NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Yafei Sang,Xiaolong Jia,Pengpeng Wu,Xiangquan Yan,Xiaotao Kuang,Quan Feng,Jiahao Qiao,Min Chen,Jian Zhang,Xiuli Yan,Tao Chang
The porous organic polymers HIP-Br-1 and HIP-Br-2 rich in bromine anions were prepared by quaternization one-pot method. The contents of N and Br in HIP-Br-1 reached 15.93 wt% and 6.94 wt% respectively. These high content of bromine ions combined with rich mesoporous and macroporous structures gave the materials good catalytic ability. The material has moderate adsorption heat (28-36 kJ/mol). The catalytic experiment shows that HIP-Br-1 has good catalytic performance. Under the mild conditions of 0.4 MPa CO2, 60 oC, and 9 h, without any cocatalyst and solvent, 93% of propylene oxide can be converted to cyclic carbonate. The catalyst has good repeatability, and the conversion efficiency to cyclic carbonate did not significantly decrease after four catalytic experiments. Density functional theory (DFT) shows that HIP-Br-1 can effectively activate PO and CO2, thereby enhancing the catalytic activity of cycloaddition reactions. This work explores the one-step synthesis of ion-type porous organic polymers rich in nitrogen atoms.
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高影响因子
MACROMOLECULES
·
2024
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IF 5.1
Dongfei Zhang,Ao Wang,Wenkai Liu,Ao Zhen,Jiehua Li,Feng Luo,Xianglong Han,Zhen Li,Hong Tan
The reported dynamic covalent bonds (DCBs) exhibit certain drawbacks, including sluggish reaction rates and high dissociation temperatures, which impede the reusability of DCBs cross-linked polymers. Herein, we develop a kind of imidazole-urea bond (IUBs) through the rapid self-catalytic reaction between imidazole and isocyanate without additional catalysts. The IUBs are found to be highly reversible via a thermally dissociative mechanism while also demonstrating an irreversible exchange with amines. Then, histamine (1H-imidazole-4-ethanamine) is first employed as a chain extender to construct IUBs in the synthesis of novel imidazole-based cross-linked polyurethane-ureas (IMCPU). The IMCPU can undergo multiple recyclings of melt processing and be aminolyzed even at room temperature. Given the wide availability of the commodity histamine, IMCPU exhibits great potential for broad applications in the fields of dynamic materials.
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LANGMUIR
·
2024
·
IF 3.7
Bizhuo Wei,Huajing Li,Huan Chu,Huanhuan Dong,Yijun Zhang,Cai-Li Sun,Yuangang Li
This work presents a study of the thermally induced aggregation of perylene diimide (PDI) and naphthalene diimide (NDI) derivatives modified with oligo ethylene glycol (OEG) chains in aqueous solution. Water-soluble and flexible OEG side chains were introduced into the π-core of glutamate-modified NDI and PDI structures, and the aggregation process was modulated by heating or cooling in water. Interestingly, a rare opposite temperature response of fluorescent behavior from the two amphiphilic chromophores was revealed, in which the PDI exhibited fluorescent enhancement, while fluorescent quenching upon temperature increase was observed from the NDI assembly. The mechanism of thermally induced aggregation is clearly explained by studies with various spectroscopic techniques including UV–visible, fluorescence, 1H NMR, 2D NMR spectroscopy, and SEM observation as well as control experiments operated in DMSO solution. It is found that although similar J-aggregates were formed by both amphiphilic chromophores in aqueous solution, the temperature response of the aggregates to temperature was opposite. The degree of PDI aggregation decreased, while that of NDI increased upon temperature rising. This research paves a valuable way for understanding the complicated supramolecular behaviors of amphiphilic chromophores.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Tao Peng,Xu Lu,Yang Jin,Xicheng Yang,Qian Liu,Chen Chen,Wanting Zhou,Yuting Guo,Yu Zhang,Yankun Gao,Hongjuan Zhang,Hongliang He,Lina Chen
It is effective through uncoupling postsynaptic density protein-95 (PSD95) and neuronal nitric oxide synthase (nNOS) for treating ischemic stroke with high disability, mortality and recurrence rate. However, there are no reliable uncouplers for PSD95-nNOS in clinical practice, and the established screening models for discovering PSD95-nNOS uncouplers have high costs and interference. In this study, epoxy functional fluorescent magnetic mesoporous silica (EFMMS) was synthesized by combining carbon dots (CDs), magnetic mesoporous silica and epoxy functionalization. Ni-EFMMS was further constructed by loading nickel ions to simultaneously purify and covalently immobilize His-tagged neuronal nitric oxide synthase (His-nNOS) and then couple with green fluorescent proteins (GFP) labeled PSD95, finally fabricating nano-biosensor (PSD95-nNOS/Ni-EFMMS). The nanomaterial was well constructed and characterized, and it distinctly constituted stable ratio fluorescence between CDs and GFP-PSD95. The ratio fluorescence intensity of PSD95-nNOS/Ni-EFMMS remained stable even after separately mixing with metal ions, amino acids and natural impurities, and the loss of ratio fluorescence intensity was less than 20% even at pH 4 or 10. PSD95-nNOS/Ni-EFMMS still kept the ratio fluorescence intensity above 90% after being recycled for seven times. Three compounds (gnetol, baicalein and emodin-8- O -β- D -glucoside) with strong uncoupling efficiency were screened from fourteen natural active ingredients. Furthermore, the theoretical feasibility of uncoupling was verified by molecular docking. In general, this study provides a novel “one-stone-four-birds strategy” to fabricate magnetic mesoporous nano-ratio fluorescence sensor for efficiently and accurately discovering PSD95-nNOS uncoupling active substances.
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JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Haiyang Shao,Zhengke Tan,Yafei Cheng,Xiang'an Yue,Lei Yuan,Weixiong Jian,Longqiang Xiao,Xiaocheng Lin
Diffusion dialysis (DD) presents a highly promising and cost-efficient approach for acid recovery, yet its performance is often hindered by the acid permeability of anion exchange membranes (AEMs). To address this challenge, a one-step approach has been developed to fabricate porous AEMs. Using brominated polyphenylene oxide (BPPO) as the porous base membrane, imidazole is employed for in-situ crosslinking and cationization. This approach not only retains the inherent porosity (>63.5 %) of the base membrane but also achieves an exceptionally thin selective layer (<0.3 μm), thereby creating abundant free space volume. Through a concurrent enhancement of ion transport sites and crosslinking density, the membrane effectively breaks acid permeability–selectivity trade-off. The optimal IPPO-20h AEM demonstrates a remarkable increase in both the acid dialysis coefficient ( U H + = 34.1 × 10 −3 m/h) and separation factor ( S H + / F e 2 + = 573.8) in the HCl/FeCl 2 system, with enhancements of 4- and 31-fold, respectively, compared to the commercial DF120 AEM, at 25 °C. This high-performance AEM, synthesized via a straightforward and mild process, offers significant potential for large-scale acid recovery applications.
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JOURNAL OF INORGANIC BIOCHEMISTRY
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2025
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IF 3.2
Hao Wang,Guozhu Ren,Yue Xu,Ruiping Deng,Rui Wang,Liang Zhou
In this work, novel erbium complex with anticancer activity against radiation resistant lung adenocarcinoma cells was obtained and demonstrated. Firstly, stronger inhibitory effect of Er 3+ on non-small cell lung cancer (NSCLC) cells and NSCLC- radiation resistant (RR) cells was experimentally confirmed. Then, by selecting highly biocompatible porphyrins as ligands, a novel erbium complex tetraphenylporphyrin erbium acetylacetonate (Er(acac)TPP) was synthesized and purified. Compared with Cisplatin, notably, Er(acac)TPP exhibits relatively higher inhibitory efficiency on NSCLC-RR cells. Moreover, the toxicities of Er(acac)TPP to normal cells are much lower than that of cancer cells. Subsequently, cell expansion, increased apoptosis, a decline in mitochondrial membrane potential (MMP), an accumulation of intracellular reactive oxygen species (ROS), increased Caspase-9 protein level and G2/M arrest were seen. These data all pointed to Er(acac)TPP as a possible candidate for more research and development as a chemotherapeutic drug.
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POLYMER INTERNATIONAL
·
2025
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IF 3.6
Liyue Zhang,Jingkai Liu,Xiaoling Liu,Jinyue Dai,Xiaoqing Liu,Xiaosu Yi
The flame-retardant modification of plant fiber-reinforced composites (PFRCs) is a fundamental requirement for achieving broader industrial applications. However, commonly used modification methods often compromise the fiber mechanical properties or surface reactivity due to structural damage. In this paper, a water-soluble system consisting of phytic acid imidazole salt and biobased benzoxazine was devised to modify a regenerated cellulose fabric through water-phase immersion. Benefiting from the neutral solution and self-assembly coating, the modified fabric (F-RCF) exhibited a typical self-extinguishing behavior while maintaining good structural integrity and mechanical properties. By further combining F-RCF with a DOPO-containing epoxy resin blend (FEB) to prepare a fiber-reinforced green composite (F-RCF/FEB), the results indicated that the co-curing reaction between the modifier and resin matrix contributed to improved interfacial adhesion. This enabled the simultaneous enhancement of tensile modulus (from 9.82 to 11.29 MPa), impact strength (from 6.58 to 7.26 kJ m −2 ) and interlaminar shear strength (from 11.41 to 13.89 MPa). More importantly, F-RCF/FEB exhibited excellent anti-flammability in terms of a high limiting oxygen index value of 34.3% and a UL-94 V-0 rating, and the peak heat release and total heat release were also markedly reduced by 44.9% and 36.9%, respectively. Mechanism analysis revealed that the modified system effectively prevented the wick effect and provided an inhibitory effect in the gaseous phase, as well as a barrier effect in the condensed phase. This study presents a non-destructive modification strategy for plant fibers, which may also inspire the synchronous enhancement of interfacial compatibility and fire-proof performance of PFRCs. © 2025 Society of Chemical Industry.
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CHEMICAL ENGINEERING JOURNAL
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2024
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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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Nature Communications
·
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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Journal of the American Chemical Society
·
2025
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IF 15.6
Deyun Sun,Shangqing Chen,Miao He,Hongxue Xu,Yongxiang Sun,Lijuan Shi,Hongbo Zeng,Qun Yi
Efficient extraction of high-purity CO2 from humid flue gas via adsorptive separation offers a promising and sustainable solution for carbon reduction and downstream applications. However, the coadsorption of H2O vapor and N2 from humid flue gas remains a persistent challenge that limits separation efficiency. To overcome this issue, this work introduces a novel concept of ionic hydrophobic gates on porous adsorbents, which enables one-step separation of high-purity CO2 directly from humid flue gas. By assembling hydrophobic ionic liquids and fluorine-rich terephthalaldehyde onto the surface of a metal–organic framework (MOF), this design establishes H2O barriers and CO2 channels on the outer shell while maintaining pore integrity in the core. The resulting core–shell material demonstrates exceptional CO2 adsorption capacity and an extraordinary CO2/N2 selectivity of 1780 (15/85, v/v), surpassing conventional adsorbents. Notably, dry CO2 with 99.999% purity is successfully extracted from humid flue gas (relative humidity, RH = 100%) in a single breakthrough experiment. In situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) and density functional theory calculations reveal that fluorine-rich hydrophobic sites act as effective H2O barriers, while ionic liquid segments facilitate the transport of CO2 through hydrogen bonding and electrostatic interactions. Owing to its excellent scalability and broad compatibility with diverse MOF platforms, this ionic hydrophobic gating strategy offers a robust and versatile approach for constructing advanced gas separation materials, holding great promise for industrial applications in carbon capture, clean energy, and sustainable chemical processes.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
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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Journal of Environmental Chemical Engineering
·
2024
·
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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