SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Yan Pan,Chuanming Tu,Xueyong Li,Luteng Gao,Wei Lan,Wenhai Zhang,Hong Meng
Compared with traditional polyamide membranes, polyimine membranes possess a more rigid structure and exhibit significantly enhanced swelling resistance in organic solvent nanofiltration, enabling highly selective separation. However, their intrinsic broad pore size distribution limits their application in high-precision separation scenarios. To address this issue, this study proposes a post-modification pore shrinkage strategy: first, a polyimine composite membrane is prepared via interfacial polymerization, followed by the in-situ polymerization of residual free p -phenylenediamine within the membrane initiated by ammonium persulfate, to construct an interpenetrating network composite membrane structure composed of porous polyimine and poly( p -phenylenediamine). Experimental results demonstrate that this method effectively improves the rejection performance of polyimine membranes toward small solute molecules. The optimized PPa-5@TpPa-2 composite membrane exhibits a methanol permeance of 4.1 L m −2 h −1 bar −1 , a molecular weight cut-off as low as 320 Da, along with excellent solvent resistance, operational stability.
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Polymers
·
2026
·Vol. 18
·期 15
·1902
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IF 5.8
Jinxiong Wen,Xianhao Mao,Shaojun Chen,Yuanyuan Li,Zhiwen Tu,Huilin Lai,Haitao Zhuo
To address the critical limitations of traditional photothermal–responsive epoxy–based shape memory polymers (ESMPs), such as poor compatibility and cyclical instability, a series of side–chain azobenzene (Azo)–functionalized linear ESMPs (EPDm) were successfully synthesized via chemical bonding. Highly rigid 4–aminoazobenzene (Azodm) units were covalently integrated into the Bisphenol A–type epoxy backbone as functional photo–responsive side chains. Systematic characterizations confirmed that the glass transition temperature (Tg) of the EPDm polymers could be precisely tuned from 41.53 °C to 53.26 °C by adjusting the Azodm content. Benefiting from the proposed homogeneous covalent architecture, the EPDm films exhibited superior photothermal sequential behavior and remarkable shape memory stability despite a slight reduction in tensile strength (≈10–12 MPa). Under 365 nm UV irradiation, the pre–stretched EPDm10specimen achieved a rapid macroscopic bending angle of over 150° within 15 s, driven exclusively by thetrans–to–cismolecular photoisomerization of the Azo side chains well below the matrix Tg. Furthermore, standard shape memory cycles demonstrated excellent shape fixity (Rf> 98%) and recovery (Rr> 95%) ratios, alongside exceptional anti–fatigue performance with minimal strain variance (≈5%) over consecutive cycles. This work establishes a robust and high–efficiency molecular design strategy for photo–thermally sequentially responsive shape memory polymers, offering immense potential for smart actuators and flexible electronics.
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Nature Energy
·
2026
·
IF 70.1
Zhang Zuhong,Zhu Rui,Li Guixiang,Tang Ying,Wu Hongzhuo,Zhao Jinbo,Wu Jiaxin,Gries Thomas W.,Musiienko Artem,Zuo Shengnan,Li Zhe,He Bingchen,Su Zhenhuang,Gao Xingyu,Zuo Weiwei,Hou Bo,Pascual Jorge,Sapienza Luca,Wang Luyao,Deng Lin-Long,Jia Yu,Li Gang,Dyson Paul J.,Nazeeruddin Mohammad Khaja,Saliba Michael,Abate Antonio,Li Meng
Realizing stable and scalable perovskite solar cells (PSCs) under real-world outdoor conditions remains a challenge for deployment. Here we report a strategy to improve the resilience of the grain boundary, achieving simultaneous improvement in the power conversion efficiency and long-term operational durability under realistic light cycling and ultraviolet exposure of PSCs. By integrating photoswitchable isomers at grain boundaries, we suppress lattice bond rupture and defect accumulation during repeated light cycling through light-triggered dynamic damage release. This approach stabilizes the triple-cation lead-based perovskite lattice against photoinduced distortions and degradation pathways. As a result, the PSCs retain over 95% of their initial performance after 2,000 h of ultraviolet-containing light cycling at 65 °C and 500 thermal cycles between –40 °C and 85 °C, and deliver a power conversion efficiency of 27.2% (certified as 26.9%). Our strategy improves the operational stability and commercial viability of triple-cation perovskite photovoltaics.
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CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Xinyu Xu,Zheng Jia,Jing Hu
The novel anti-counterfeiting label operates under synergistic logical modulation. • Multimode pattern storage relies on photo-liquefaction of azobenzene derivative. • Eco-friendly and crack-recovery composites show unique interfacial characteristic. Information storage labels that respond to multiple stimuli and enable multimode storage exhibit higher flexibility and security. However, this goal typically demands elaborate structural design and specialized storage strategies. In this study, a room-temperature photo-liquefiable crystal based on small-molecule azobenzene derivative was combined with an eco-friendly waterborne polyurethane (WPU) matrix, adopting the crystalline composite strategy. The results showed that the appropriate photo-liquefiable crystal can still retain sufficient solid-to-liquid phase transition ability in the encapsulated state, and can also solve the problem of leakage as well as the environmental pollution after liquefaction. The information storage labels fabricated from photo-liquefiable crystal and WPU matrix showed dual responsiveness to light and temperature, and featured multiple storage modes including short-term rewritable photochromic pattern storage mode and long-term anti-tampering light-scattering pattern storage mode, etc. It is presumably attributed to the synergistic effect between the photo-liquefiable crystal and WPU matrix. A variety of behaviors occurring within individual components and at their interfaces, including photochemical phase transition, interfacial microregional internal stress and polymer chain segment relaxation, jointly contribute to this effect. Furthermore, the information storage labels possessed intrinsic stimulus-responsive crack recovery ability, which further boosted the overall material properties. This study demonstrates the potential of the encapsulated photo-liquefiable crystal in information storage and provides a new strategy for synergistic interfacial regulation of composite materials. Download: Download high-res image (201KB) Download: Download full-size image
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Zhenyu Lei,Siqi Liu,Ziyi Chen,Tao Gan,Lin Wu,Honglei Sun,Xiaomin Yang,Jingyao Liu,Peng Zhang,Mingjun Jia
Constructing highly efficient and stable non-noble metal catalysts for selective hydrogenation of nitroarenes is a very appealing yet challenging task in the fields of materials science and catalysis. Herein, a series of N-doped carbon-anchored Zn single-atom catalysts were prepared by pyrolyzing the biomass-based composite precursors composed of chitosan, tannic acid, and ZnCl 2 . The optimal sample of Zn-Cl/NC-3_900 displays superior catalytic activity with a turnover frequency of 4817 h −1 at 80°C, selectivity (∼99%), and recyclability (without any post-treatment) for hydrogenation of p -chloronitrobenzene to p -chloroaniline with N 2 H 4 ·H 2 O. Its catalytic performance is well kept even after HCl or KSCN treatments, revealing excellent chemical stability and anti-poisoning capability. Additionally, a very high p -chloroaniline selectivity (∼98%) could be obtained under mild conditions (1.0 MPa, 100°C) when H 2 is used as reductant. Characterization results and theory calculations demonstrate that introducing an appropriate amount of N/Cl species may finely modulate the local coordination environments of Zn single-atoms. The resultant axially Cl-coordinated ZnN 2 sites (Zn-N 2 Cl) possess moderated adsorption/desorption capability and lower activation barriers, in line with the Sabatier principle, thereby significantly boosting the catalytic hydrogenation performance. This work provides a simple and effective approach for developing efficient hydrogenation catalysts through manipulating the coordination structure of metal single-atom sites.
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Nanoscale Horizons
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2023
·Vol. 8
·期 6
·812-826
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IF 9.7
Junqing Ye,Meizan Jing,Yu Liang,Wenjin Li,Wanting Zhao,Jianying Huang,Yuekun Lai,Weiyu Song,Jian Liu,Jian Sun
Exploring eco-friendly and cost-effective strategies for structure engineering at the nanoscale is important for boosting heterogeneous catalysis but still under a long-standing challenge. Herein, multifunctional polyphenol tannic acid, a low-cost natural biomass containing catechol and galloyl species, was employed as a green reducing agent, chelating agent, and stabilizer to prepare Au nanoparticles, which were dispersed on different-shaped CeO2 supports (e.g., rod, flower, cube, and octahedral). Systematic characterizations revealed that Au/CeO2-rod had the highest oxygen vacancy density and Ce(III) proportion, favoring the dispersion and stabilization of the metal active sites. Using isopropanol as a hydrogen-transfer reagent, deep insights into the structure–activity relationship of the Au/CeO2 catalysts with various morphologies of CeO2 in the catalytic nitrobenzene transfer hydrogenation reaction were gained. Notably, the catalytic performance followed the order: Au/CeO2-rod (110), (100), (111) > Au/CeO2-flower (100), (111) > Au/CeO2-cube (100) > Au/CeO2-octa (111). Au/CeO2-rod displayed the highest conversion of 100% nitrobenzene and excellent stability under optimal conditions. Moreover, DFT calculations indicated that nitrobenzene molecules had a suitable adsorption energy and better isopropanol dehydrogenation capacity on the Au/CeO2 (110) surface. A reaction pathway and the synergistic catalytic mechanism for catalytic nitrobenzene transfer hydrogenation are proposed based on the results. This work demonstrates that CeO2 structure engineering is an efficient strategy for fabricating advanced and environmentally benign materials for nitrobenzene hydrogenation.
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高影响因子
Journal of Cleaner Production
·
2023
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IF 11.1
Shuangying Li,Qingxiang Zhou,Zhi Li,Menghua Liu,Yanhui Li,Chunmao Chen
In this work, an effective fluorescent probe for analysis of p-aminoazobenzene (p-AZO) was established with carbon dots (CDs) and magnetic molecularly imprinted nanomaterial , in which CDs and the magnetic nanomaterial were simultaneously derived from prussian blue (PB) by one-pot hydrothermal method . The sensitivity of the constructed probe is greatly improved owing to the introduction of magnetic solid phase extraction. Factors affecting the enrichment efficiency and detection performance of p-AZO were optimized. Under optimal conditions, the probe exhibited good selectivity and sensitivity for p-AZO. Good linearity was achieved in the range of 2–600 nmol L −1 . Low detection limit for p-AZO was 1 nmol L −1 . Satisfactory recoveries in the range of 95.8–98.7% were obtained at two spiked concentrations of 0.02 and 0.1 μmol L −1 , indicating that the probe established with CDs and MMIPs based MSPE was reliable and robust for determination of p-AZO in real water samples.
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Molecular Catalysis
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2022
·
IF 5.089
Zichen Zhang,Donglin Yang,Jiaqiang Wang,Chaoting Deng,Hengjun Gai,Meng Xiao,Tingting Huang,Quanhong Zhu,Hongbing Song
Ionic liquids (ILs) are unique substances with unique ionic sites. They are regarded as one of the most promising green solvents and catalysts in the 21st century. In this work, the synthesis of imidazolium-based ILs as metal-free catalysts by molecular design is reported for the first time. By using the ILs as precursors, hyper-crosslinked poly(ionic liquid) (HCPIL) was synthesized by Friedel–Crafts alkylation reaction. These metal-free catalysts can effectively activate ethanolamine for the hydrogenation of nitrobenzene, and they have definite active sites. As the synthesized HCPIL-Cl has a rich porous structure and IL structural units, it could maintain the catalytic activity of ILs and recover them via efficient facile filtration and washing. Density functional theory (DFT) calculation suggested that the imidazolium structure is essential to ethanolamine activation. The calculated results of DFT agree well with the experimental results. The hydrogenation of nitrobenzene has many intermediates whose selectivity can be regulated by different gas atmosphere or alkaline environments. This work provides a promising method for the design of metal-free catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Dan Xu,Jianfeng Li,Boyang Li,Huacheng Zhao,Hanghang Zhu,Jinfang Kou,Fengwei Zhang,Zhengping Dong,Jiantai Ma
The sustainable catalytic transformation of alcohols to high value-added fine chemicals is a significant and challenging research topic. Herein, a set of nitrogen-doped carbon encapsulated Co-based catalysts (Co-Co 3 O 4 @NC-T) were prepared by using low-cost dicyandiamide, glyoxal and cobalt nitrate as precursors. The obtained catalysts were utilized for the selective oxidation of alcohols to high value-added esters and carboxylic acids with air as the oxygen source and displayed wide applicability for the oxidation of both aromatic and aliphatic alcohols. Based on the controlled experiments, the protective effect of N-doped carbon structure and the synergistic effect between Co core and Co 3 O 4 species guaranteed the high reaction conversion and selectivity. Benefitting from heterogeneity and magnetism of the catalyst, it can be easily recycled and reused for long-term stability. Reasonable mechanisms of selective oxidation reaction were proposed through EPR analysis and controlled experiments. The present work provides a facile strategy for potential large-scale preparation of heterogeneous catalyst for sustainable and green catalytic transformations.
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Computational and Theoretical Chemistry
·
2021
·
IF 1.926
Jianqiang Zhao,Yue Zhang,Lihua Gan,Guanlei Wang
Here, we combined experimental measurements and DFT calculations to study UV–vis absorption spectra. DFT calculations of azobenzene and its derivatives proved useful for estimation of experimental spectra with near one-to-one correspondence. Calculation results show that substituents have no obvious effect on the coplanarity of benzene rings and N N bond. Potential energy surfaces were calculated for DHA and DEA. In the ground state, the inversion pathway was found to be preferred. A conical intersection was found between the ground and first excited states along the rotation pathway, indicating that the rotation mechanism is favored in the first excited state for DHA and DEA. UV–vis spectra of DHA and DEA were calculated by TD-DFT. Compared with azobenzene, the calculated wavelength of maximum absorption of DHA- trans and DEA- trans has red shift in UV–vis absorption spectra, which are in reasonable agreement with the experimental data.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yuhang Chen,Yaheng Zhang,Hongwei Zou,Minglei Li,Gang Wang,Min Peng,Jie Zhang,Zhiyong Tang
Difficult handling the solid catalysts remains one of the pain points in the continuous flow photochemistry. In this work, the gas–liquid-solid segmented flow was employed in the photocatalytic production of azo- compounds (azoxybenzene and azobenzene) from nitrobenzene using graphitic carbon nitride (g-C 3 N 4 ) as solid catalyst. Compared with the batch reactor, the photocatalytic reaction rate was greatly improved in the microreactor, and the reaction time was shortened from 180 min of the batch to 7.5 min for near-full conversion of nitrobenzene. The effects of various reaction parameters (temperature, light source power, catalyst content) in the continuous system were examined, and the reaction kinetic was found in first order. The photocatalytic reaction performance was very sensitive to the gas–liquid-solid segmented flow conditions, which needed to be carefully tuned. With the help of high-speed camera and micro particle image velocimetry (µ-PIV) techniques, it was identified that the increasing inert gas fraction resulted in more stable segmented flow with shorter liquid segments, favoring the reaction rate. With a high gas fraction, the intensity of recirculation in the liquid segments was strengthened by the increasing total flow rate, enhancing the local mass transfer, thereby benefiting the photocatalytic reaction. Overall, the continuous microreactor reached 5.6 times higher productivity per volume (26.1 mmol/h*L) of azo- compounds than the batch reactor under the same conditions. The successful photosynthesis of azo- compounds demonstrated the great potential of the presented gas–liquid-solid segmented flow, and the findings of this work provide useful guidance on its future application in other heterogeneously catalyzed reactions.
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JOURNAL OF CONTROLLED RELEASE
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2020
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IF 7.727
Xinghui Si,Sheng Ma,Yudi Xu,Dawei Zhang,Na Shen,Haiyang Yu,Yu Zhang,Wantong Song,Zhaohui Tang,Xuesi Chen
As the most common malignancy in women, breast cancer causes >40,000 deaths annually. Ribonuclease A (RNase), a new anti-cancer agent, has attracted intense interest due to its high efficacy and specificity. However, RNase suffers from instability, a short half-life in the circulation and poor membrane penetration. To overcome these challenges, we designed a supramolecular nanogel for the cytosolic delivery of RNase. The nanogels were fabricated using host–guest interactions between azobenzene (Azo) and β-cyclodextrin (βCD) conjugated to poly (L-glutamic acid)- graft -poly (ethylene glycol) methyl ether (PLG- g -mPEG). RNase could be loaded inside the nanogels in mild aqueous conditions. Following optimization, the RNase-loading content and efficiency of the nanogel were 23.5 wt% and 50.4%, respectively. In the presence of nitroreductase (NTR), the cross-linking point between Azo and βCD was destroyed due to the conformation transition of Azo, ensuring the hypoxia-sensitive release of cargo from the nanogels in tumors in which NTR is overexpressed. In vitro release profiles revealed that 75.0% of the RNase was released under hypoxic conditions in 72 h, whilst only 19.7% was released under normoxic conditions. Cytotoxicity assays showed that the RNase-loaded nanogels (nano-RNase) were more efficient in inhibiting the proliferation of 4T1 cells than free RNase. In vivo studies showed 68.7% tumor suppression rates (TSR %) in the nano-RNase treated group, whilst free RNase treatment led to a lack of tumor inhibition. To further enhance the hypoxia status of tumors, we combined nano-RNase with a nanoformulation of vascular disrupting agents PLG- g -mPEG/combretastatinA4 (nano-CA4) and obtained a TSR of 91.7%. The hypoxia-sensitive supramolecular nanogels provided a versatile platform for the delivery of RNase, highlighting its applicability for cancer therapy.
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