promising opportunities for the development of customized separation membranes for various industrial and environmental applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Liwu Qiang,Xuemin Yang,He Xiao,Peipei Zhao,Qinyun Yan,Wei Wen,Chunmei Liu,Qilin Guo,Yanxia Zhang,Man Zhao,Jianfeng Jia
Electrolytic water splitting for hydrogen production is considered as one of the promising directions due to its environmental friendliness and high generated hydrogen purity. To address the high overpotential caused by the sluggish kinetics of the oxygen evolution reaction (OER), a modified four-electrode system has been designed to synthesize bifunctional PtCo/graphene (PtCo/G) composites, which feature dual active sites. This method allows for the electrolysis of Pt at a high voltage (30 V) and Co at a lower voltage (10 V), while graphene is prepared through the exfoliation of graphite sheets at the cathode. This process concurrently resolves the issues of differential dissolution voltages between Pt and Co and the poor conductivity of the material, achieving the efficient synthesis of metal/graphene composites. The PtCo/G-2h composite exhibits excellent electrocatalytic activity. In the 0.5 M H 2 SO 4 , the overpotential for hydrogen evolution reaction (HER) at 10 mA cm −2 is 18 mV lower than that of commercial Pt/C catalyst. In 1 M KOH, PtCo/G-2h demonstrates superior electrocatalytic OER activity, with an overpotential at 10 mA cm −2 that is only 2 mV higher than that of the commercial RuO 2 catalyst. As a bifunctional catalyst for water electrolysis, the PtCo/G composites can effectively facilitate the adsorption of OH − ions, and assist in altering the rate-determining step, thus significantly reducing the activation energy (E a ) of the reaction. This work introduces a novel approach for the synthesis of graphene-based materials using a self-designed electrochemical method.
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JOURNAL OF MEDICINAL CHEMISTRY
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2025
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IF 6.8
Qing-Hua Shen,Long-Bo Yu,Shan-Ming Yao,Zhi-Yuan Li,Qi-Qi Zhang,Peng Wang,Cai-Ping Tan
Metalloenzyme mimics based on small molecules are valuable therapeutic candidates, but there are few reports on their mechanism of action. Inspired by natural enzymes, we designed two Cu–Fe bimetallic multienzyme mimetics (CuFc1 and CuFc2). Due to the coordination of the bimetallic centers, CuFc1 exhibits mimetic activities for multiple enzymes, including peroxidase (POD), catalase (CAT), superoxide dismutase (SOD), and glutathione oxidase (GSHOx). CuFc1 can catalyze cascade reactions from •O2– and H2O2 to O2 and •OH, which leads to a storm of reactive oxygen species and causes cuproptosis and ferroptosis in cancer cells simultaneously. As CuFc1 treatment upregulates the expression of PD-L1, it acts synergistically with the PD-L1 inhibitor (BMS-1) to remodel the tumor immune microenvironments and stimulates intense anticancer immune responses in vivo. In summary, through reasonable molecular design, we first demonstrate the enormous potential of metallo small molecule-based multienzyme mimics in cancer immunotherapy.
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FOOD CHEMISTRY
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2025
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IF 9.8
Rongmi Zhou,Fangfang Ni,Shiyi Wu,Xinyu Wang,Jing Ming,Lantong Zhang,Lijuan Dong,Zhijun Song,Gerui Ren,Min Huang,Shuangbin Xu,Qiong Zhang,Khaled F. El-Massry,Hujun Xie
Lactobacillus plantarum (LP) and curcumin (CUR) were co-encapsulated in sodium alginate– Lactobacillus plantarum– curcumin–gelatin (ALG–LP–CUR–GE) hydrogel beads to evaluate the synergistic function of probiotics and prebiotics. The encapsulation efficiency of LP and CUR peaked at 84.6 % and 94.7 %, respectively. Results of scanning electron microscope, Fourier transform infrared spectrometry, and X-ray diffraction confirmed the encapsulation of LP and CUR in the hydrogel beads. In vitro digestion suggested that both CUR and LP can achieve successful release in the simulated intestinal fluid. The release kinetics of CUR showed that it exhibited predominantly Fickian release and non-Fickian release in gastric fluid and intestinal fluid, respectively. The application of co-encapsulated hydrogel beads in mimic milk tea illustrated that the viable count of LP remained above the minimum recommended threshold of 10 7 CFU/mL, offering a promising avenue for the delivery of synergistic probiotic and prebiotic functionalities.
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高影响因子
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