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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 21 ·10372-10380 · IF 3.3

Enhancing the photothermal performance of graphene oxide by embedding perylene diimide radical anions/α-phenylethylamine hydrogen bonded complexes in graphene oxide films for solar water evaporation

Yuanyuan Li,Jinming Liu,Wei Li,Yingru Li,Wei Zhao,Haiquan Zhang

Typically, perylene diimide radical anions have broad and strong absorption in the near-infrared light region and exhibit excellent photothermal conversion performance, so they are considered as new potential organic photothermal materials. However, the stability of perylene diimide radical anions in air has always been a thorny issue. We found an effective way to improve the stability of perylene diimide radical anions through formation of low barrier hydrogen bonds between perylene diimide radicals and alkyl primary amines. In this paper, we report the synthesis of a stable perylene diimide radical anion/α-phenylethylamine hydrogen bonded complex (α-PEA⋯PDI˙−), and preparation of a kind of α-PEA⋯PDI˙−/GO (graphene oxide) film using a simple impregnation method. Compared to GO films and α-PEA⋯PDI˙− powder, the film exhibited a good photothermal response with the highest photothermal conversion temperature of 82.4 °C under light, a temperature increase rate of up to 35 °C, and a photothermal conversion efficiency of 24.07%. The film is optically stable and reusable, and also exhibits superior performance compared to pure graphene oxide for solar water evaporation.

CAS / MDL: 3886-69-9
研究领域: 材料科学 · 化学 · 纳米技术 · 太阳能
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JOURNAL OF CATALYSIS · 2025 · IF 6.5

Tailoring microenvironments of metal-enzyme cascade catalysts for efficient DKR reaction of chiral amine

Mengyu Li,Wei Zhuang,Xia Meng,Wenxia Zhang,Keke Zhang,Zhenfu Wang

Metal-enzyme integrated catalysts combine the high selectivity of enzyme catalysts with the broad substrate spectrum of metal catalysts and offer tremendous possibilities for chemoenzymatic cascade processes. However, the rational design of microenvironments in nanostructures that make metals and enzymes compatible for efficient activity still remains challenging. In this report, a nanocomposite catalyst was fabricated by integrating ultrafine Pd nanoparticles (Pd NPs) and Candida antarctica lipase B (CALB) on the hydrophobic polydopamine-coated SiO 2 (SP) to enhance the compatibility of enzyme-metal catalysts. In detail, Pd NPs were in situ reduced by PDA on the SP surface, and the obtained SP-loaded Pd (Pd/SP) was hydrophobically modified by octadecyltrimethoxysilane for the subsequent adsorption immobilization of CALB to prepare the integrated catalyst, CALB/mPd/SP. The hydrophobic PDA coating on SiO 2 not only stabilized the loaded ultrasmall Pd nanoparticles but also facilitated the activation of the immobilized lipase, which helped to improve the cascade catalytic efficiency of CALB/mPd/SP. Afterward, CALB/mPd/SP was used in a one-pot dynamic kinetic resolution (DKR) reaction of α-phenylethylamine with high conversion (>99 %), selectivity (93.9 %), and ee p (>99 %). After 25 days of storage and 5 h of sonication, CALB/mPd/SP exhibited no significant reduction in the DKR catalytic activity. This study proposed a simple and sustainable method for the preparation of enzyme-metal cascade catalysts to enhance their stability and achieve significantly increased activity through interfacial microenvironmental modulation.

研究领域: 生物化学 · 催化化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

High-performance polyester composite nanofiltration membrane fabricated by interfacial polymerization of ribitol and trimesoyl chloride: Dye desalination performance and mechanisms

Zhongyue Sun,Hui Qiu,Xinwei Kang,Weiwei Zhou,Wenxin Yan,Feiyong Chen,Jingtao Xu,Daoji Wu,Daliang Xu,Xuewu Zhu

A loose nanofiltration (LNF) membrane with high permeance and excellent dye/salt selectivity is highly desirable for dye/salts recovery from textile wastewater. Herein, commercial and green ribitol (RT) was employed to fabricate the LNF membrane for dye desalination. The hydroxyl in the RT reacted with acyl chloride under the catalysis of sodium hydroxide, forming a polyester film structured with microspheres, negative charge, and hydrophilic networks. The resultant RT-M membrane possessed a smooth and thin active layer with numerous polar groups. The dye desalination performance of the RT-M membrane was tailored by controlling various IP fabrication conditions. The optimized membrane (RT-M1.0) had superior water permeance (100.3 L m −2 h −1 bar −1 ) and satisfactory CR/Na 2 SO 4 selectivity (281.3). Additionally, the RT-M membrane had favorable stability and antifouling properties, demonstrating excellent potential for application in dye desalination. Therefore, a novel approach for fabricating membranes with outstanding dye desalination properties by using RT was proposed to achieve resource recycling.

研究领域: 材料科学 · 环境工程
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LAB ON A CHIP · 2025 · IF 5.4

Chiral organic-inorganic hybrid perovskites synthesized using acoustofluidic closed system

Tao Zhou,Ran Tao,Yan Yu,Chong Li,Zhang Haonan,Jing-Ting Luo,Chen Fu,Fujian Ren,Yong Qing Fu

Chiral organic-inorganic hybrid perovskite films hold significant promise for optoelectronic applications due to their unique optical activity and excellent optoelectronic properties. However, their air and moisture sensitivity necessitates inert atmosphere processing, hindering practical application. In this work, we present a closed acoustofluidic system utilizing surface acoustic wave-based microcentrifugation for the synthesis of high-quality synthesizing (S-MBA)2PbI4 films. By confining both synthesis and film deposition within a sealed chamber, this approach eliminates air exposure, enabling the fabrication of films with enhanced crystallinity and a reduced bandgap of 2.37 eV. The resulting chiral perovskite films exhibit significant circular dichroism, with an asymmetry factor of 9.3×10-4. Furthermore, control over film surface roughness (achieving < 0.6 μm) is demonstrated through modulation of acoustic operation parameters. The cost-effectiveness and versatility of this acoustic microcentrifugation system highlight its potential for advanced film material fabrication.

研究领域: 材料科学 · 光学工程
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DESALINATION · 2025 · IF 9.8

Polyester-polyamide interpenetrating network-structured nanofiltration membranes for efficient natural surface water purification

Xuewu Zhu,Feiyue Ge,Xinwei Kang,Liping Qiu,Jinyu Li,Xiaozhen Lu,Bin Liu,Daoji Wu,Zhe Yang,Daliang Xu

Conventional polyamide nanofiltration (NF) membranes face limitations in water treatment due to perm-selectivity trade-offs and chlorine sensitivity. This study introduced a phloroglucinol (PG) post-treatment strategy to construct polyester-polyamide interpenetrating network (IPN) NF membranes capable of overcoming these limitations. The IPN membranes featured a unique Turing surface morphology and a compact crosslinked network, which increased the effective filtration area while forming a thinner yet denser selective layer. This structural design enhanced hydrophilicity and negative surface charge, resulting in improved water permeance (24.5 L·m −2 ·h −1 ·bar −1 ) and a high organic matter rejection of 90.7 %. Notably, the modified membranes demonstrated remarkable chlorine stability, maintaining over 93 % of their initial rejection efficiency even after extreme chlorine exposure (20,000 ppm·h). This advancement addresses the rapid degradation of traditional polyamide membranes in chlorinated environments. Such extraordinary stability arises not only to from the inherent chlorine resistance of the polyester network but also from the multi-layered protective architecture enabled by the unique IPN configuration. The proposed IPN strategy provides an effective pathway for developing next-generation potable water treatment membranes.

研究领域: 环境科学 · 材料科学 · 化学工程 · 水处理技术
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DESALINATION · 2025 · IF 9.8

Thin film nanocomposite nanofiltration membrane uniformly embedded with sulfonic Noria cages at high loading for elevated perm-selectivity and antifouling properties

Chunhui Zhang,Jiahe Sun,Xinyu Zhang,Bing Xu,Yuanqing Guo,Ming Xie,Jianguo Zhu,Jingtao Xu,Feiyong Chen

Water perm-selectivity and membrane fouling are the major challenges faced by nanofiltration (NF) membranes. In this work, a thin film nanocomposite (TFN) membrane with excellent separation and antifouling performances was fabricated by uniformly doping S-Noria (sulfonic Noria, a macrocyclic molecule) in polyamide layer with high loading capacity. S-Noria synthesized by sulfonating Noria with taurine has smaller nanoparticle size of ~5.9 nm and better water dispersion compared with Noria. Therefore, the water permeability of the optimal S-TFN 0.75 membrane can be increased to 2.2 times and 3.4 times that of the Noria-TFN and control TFC membranes, respectively, while maintaining a comparable Na 2 SO 4 rejection of ~98 %. During the dynamic organic fouling tests, the S-TFN 0.75 membrane with higher surface hydrophilicity and surface capacity of sulfonic groups showed milder flux decay and better flux recovery than the control TFC membrane. In addition, the S-TFN 0.75 membranes could more effectively alleviate the membrane fouling exacerbated by “Ca 2+ bridging effect”. In conclusion, this study provides a reliable method for the fabrication of TFN membrane with a high load of S-Noria uniformly dispersed in the polyamide layer, solving the bottleneck problems of water perm-selectivity and membrane fouling.

研究领域: 膜科学 · 水处理技术 · 材料科学 · 纳米技术 · 环境工程
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CHINESE JOURNAL OF POLYMER SCIENCE · 2026 · IF 4.6

Towards Oxygen-stable Vinylene-linked Covalent Organic Frameworks: Mitigating Photobleaching for Enhanced Photostability

Zhu Zi-Han,Guo Jia

Conjugated covalent organic frameworks (COFs) possess distinct advantages over amorphous organic photocatalysts, including high charge transfer efficiency and effective light utilization. However, their photocatalytic performance often declines under prolonged solar irradiation in air, largely owing to their limited photostability. In this study, we systematically investigated the photobleaching mechanism of vinylene-linked COFs synthesized via aldol condensation between 2,4,6-trimethyl-1,3,5-triazine and aldehydes. When the COF contains phenylene as the linker, oxygen can undergo photoinduced addition across the vinylene bond, leading to cleavage of the vinylene bonds and the formation of terminal aldehydes, thereby causing photobleaching. Mechanistic studies indicated that superoxide anion radicals play a key role in this oxidative degradation process, accompanied by the partial cycloaddition of adjacent vinylene bonds. To enhance photostability, we incorporated naphthyl groups into the framework at the strut, replacing phenylene to modulate the excited-state electronic structure at the vinylene linkages. The newly synthesized COF exhibited notable anti-photobleaching capability in the presence of oxygen. This work not only deepens the understanding of photodegradation mechanisms in conjugated COFs but also offers valuable insights for the design and application of photostable COF-based catalysts.

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JOURNAL OF CHROMATOGRAPHY A · 2019 · IF 3.858

Polysiloxane assisted fabrication of chiral crystal sponge coated capillary column for chiral gas chromatographic separation

Zi-Meng Wang,Cheng-Xiong Yang,Xiu-Ping Yan

Chiral crystalline sponges (CCSs) are a recent class of chiral porous metal complexes potential in chiral recognition. Here we report the fabrication of polysiloxane OV-1701 incorporated CCS-3S (PSO/CCS-3S) coated capillary column as a novel stationary phase for gas chromatographic separation of diverse racemates. CCS-3S with the chiral ligand of ( S )-mandelic was selected as the model CCS. With the aid of polysiloxane OV-1701, PSO/CCS-3S coated capillary column gave improved resolution, broader enantiomers separation scope and much larger McReynolds constants than CCS-3S coated capillary column. Many racemates that cannot be separated on CCS-3S coated capillary column were well resolved on PSO/CCS-3S coated capillary column. The PSO/CCS-3S coated capillary column also gave wide linear range, low limit of detection, good repeatability and reproducibility, and fine inertness and anti-column bleeding properties for the separation of enantiomers. In addition, the PSO/CCS-3S coated capillary column presented better resolution for the studied racemates than commercial β-cyclodextrin based Cyclosil B (30 m long ×0.32 mm i.d. × 0.25 μm film thickness), β-DEX 225 (30 m long ×0.25 mm i.d. × 0.25 μm film thickness) and amino acid based Chirasil L-Val (25 m long ×0.25 mm i.d. × 0.12 μm film thickness) capillary columns. These results indicate the great potential of PSO/CCS-3S coated capillary column in separation of enantiomers.

研究领域: 分析化学 · 材料科学
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APPLIED SURFACE SCIENCE · 2015 · IF 2.711

Enhanced visible-light photocatalytic activity for selective oxidation of amines into imines over TiO2(B)/anatase mixed-phase nanowires

Jun Dai,Juan Yang,Xiaohan Wang,Lei Zhang,Yingjie Li

Wirelike catalysts of mixed-phase TiO 2 (B)/anatase TiO 2 , bare anatase TiO 2 and TiO 2 (B) are synthesized via calcining precursor hydrogen titanate obtained from hydrothermal process at different temperatures between 450 and 700   °C. Under visible light irradiation, mixed-phase TiO 2 (B)/anatase TiO 2 catalysts exhibit enhanced photocatalytic activity in comparison with pure TiO 2 (B) and anatase TiO 2 toward selective oxidation of benzylamines into imines and the highest photocatalytic activity is achieved by TW-550 sample consisting of 65% TiO 2 (B) and 35% anatase. The difference in photocatalytic activities of TiO 2 samples can be attributed to the different adsorption abilities resulted from their crystal structures and interfacial charge separation driven by surface-phase junctions between TiO 2 (B) and anatase TiO 2 . Moreover, the photoinduced charge transfer mechanism of surface complex is also proposed over mixed-phase TiO 2 (B)/anatase TiO 2 catalysts. Advantages of this photocatalytic system include efficient utilization of solar light, general suitability to amines, reusability and facile separation of nanowires catalysts.

研究领域: 材料科学 · 环境科学
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JOURNAL OF CHROMATOGRAPHY A · 2021 · IF 4.759

Highly sensitive novel fluorescent chiral probe possessing (S)-2-methylproline structures for the determination of chiral amino compounds by ultra-performance liquid chromatography with fluorescence: An application in the saliva of healthy volunteer

Xi-Ling Li,Yu Han,Yuan Huang,Xiaoqi Sun,Shuyun Xiao,Jun Zhe Min

We developed a novel fluorescent chiral probe, DBD-trans-2-methyl-L-proline (DBD-M-Pro), which can be used to target recognition of amino functional groups using chiral resolution. To investigate the chiral resolution efficiency, 20 chiral amino enantiomers (19 DL-amino acids and phenylethylamine) were labeled using ultra-performance liquid chromatography (UPLC) with a fluorescence (FL) system. Diastereomers were formed by the reactions of DBD-M-Pro with enantiomers of amino functional groups at 60 °C for 60 min and detected on a BEH C18 column (100 × 2.1 mm, 1.7 μm). Gradient elution of 10 mM ammonium acetate with 0.05% formic acid (FA) aqueous solution and 0.1% FA acetonitrile or 0.1% FA methanol solution was performed at an excitation wavelength (Ex) 460 nm and emission wavelength (Em) 550 nm. Each resulting derivative of D- and L- type was effectively separated. The results showed that the resolution (Rs) of 17 amino acids and phenylethylamine (PEA) in the range of 1.59–24.11, except for histidine (His) (Rs = 1.32) and serine (Ser) (Rs = 1.47), achieved completely separation. The DBD-M-Pro chiral probe has a robust chiral selectivity for D-amino acids. Furthermore, a new method for the simultaneous determination of six DL-amino acids (Pro, Val, Trp, Phe, Leu, Lys) in human saliva was developed. The proposed method showed resolution values of 1.78–16.38, and an excellent linear relationship was obtained in the range of 2.5–500 pmol ( R 2  ≥ 0.9990). The limit of detection (S/ N  = 3) ranged from 0.5 to 3.75 pmol. The intra-day and inter-day coefficient of variation (CV) were within the range of 1.75–11.73%. The average addition recoveries in saliva ranged from 95.99 to 106.97%. The methodology was used to determine the content of DL-amino acids and the D/L-amino acid ratio in the saliva of 40 healthy volunteers (15 males and 25 females), as well as evaluating the differences between men and women. Our study suggests that the DBD-M-Pro chiral probe could be an effective tool for screening potential D-amino acid biomarkers in disease.

研究领域: 分析化学 · 生物化学 · 医学诊断
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MOLECULES · 2023 ·Vol. 28 ·期 3 ·922 · IF 4.6

Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine

Pengcheng Li,Jingjing Zhu,Hongyu Zhang,Lan Wang,Shulin Wang,Mengting Zhang,Jianping Wu,Lirong Yang,Gang Xu

Chiral amines are essential components for many pharmaceuticals and agrochemicals. However, the difficulty in obtaining enantiomerically pure amines limits their application. In this study, hollow amorphous ZIF-90 (HamZIF-90) materials were prepared by template engraving, and chemical–enzyme coupling catalysts (HamZIF-90@Pd@CALB) were constructed for the chiral resolution of 1-phenylethylamine. Different from conventional materials, HamZIF-90 had tunable hollow structures by altering its central node zinc ion concentrations, and the embedded hydrogel template gave it more pore structures, which facilitated the loading of enzyme molecules and Pd nanoparticles (NPs). The establishment of the coupling catalysts shortened the mass transfer distance of the reactant molecules between the metal nanoparticles and the enzyme catalyst in the dynamic kinetic resolution (DKR) reaction, resulting in 98% conversion of 1-phenylethylamine and 93% selectivity of Sel.R-amide. The proposal of this idea provided a good idea for future tailor-made MOFs loaded with chemical and enzyme coupled catalyst.Keywords:hollow amorphous;HamZIF-90@Pd@CALB;DKR;1-phenylethylamine

研究领域: 化学 · 生物催化 · 材料科学
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-11 · IF 16.6

Ligand vacancy channels in pillared inorganic-organic hybrids for electrocatalytic organic oxidation with enzyme-like activities

Chen Zhe,Li Jili,Meng Lingshen,Li Jianan,Hao Yaming,Jiang Tao,Yang Xuejing,Li Yefei,Liu Zhi-Pan,Gong Ming

Simultaneously achieving abundant and well-defined active sites with high selectivity has been one of the ultimate goals for heterogeneous catalysis. Herein, we construct a class of Ni hydroxychloride-based inorganic-organic hybrid electrocatalysts with the inorganic Ni hydroxychloride chains pillared by the bidentate N-N ligands. The precise evacuation of N-N ligands under ultrahigh-vacuum forms ligand vacancies while partially retaining some ligands as structural pillars. The high density of ligand vacancies forms the active vacancy channel with abundant and highly-accessible undercoordinated Ni sites, exhibiting 5-25 fold and 20-400 fold activity enhancement compared to the hybrid pre-catalyst and standard β-Ni(OH) 2 for the electrochemical oxidation of 25 different organic substrates, respectively. The tunable N-N ligand can also tailor the sizes of the vacancy channels to significantly impact the substrate configuration leading to unprecedented substrate-dependent reactivities on hydroxide/oxide catalysts. This approach bridges heterogenous and homogeneous catalysis for creating efficient and functional catalysis with enzyme-like properties.

研究领域: 催化 · 电化学 · 材料科学 · 化学工程
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