Nature Communications
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2024
·Vol. 15
·期 1
·1-10
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IF 14.7
Lin Xinyu,Hao Yue,Gong Yanjun,Zhou Peng,Ma Dongge,Liu Zhonghuan,Sun Yuming,Sun Hongyang,Chen Yahui,Jia Shuhan,Li Wanhe,Guo Chengqi,Zhou Yiying,Huo Pengwei,Yan Yan,Ma Wanhong,Yuan Shouqi,Zhao Jincai
Direct solar-to-hydrogen conversion from pure water using all-organic heterogeneous catalysts remains elusive. The challenges are twofold: (i) full-band low-frequent photons in the solar spectrum cannot be harnessed into a unified S 1 excited state for water-splitting based on the common Kasha-allowed S 0 → S 1 excitation; (ii) the H + → H 2 evolution suffers the high overpotential on pristine organic surfaces. Here, we report an organic molecular crystal nanobelt through the self-assembly of spin-one open-shell perylene diimide diradical anions (:PDI 2- ) and their tautomeric spin-zero closed-shell quinoid isomers (PDI 2- ). The self-assembled :PDI 2- /PDI 2- crystal nanobelt alters the spin-dependent excitation evolution, leading to spin-allowed S 0 S 1 → 1 (TT) → T 1 + T 1 singlet fission under visible-light (420 nm~700 nm) and a spin-forbidden S 0 → T 1 transition under near-infrared (700 nm~1100 nm) within spin-hybrid chromophores. With a triplet-triplet annihilation upconversion, a newly formed S 1 excited state on the diradical-quinoid hybrid induces the H + reduction through a favorable hydrophilic diradical-mediated electron transfer, which enables simultaneous H 2 and O 2 production from pure water with an average apparent quantum yield over 1.5% under the visible to near-infrared solar spectrum.
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Materials Horizons
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2025
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IF 10.7
Linlin Zhao,Meiyu Hu,Xiaohang Yin,Hao Yang,Liyun Zhu,Pingyuan Sun,Xiya Wang,Songwei Ai,Yonghui Zheng,Genjie Li,Tingting Yang,Xuerui Chen,Jingyu Zhang
Effectively alleviating cerebral ischemia-reperfusion (I/R) injury is challenging despite medical advances. Prompt restoration of blood flow after ischemic stroke causes secondary damage to brain tissue, triggers neuroinflammation and overproduces reactive oxygen species (ROS). MiRNA regulates genes involved in neuron apoptosis and neuroinflammation, thus exhibiting potential in ameliorating cerebral I/R injury. However, as miRNA is vulnerable to degradation, its effective delivery poses obstacles to clinical applications. Inspired by therapeutic potential of miR-210 inhibitors in ischemic stroke-induced neuroinflammation, we constructed a multifunctional nanosystem composed of ceria nanozymes and zeolitic imidazolate framework-90 (ZIF-90) nanoparticles to deliver miR-210 inhibitors to treat cerebral I/R injury. Attributed to proton sponge effect of ZIF-90, this nanosystem allows for lysosome escape of miR-210 inhibitors to protect their intracellular bioactivity, while integration of ZIF-90 and ceria nanozymes utilizes multi-enzyme cascade activities to constrain lipid peroxidation and reduce oxidative damage in brain tissues of mice with middle cerebral artery occlusion (MCAO). After crossing the blood-brain barrier, miR-210 inhibitors target TET2 to suppress pro-inflammatory cytokines, finally inhibiting neuroinflammation. More than uncertain stability and efficacy of direct TET2 protein administration, delivery of miR-210 inhibitors by multifunctional nanosystems engendered neuroprotection, indicating their potential for protein replacement therapy against cerebral I/R injury.
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EUROPEAN POLYMER JOURNAL
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2025
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IF 6.3
Chi Zhang,Zixuan Lei,Yuhong Liu
Mechanical properties of thermosetting polymers are intricately linked to the heterogeneity of cross-linked network structures, particularly in balancing strength and toughness. To tackle this trade-off, this work presents how the cross-linking and heterogeneous network influence the viscoelastic and mechanical behaviors of polybenzoxazine (PBZ) resins via tuning cross-linked bonding modes and network topologies. A novel epoxy resin bearing Si-O-Si flexible groups (ES) with different pre-polymerization conversions was incorporated into PBZ cross-linking network. Utilizing imidazole as both a catalyst and curing agent, three network topologies of P(BZ-PESI X ) blends were fabricated via the specific curing cycles. Note that the ratio of thermal and catalytic curing units for three network topologies increased and then dropped as the PESI conversions increased from PESI 0 to PESI 100 . It was found that the chemical reactions involving functional groups, active sites and end groups from free, dangling, and unequal length chains can be significantly enhanced by thermal curing at high temperature ranges. This resulted in a decrease in heterogeneity of the cross-linked network. For cross-linked copolymer networks topology (P(BZ-PESI 40 )), the flexural strength, impact strength and K IC were 26.6 %, 36.7 % and 193.5 % higher than that of neat PBZI respectively. Meanwhile, a significant increase in cross-linking density and storage modulus was observed. It was confirmed that the strengthening and toughening mechanism of resins can be summarized as the synergistic effect of reduced network heterogeneity, plastic deformation effect of Si-O-Si flexible chain segments, and weakened hydrogen-bonding interactions. These insights offer practical and economic prospects for the development of versatile, high-performance thermosetting materials.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yuqing Wang,Miao Jiang,Na Liu,Tian Tian,Changdao Li,Zhao Sun,Gewen Yu,Yanming Wang,Wenxiu He,Jian Ding,Li Yan,Yunjie Ding
Designing low-cost and highly efficient heterogeneous catalysts for olefin hydroformylation, particularly utilizing abundant internal olefins, represents a research area of considerable scientific and industrial significance. Herein, a series of N or P doped porous organic polymers (POPs-N&P) are designed and fabricated to serve as carriers by the solvothermal polymerization of vinyl functionalized amine-type N, pyridinic N, imidazole N and PPh 3 ligands. The microenvironments surrounding cobalt were effectively regulated in Co/POPs-N&P catalysts. Specifically, single atom Co/POPs-NPh 3 catalyst with amine-type N chemical configurations possesses superior olefins isomerization abilities, thereby presenting an excellent 2-octene conversion of 95.9 % with the oxygenates selectivity of 62.6 % and a turnover number of 561, outperforming most of heterogeneous cobalt-based catalysts reported to date. Experimental results verify that distinct electronic environment of Co sites lead to different olefins isomerization abilities. Abundant Co N active species are generated on the Co/POPs-NPh 3 catalyst, which are different with those active species produced on the Co/POPs-PPh 3 , Co/POPs-Im&DVB and Co/POPs-Py&DVB catalysts. Furthermore, a reaction mechanism was also suggested for 2-octene hydroformylation over the Co/POPs-NPh 3 catalyst. This work underlines the potential of POPs as an ideal platform for the modulation of the coordination environment of the Co sites toward improved hydroformylation of internal alkenes.
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Carbon Capture Science & Technology
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2025
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IF 10.5
Dudu Li,Zhifang He,Ying Chen,Zelong Xu,Zibo Yang,Hao Zhang,Zhihua Qiao
Carbon nanotubes (CNTs), known for their elevated specific surface area, exemplary mechanical properties and thermal stability, are regarded as optimal reinforcing fillers for the fabrication of mixed matrix membranes (MMMs). In this study, self-supported MMMs were prepared using melted zeolitic imidazolate framework (ZIF), denoted ZIF-62 glass, as the continuous phase and multi-walled CNTs (MWCNTs) particles as the dispersed phase. The resulting membranes were thoroughly characterized, and the effect of different incorporation amounts of MWCNTs on the gas separation performance was investigated. It is noteworthy that at an incorporation amount of 4 wt. % MWCNTs, the ideal selectivity of prepared self-supported ( a g ZIF-62) 0.96 (MWCNTs) 0.04 MMM for CO 2 /N 2 and CH 4 /N 2 was 31.2 and 8.6 respectively, exceeding the 2019 Robeson upper bound. The results demonstrated that MWCNTs have excellent gas transport properties and significantly enhance the separation performance. Furthermore, the self-supported ( a g ZIF-62) 0.96 (MWCNTs) 0.04 MMM also exhibited excellent mechanical properties and pressure resistance, making them highly promising candidates for advanced gas separation applications. This study not only highlights the effectiveness of MWCNTs as functional fillers in MMMs but also presents a novel approach for designing high-performance gas separation membranes.
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Carbon Capture Science & Technology
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2024
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IF 10.4
Ming Jiang,Xintong Zhang,Mi Feng,Shijie Wang,Zhencai Zhang,Xiangping Zhang,Xingmei Lu,Fei Xu
Using CO 2 -derived dimethyl carbonate (DMC) instead of diphenyl carbonate (DPC) as a carbonyl source for synthesizing bio-based polycarbonates is a green and cost-effective route. However, the synthesis of high-performance polycarbonates via the DMC route remains challenging due to the poor reactivity and selectivity of DMC compared to DPC. Herein, we designed a series of highly active protic ionic liquid (PIL) catalysts for the synthesis of poly(isosorbide carbonate) (PIC) from DMC with ISB. The influences of the structures of anion and cation on the catalytic activity of PILs were systematically studied. Compared with the reported aprotic IL catalysts, the unique reactive hydrogen of the cation in PILs could form a strong hydrogen bond interaction with the carbonyl group of DMC, resulting in higher reactivity of the carbonyl carbon of DMC. Moreover, the nucleophilicity of the anion could be easily tuned by adjusting the p K a value, which effectively realized the balance of the reactivity difference between exo -OH and endo -OH in ISB. Among them, [DBUH][Im] showed the highest catalytic activity, and the weight-average molecular weight ( M w ) and glass transition temperature of PIC reached 55,700 g/mol and 160 °C, respectively. Combined with NMR analyses and DFT calculations, the mechanism that exhibited the synergetic catalytic effect of anion-cation for the polymerization of DMC and ISB was presented.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuhang Ren,Yu Tian,Yating Lu,Dongyu Nie,Huayi Zhu,Xia Yang
Malathion (MA) is a widely used organophosphorus pesticide globally. Developing efficient photocatalysts is crucial for eliminating MA pollution in water by photocatalytic technology. This study focuses on preparing a series of H-PDI supermolecule/NH 2 -MIL-101(Fe) (PM) materials by amidating NH 2 -MIL-101(Fe) with the more stable H-PDI supermolecule, forming a covalent O C–NH bond. Among these materials, 40 %PM (indicating a mass percentage content of 40 % H-PDI supermolecule in PM) exhibited the best performance for degradation of MA. Under simulated sunlight irradiation of a 10 mg·L 1 MA solution for 180 min, the reaction rate constants of 40 %PM were 5.95 times and 3.13 times higher than those of NH 2 -MIL-101(Fe) and H-PDI supermolecule, respectively. The enhanced performance is attributed to the formation of Z-scheme heterojunctions in the 40 %PM composite lead to fast separation of photogenerated e − and h + . Combining the results of HPLC-MS with Fukui Function, the HOMO, LUMO, and pathway of degradation of MA attracted by 1 O 2 , •OH, and h + were speculated. The pathway involves oxidation, demethylation, P-S bond breakage, decarboxylation, and final conversion to some inorganic molecules. The toxicity of the degradation byproducts were lower than that of MA estimated by Toxicity Estimation Software Tool.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Ke Xiang,Shaoyi Wu,Tiefeng Xu,Wangyang Lu
The photocatalysis-assisted peroxymonosulfate (PMS) activation process has shown great potential for organic wastewater treatment. Herein, the composite photocatalyst (FeTAPc/PDI/CN) was obtained by grafting graphitic carbon nitride (CN) and amino iron phthalocyanine (FeTAPc) onto both ends of perylene tetracarboxylic anhydride (PTCDA) through an imidization process. Under simulated solar irradiation, the catalyst exhibited a remarkable degradation performance toward the target pollutant by activated PMS over a wide pH range from 3 to 11. The degradation efficiency of SMX reached 100 % in 7 min with the reaction kinetic constant of 0.845 min −1 , which was 13 times higher than that of pure CN. In addition, the removal rate of FeTAPc/PDI/CN-4 for SMX was more than 80 % after 9 cycles. The introduction of phthalocyanine and PDI improved the separation efficiency of photogenerated electron-hole pairs. Furthermore, the active species involved in the SMX degradation were identified as •OH, SO 4 • - , •O 2 – and 1 O 2 . The possible degradation pathways were proposed based on the identified intermediates, in which the oxidation of the amino group on the benzene ring was the main degradation pathway. This study is anticipated to result in a favorable method for designing CN-based photocatalysts with high stability and excellent catalytic activity for environmental remediation.
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MICROCHIMICA ACTA
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2024
·Vol. 191
·期 9
·1-10
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IF 5.3
Zhai Xiurong,Li Qian,Cao Yang,Han Mengjie,Sun Hailian,Du Lelin,Yang Xiyun,Wei Yuxin,Yu Congcong
An electrochemical platform for signal amplification probing chloride ions (Cl − ) is constructed by the composite integrating core–shell structured nitrogen-doped porous carbon@Ag-based metal–organic frameworks (NC@Ag-MOF) with polypyrrole (PPy). It is based on the signal of solid-state AgCl derived from Ag-MOF, since both NC and PPy have good electrical conductivity and promote the electron transport capacity of solid-state AgCl. NC@Ag-MOF was firstly synthesized with NC as the scaffold and then, PPy was anchored on NC@Ag-MOF by chemical polymerization. The composite NC@Ag-MOF-PPy was utilized to modify the electrode, which exhibited a higher peak current and lower peak potential during Ag oxidation compared with those of Ag-MOF and NC@Ag-MOF-modified electrodes. More importantly, in the coexistence of chloride (Cl − ) ions in solution, the NC@Ag-MOF-PPy-modified electrode displayed a fairly stable and sharp peak of solid-state AgCl with the peak potentials gradually approaching zero, which might effectively overcome the background interference caused by electroactive substances. The oxidation peak currents of solid-state AgCl increased linearly with the concentration of Cl − ions in a broad range of 0.15 µM–40 mM and 40–250 mM, with detection limits of 0.10 µM and 40 mM, respectively. The practical applicability for Cl − ions determination was demonstrated using human serum and urine samples. The results suggest that NC@Ag-MOF-PPy composite could be a promising candidate for the construction of the electrochemical sensor.
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JOURNAL OF CHROMATOGRAPHY A
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2024
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IF 3.8
Can Zhang,Pingping Zhang,Wenyuan Zhu,Shuo Li,Yue Gu,Jing Wu,Di Wen,Weili Hao,Ke Wang,Ling Ma,Kaoqi Lian
Herein, a magnetic cationic Schiff base polymeric material (Fe 3 O 4 @SiO 2 - Schiff -TAPB-DA) was fabricated simply and rapidly, which was explored as a magnetic adsorbent for magnetic solid-phase extraction (MSPE) for enriching seven avermectins insecticides in surface water and milk matrices combined with ultra-high performance liquid chromatography mass spectrometry (UPLC-MS/MS). Under the optimized pretreatment and instrumental parameters, the analytes showed good linearity in the range of 0.5–200.0 ng·mL −1 with a correlation coefficient (R 2 ) greater than 0.9990 and high precision. The limits of detection for the analytes were 0.004–0.047 μg· L −1 for surface water sample and 0.008–0.250 μg·kg −1 for milk samples. Satisfactory recoveries of spiked target compounds were in the range of 82.25- 100.87 % for surface water sample and 72.73- 119.62 % for milk samples. The results indicated powerfully Fe 3 O 4 @SiO 2 - Schiff -TAPB-DA was of significant potential as an MSPE adsorbent for the detection of avermectin insecticides in surface water and milk, which provides a quick and efficient idea for enriching avermectins insecticides in complicated matrices.
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BIOSENSORS & BIOELECTRONICS
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2025
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IF 10.5
Hang Ao,Jinshan Xiong,Wencheng Xiao,Wenrui Hu,Jie Wu,Huangxian Ju
Owing to the continuous mutations of the coronavirus, the sensitive and accurate detection of the SARS-CoV-2 nucleocapsid protein is still necessary in clinical diagnosis. Aim to the challenge of sensitivity in chemiluminescence (CL) imaging detection and the need for high-throughput clinical screening, this work used imidazole (Im) as an enhancer for hemin-DNA/luminol/H 2 O 2 CL system to propose a CL imaging method for SARS-CoV-2 nucleocapsid protein detection. In this system Im could reduce the hemin-DNA catalyzed oxidation energy of luminol by H 2 O 2 to promote the CL emission through the accelerated breaking of O-O bond of dianionic cyclic peroxide. The enhancement mechanism was demonstrated with theoretical calculations and several characterization techniques. By combining the proximity-induced initiator release with immunological recognition, an initiator-triggered DNA nanomachine was designed to achieve the release of abundant primers for activating hemin-DNA switch. This signal amplification strategy led to strong CL emission for highly sensitive imaging detection of the target. The Im-enhanced hemin-DNA/luminol/H 2 O 2 CL imaging assay exhibited a linear detection range over 4 orders of magnitude with a detection limit down to 2.75 pg/mL for SARS-CoV-2 nucleocapsid protein, exhibiting promising potential of both Im sensitization and the proposed DNA nanomachine to improve the sensitivity of high-throughput CL biosensing for the early diagnosis and clinical screening of the coronavirus and other diseases.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yixin Pan,Bo Sun,Yingying Zhou,Jian Jiao,Liping Deng,Xiaowu Dong
This study reported a Ni 0 @ZIF-8 nanocomposite synthesized via co-precipitation that synergistically integrated the high adsorption capacity of ZIF-8 with the redox activity of zero-valent nickel (Ni 0 ) for efficient uranium(VI) extraction. The composite with an optimized 1:1 ZIF-8:Ni 0 molar ratio achieved an exceptional adsorption capacity of 830.5 mg/g. Kinetic and thermodynamic analyses confirmed chemisorption-dominated monolayer adsorption following pseudo-second-order kinetics (R 2 > 0.999) and spontaneous endothermic behavior. Mechanistic investigations through spectroscopy and density functional theory (DFT) calculations revealed a dual-function mechanism that ZIF-8 facilitated U(VI) capture through electrostatic/coordination interactions, while Ni 0 mediated partial reduction of U(VI) to U(IV) via electron transfer, enhancing immobilization stability. Notably, only Pb 2+ , Cu 2+ , Cr 6+ , and organic ligands inhibited adsorption through redox competition and solution complexation. Comparative studies demonstrated minimal matrix interference-deionized water versus seawater systems exhibit merely 4.7 % deviation in adsorption efficiency at trace U(VI) concentrations (0.1–0.6 mg/L). Critically, direct uranium extraction from unprocessed natural seawater (ambient U: 4.27 μg/L) with only pH adjustment (5.0) achieves 86.02 % efficiency at ultra-low adsorbent dosage (0.001 g/L), yielding residual uranium concentrations of 0.597 ± 0.04 μg/L. By harmonizing adsorption and redox pathways, Ni 0 @ZIF-8 overcome limitations of conventional materials, establishing itself as a paradigm-shifting solution for uranium remediation in complex ionic matrices and real marine environments.
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