Journal of Water Process Engineering
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2026
·
IF 6.6
Kudakwashe Meki,Shiyu Meng,Zihao Liu,Zhuowen Wang,Baojian Jing,Huiqun Zhang,Peng Liu,Shan Qiu
DMS gradient improves micropore access and O₂ transport, reducing flooding. • CB-DV06 yields 750 mg L −1 H₂O₂ at >60% Electro-Fenton efficiency. • DMS-modified GDEs remove 85% RBB and reduce TOC 60% in 120 min. • Surface area reaches 222.9 m 2 /g; electroactive sites increase sixfold. • Dual-phase oxygen diffusion boosts ORR kinetics and degradation rate. Hydrogen peroxide (H₂O₂) electrosynthesis via the two-electron oxygen reduction reaction (2e − ORR) is critically dependent on the formation of stable and well-regulated triple-phase interfaces (TPIs), where gas, liquid, and catalyst converge. However, micropore flooding and uneven wettability in carbon-black gas diffusion electrodes (GDEs) often hinder oxygen transport and deactivate active sites. In this work, we address these challenges by introducing a dimethyl silicone oil (DMS) volume-gradient strategy to engineer confined TPIs within the carbon catalyst layer. Carbon-black GDEs were prepared using DMS volume-controlled of 0.4, 0.6, and 1.2 mL, with CB-DV06 identified as the optimum configuration. This design balances hydrophobicity and pore accessibility, promoting sustained oxygen diffusion and suppressing water blockage without impeding electron or ion transport. The optimized GDE (CB-DV06) achieved ~750 mg L −1 H₂O₂ after 180 min with current efficiencies exceeding 60% and enhanced electrochemically active surface area. To demonstrate the practical applicability of the in situ generated H₂O₂, Reactive Black B (RBB) degradation was employed as a model pollutant-removal reaction. The integrated system achieved approximately 85% RBB decolourisation, demonstrating the applicability of this interface-engineering strategy for pollutant-removal applications. Overall, this study highlights a low-impact approach for optimizing oxygen reduction environments in porous electrodes, advancing sustainable oxidant generation and environmental remediation. Download: Download high-res image (127KB) Download: Download full-size image
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Shuai Han,Cai Xu,Jun Li,Jia Guo,Jianhai Yang,Xiaozhong Wang,Liyan Dai
The selective C−H bond oxidation of toluene to benzaldehyde using molecular O2 with non-noble metal catalysts is challenging but desirable. Herein, a series of high-entropy oxides (FeCoNiCrMn)3O4 supported on mesoporous N-doped carbon was fabricated via a reverse impregnation and calcination method (denoted as HEOs@NC). It was found that high-entropy oxides (FeCoNiCrMn)3O4 nanoparticles were distributed well onto the surface of N-doped carbon, and a distinct interface between them was observed, contributing to the formation of metal-support electronic interaction. XPS and Bader charge results verified that an electron was transferred from (FeCoNiCrMn)3O4 to N-doped carbon. Under the optimized reaction conditions, 12.2% of toluene conversion and 2.0 ×10−4 mmol mg−1cat. h−1 of benzaldehyde formation rate could be obtained with 1.5HEOs@NC catalyst. Moreover, DFT calculations revealed that the supported (FeCoNiCrMn)3O4 displayed stronger adsorption ability toward N-hydroxyphthalimide, and the formation of *PhCH2OH was determined as the rate-determining step. A lower energy barrier was achieved over the supported HEOs owing to the interfacial interaction between (FeCoNiCrMn)3O4 and N-doped carbon. This work developed a supported high-entropy oxides catalyst by rational design of interfacial engineering for the aerobic C−H bond oxidation of toluene.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2026
·Vol. 40
·期 10
·e70655
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IF 4.3
Xiaoju Liu,Sunqiu Fan,Shijin Hu,Zeyu Ye,Xiaoyan Ma,Guoxiong Wang,Xiangrong Ma
Two novel trinuclear ferrocenyl coordination compounds, Fc 3 N 4 /Fe and Fc 3 N 4 /Co, were synthesized as burning-rate catalysts for ammonium perchlorate (AP). The trinuclear architecture, featuring a nitrogen-rich ligand bridging three ferrocene units with transition metal centers, was designed to enhance multi-site electron transfer and thereby promote catalytic performance. At 3 wt% loading, Fc 3 N 4 /Co reduced AP's high-temperature decomposition temperature by 126°C, decreased the apparent activation energy by 74.0 kJ · mol −1 , and increased heat release by 718 J · g −1 , outperforming the corresponding mononuclear analogues and commercial binuclear ferrocene catalysts. Structural characterization (XRD, BET, XPS) and DFT calculations suggest that the superior catalytic activity arises from synergistic Co–Fe electronic modulation that facilitates N–H and Cl–O bond activation, together with a high specific surface area (310.6 m 2 · g −1 ) that provides abundant active sites. This work establishes trinuclear ferrocenyl coordination compounds as a promising platform for high-performance burning-rate catalysts in composite solid propellants.
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NANO
·
2026
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IF 1.3
Weifeng Chen,Dandan Han,Zhiwei Huang,Xuan Tian,Ting Xiao,Yizhu Lei
Ice accretion severely compromises infrastructure safety and efficiency. While integrating photothermal function with superhydrophobicity offers a promising solution, achieving this synergy within a mechanically robust coating remains challenging. Herein, we present a superhydrophobic nanocomposite coating fabricated by embedding multi-walled carbon nanotubes (MWCNTs) and hydrophobic silica (H-SiO 2 ) in an organosilicon polymer (OSP) matrix. The OSP/MWCNT/H-SiO 2 coating exhibits good mechanical durability, maintaining superhydrophobicity after severe water and sand impact, owing to the reinforced composite structure. Crucially, the design yields a remarkable photothermal conversion efficiency, achieving a temperature rise of 85 °C under 1.0 kW·m −2 irradiation. This photothermalsuperhydrophobic synergy enables outstanding anti-icing performance, delaying ice formation for over 578 s at -20 °C, and efficient solar-driven de-icing (complete melting within 462 s). Successfully demonstrated on insulators, our coating offers a viable dualfunctional platform to address icing challenges in practical settings.
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FOOD CHEMISTRY
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2026
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IF 10.4
Qian Zhou,Ran Feng,Chen-Chen Wang,Si-Jie Wu,Qiu-Ya Ji,Ran Meng,Bao Zhang
Nanoparticles are successfully constructed by a green H₂O₂ oxidation strategy. • Formation entails EGCG oxidation, Mannich cross-linking and H-bonding/π-π stacking. • Nanoparticles show excellent antioxidant activity and enhanced stability. • The greater the number of hydroxyl groups, the stronger the interaction force. This study developed a green, carrier-free EGCG-flavonoid nanoparticle assembly strategy driven by H₂O₂. This approach overcomes the drawbacks of traditional formaldehyde-induced methods, including solvent toxicity and poor biocompatibility. It further investigated how the number of flavonoid hydroxyl groups regulates the assembly process and properties of EGCG-flavonoid nanoparticles. The formation involves H₂O₂-mediated oxidation of EGCG hydroxyl groups to generate aldehyde and carboxyl groups, which then undergo covalent bonding with the amino group of glycine. Flavonoids are embedded into the EGCG–glycine network through noncovalent interactions, resulting in spherical nanoparticles (200–260 nm, PDI ≈ 0.3). Increasing hydroxyl groups on flavonoids enhanced their loading capacity and interaction with EGCG. Nanoparticles with polyhydroxylated flavonoids exhibited strong antioxidant activity (>85% DPPH•/ABTS• + scavenging), high storage stability (>70% retention after 60 days), and improved thermal stability. This work provides a theoretical foundation for green synthesis of polyphenol-flavonoid nanosystems in functional foods and targeted delivery. Download: Download high-res image (114KB) Download: Download full-size image
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PubMed
高影响因子
Vaccines
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2026
·Vol. 14
·期 7
·581
·
IF 3.5
Ren Yang,Xiaohong Wu,Xiaowei Zhang,Shengqing Fu,Kaiping Gu,Zhe Lv,Xiaoli Li,Qunying Mao
Background:The m7G cap structure, which mimics the natural cap of eukaryotic mRNA, is a critical determinant of mRNA vaccine efficacy, safety, and stability. However, its precise quantification remains challenging due to complex impurity profiles and the high physicochemical similarity between the target cap and related impurities. Although liquid chromatography mass spectrometry (LC-MS) is widely employed for this purpose, current methodologies still face significant limitations, including labor-intensive sample preparation, low analytical throughput, poor reproducibility in quantifying low-level impurities, and a lack of universally applicable strategies across diverse mRNA vaccine platforms.Methods: We systematically optimized sample preparation and LC-MS detection workflows. RNase H-mediated cleavage was compared with DNAzymes, guide DNA probes were rationally designed, and thermostable RNase H was introduced for one-step denaturation and cleavage. To establish an accurate, efficient, and universal sample preparation workflow. Chromatographic conditions were optimized using an ion-pairing reagent system to suppress ESI-MS metal adducts. Eliminating sample purification improves recovery, reduces manual handling errors, and boosts assay efficiency.Results: Through optimally designed guide DNA probes, RNase H cleavage specificity reached ≥98% with high cleavage efficiency, offering higher efficiency than DNAzyme. Furthermore, the incorporation of thermostable RNase H enabled a single-step workflow combining high-temperature denaturation and site-specific cleavage, substantially streamlining sample preparation. On the chromatographic side, optimization of the ion-pairing reagent system effectively suppressed metal adduct formation in electrospray ionization mass spectrometry (ESI-MS). This advancement enabled direct injection of the 5′ cap fragments without purification, achieving high-recovery quantification while demonstrating broad compatibility across mainstream LC-MS platforms. The optimized assay reduces the total analytical workflow from 4~6 h to under 1.5 h.Conclusions:Combining high accuracy, robustness, and broad platform compatibility, this method offers a universal, high-throughput analytical solution for mRNA vaccine quality control and continuous process development.
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Green Carbon
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2026
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IF 14.2
Shihao Li,Xiaoyang Yue,Fei Huang,Qian Zhang,Xiao Huang,Jingjing Zhao,Luwei Bao,Yanjun Jiang
Unspecific peroxygenases (UPOs) enable the selective hydroxylation of inert C–H bonds using H 2 O 2 under mild conditions. However, their practical application is fundamentally limited by oxidative deactivation at elevated H 2 O 2 concentrations. Herein, a highly synergistic photobiocatalytic system is constructed by covalently immobilizing UPOs onto a Rh-complex-coordinated covalent organic framework (COF) to facilitate the in-situ generation of H 2 O 2 and sequential enzymatic utilization. Specifically, a COF featuring a pyridinic imine structure (COF PyIm ) is designed to precisely anchor Rh(III) complexes. Compared with its bipyridine-structured analog (COF Bpy ), COF PyIm provides more coordination sites and a shorter electron-transfer distance. Consequently, the photocatalytic H 2 O 2 synthesis rate reached 22.17 mM·g -1 ·h -1 , representing a performance improvement of approximately 40%. This enhancement is attributed to the optimized pyridine–imine coordination microenvironment, which promotes charge separation and electron transfer. Subsequently, UPO from Agrocybe aegerita ( Aae UPO) is covalently immobilized onto COF PyIm to yield Aae UPO@Rh-COF PyIm , which achieves efficient spatiotemporal coupling between in situ H 2 O 2 generation and enzymatic hydroxylation of the C–H bond. This integrated photobiocatalyst can achieve 90% yield, >99% enantiomeric excess ( ee ), and a turnover number of 41,666 in the asymmetric hydroxylation of ethylbenzene. It also exhibits excellent reusability (retaining 70.4% of its initial activity after six cycles) and broad substrate scope.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Qunfang Lin,Zeyang Li,Zeyuan Zhang,Zhikang Chen,Changxi Yu,Siguo Xiao,Kailing Sun,Tongye Wei
Aqueous aluminum–ion batteries (AAIBs) have attracted considerable attention owing to their high theoretical capacity, high safety, and low cost. However, as a strong Lewis acid, Al 3+ readily coordinates with the lone–pair electrons of water molecules, which significantly polarizes the O H bonds and promotes water dissociation and proton generation. The generated protons can cause severe corrosion of electrode materials, thereby limiting cycling stability and hindering practical applications. In this work, a novel manganese oxide cathode with a hollow hexagonal pyramidal layered nanostructure is successfully synthesized and coupled with 1 M Al₂(SO₄)₃ electrolyte containing 0.06 M K₂SO₄. In situ and ex situ characterizations reveal that the cathode delivers high capacity through a synergistic Al 3+ /H + co–intercalation and deintercalation mechanism. Importantly, the introduction of potassium sulfate induces the formation of a potassium aluminum sulfate passivation layer, which effectively suppresses acid−induced electrode corrosion and enhances cycling stability. As a result, the assembled battery achieves a high specific capacity of 354 mAh g −1 at 0.2 A g −1 and a high discharge voltage plateau of 1.7 V . At 0.5 A g −1 , it maintains 90% of its capacity (based on a maximum activated capacity of 188 mAh g −1 ) over 420 cycles. This work provides a facile and effective strategy for developing high–performance aqueous aluminum–ion batteries.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Qunhua Zhong,Yimeng Zhou,Tianle Ren,Jianjun Zhu,Di Li,Deli Jiang
Abstract Photocatalytic CO2 reduction to carbonaceous fuels is a promising strategy to mitigate massive carbon emissions, yet the highly selective CO2 conversion remains challenging due to the unsatisfactory charge separation and limited active sites of pristine semiconductor photocatalysts. Herein, we report the in situ fabrication of oxygen vacancy rich W/H co-doped rutile TiO2 (W/H-TiO2) via a two-step wet chemical approach for high-efficiency photocatalytic CO2 reduction to CO. The optimized W/H-TiO2 exhibited high activity and selectivity for the photocatalytic reduction of CO2 to CO (57.96 μmol g–1 h–1 and 96.3%), which were significantly higher than those of other TiO2 counterparts. Experimental characterizations and density functional theory (DFT) calculations reveal that the synergistic effect of H/W co-doping accelerates the migration and separation of photogenerated charge carriers and reduces the formation energy barrier for the key *COOH intermediate, thereby markedly boosting the CO2 photoreduction activity and product selectivity of W/H-TiO2. This work establishes a dual-doping-induced oxygen vacancy strategy for electronic structure engineering, providing a new paradigm for the rational design of high-performance TiO2 based photocatalysts toward efficient CO2 photoreduction.
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高影响因子
IONICS
·
2025
·
IF 2.6
Yong Daming,Kang Xiaomeng,Yin Ming,Wu Qichao
First, a spherical Fe 3 O 4 was synthesized using the hydrothermal method, and subsequently coated with carbon to form a core–shell C/Fe 3 O 4 composite. The Fe 3 O 4 core was then dissolved in an etching solution to create a hollow carbon (H-C) structure. This H-C served as a substrate onto which a Fe 3 O 4 layer was deposited via the hydrothermal method, resulting in a hollow core–shell Fe 3 O 4 /C composite. Finally, the solvothermal method was employed to coat the Fe 3 O 4 /C composite with a layer of hydrogenated titanium dioxide (H-TiO 2 ), resulting in a hollow-structured H-TiO 2 /Fe 3 O 4 /C material. This structure not only ensures the formation of a dual-core shell structure, but also reduces the proportion of carbon material in the composite electrode, thereby enhancing the theoretical specific capacity of the composite electrode. The presence of H-TiO 2 and carbon improved the cyclic stability of Fe 3 O 4 within the composite. This hollow sandwich–structured composite demonstrated excellent electrochemical performance, delivering a discharge specific capacity of 629.5 mAh g −1 after 500 cycles at 0.2 A g −1 , along with a high initial coulombic efficiency of 80.6%.
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高影响因子
CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Ping Xin,Hongjiang Li,Ziwei Huang,Kexin Su,Ying-Ying Gu
To address the challenges of low selectivity and poor stability in hydrogen peroxide (H 2 O 2 ) electrosynthesis within neutral media, this study developed an O/N co -doped carbon nanotube-polytetrafluoroethylene composite cathode (designated as GF/ONCNTs-6/PTFE). Through precise control of the synergistic effects between pyrrolic-N doping (40.7 %) and carboxyl/ether functional groups, the adsorption of *OOH intermediates was significantly enhanced; simultaneously, PTFE micro-cracks were employed to establish triple-phase interfaces for facilitated oxygen diffusion. The cathode achieved a high H₂O₂ yield of 139.45 mg/L under neutral conditions (pH 7), with a current efficiency of 67.06 %, and exhibited only 8.2 % activity loss after 10 cycles. In an integrated electro-Fenton system, it accomplished 98.8 % degradation of methyl orange within 2 h under optimal conditions. This work demonstrates that defect engineering and O/N functionalization in composite cathodes significantly boost 2e − ORR efficiency, offering a promising laboratory-scale platform for electrochemical wastewater purification
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Shaohui Xiong,Xingyi Ou,Qingquan Liu,Yiwen Li,Juntao Tang,Guipeng Yu,Chunyue Pan,Shibo Guo,Sitong Li,Menghan Yong
Polymers of intrinsic microporosity (PIM) have attracted considerable attention in the development of mixed matrix membranes (MMMs) for CO 2 separation. A prominent challenge lies in engineering the spacing of the polymer matrix chains while eliminating non-selective interfacial defects. In this study, a CO 2 -philic triazine-based porous polymer, featuring robust hydrogen bond donating groups, was employed to fabricate a series of interfacial defect-free PIM-1 based MMMs (denoted as PIM-1/CSU-1). The interfacial adhesion and compatibility have been greatly improved due to the strengthened hydrogen bond interaction, which was systematically validated through variable-temperature infrared spectroscopy. Additionally, the formation of hydrogen bonds allowed for the regulation of the polymer matrix chain spacing, making the chain distance loose. Remarkably, the resulting membrane exhibited a CO 2 permeability of 13,429 Barrer and CO 2 /N 2 selectivity of 33.1—246.6% and 70.2% higher than pristine PIM-1, respectively, surpassing the latest Jansen/McKeown upper bound established in 2019, but also significantly exceed the performance of previously reported MMMs for CO 2 separation. The strategy of mitigating interfacial defects through the formation of hydrogen bonds between fillers and the polymer matrix emerges as a viable and effective method for fabricating gas separation membranes with exceptional separation capabilities.
研究领域:
材料科学
·
高分子化学
·
气体分离
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膜技术
·
物理化学
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