EES Catalysis
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2025
·
IF 8.1
Ganchang Lei,Jiayin Wang,Xinhui Liu,Shiping Wang,Lijuan Shen,Shijing Liang,Yingying Zhan,Lilong Jiang
Developing efficient strategies that convert industrial waste hydrogen sulfide (H2S) into value-added products is meaningful for both applied environmental science and industrial chemistry. Here we report a series of heterogeneous N-doped carbon catalysts with synergistic C-N sites that enable the nucleophilic addition of H2S into aromatic nitrile compounds (PhCN) under mild conditions to produce thiobenzamide (PhCSNH2). The as-designed C-N sites achieve a high thioamide production rate of 26400 μmolPhCSNH2/L·h and a notable selectivity of ca. 80% at 60 °C within a short 2-hour timeframe. Additionally, the catalyst exhibits easy recyclability and maintains high stability over ten cycles during a 6-month period. Systematic microscopic and in situ spectroscopic characterizations, combined with theoretical calculations, reveal that C-pyridinic N coordination sites effectively lower the adsorption energy barrier of the crucial intermediate *PhCSHNH, offering a dynamically favorable pathway for PhCSNH2 production. Furthermore, the protocol demonstrates excellent compatibility with various substituted substrates, providing access to a diverse range of thioamides.
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ANALYTICA CHIMICA ACTA
·
2026
·
IF 6.1
Ping Wang,Meijuan Xue,Xinhui Guan,Xiaofei Gu,Xiaoqiang Qiao
Background Phospholipids in serum exosomes are promising biomarkers for breast cancer diagnosis. However, the separation of phospholipids by liquid chromatography presents several challenges due to their inherent structural heterogeneity and the presence of isomeric forms. Traditional columns often struggle with the overlapping retention times of phospholipid species, which can result in poor resolution and difficulty in accurate quantification. Furthermore, the varying polarities and hydrophobicities of different phospholipid classes necessitate specialized stationary phases to achieve optimal separation. This study aimed to develop a novel chromatographic material for the comprehensive analysis of phospholipids in complex biological matrices. Results In this study, a novel silica-based Sil-SMA-GMS copolymer brush stationary phase was fabricated for the first time via reversible addition-fragmentation chain transfer (RAFT) polymerization, using styrene-maleic anhydride (SMA) copolymer as the functional matrix and glycerol monostearate (GMS) as the derivatization reagent. Benefiting from the synergistic effects of hydrophobic moieties (benzene rings and long alkyl chains) and hydrophilic groups (carboxyl and hydroxyl groups) in the SMA copolymer, the prepared stationary phase exhibited a unique mixed hydrophilic interaction chromatography/reversed-phase liquid chromatography (HILIC/RPLC) retention mechanism. It demonstrated excellent separation selectivity and stability for both hydrophilic and hydrophobic small molecules, achieving a maximum column efficiency of 81,029 N/m. Notably, this stationary phase overcame the limitations of traditional single-mode chromatographic columns, enabling the simultaneous separation and analysis of phospholipids that vary in class, acyl chain length, and degree of unsaturation. Furthermore, by coupling the Sil-SMA-GMS column with mass spectrometry (MS), a non-targeted analytical method for serum exosomal phospholipids was developed. Applying this method to serum exosomes from breast cancer patients and healthy controls led to the identification of 9 major classes encompassing 200 phospholipid molecular subtypes, as well as the screening of phospholipid markers closely associated with breast cancer pathogenesis. Significance This work presents a novel chromatographic material for the efficient separation of phospholipids in complex biological samples and establishes a technical foundation for the construction of multidimensional lipidomics platform. This advancement provides crucial support for the screening of cancer-related biomarkers, elucidating tumor metabolic mechanisms, and exploring targeted therapeutic targets.
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高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 9
·7882
·
IF 5.6
Biao Yang,Xinbo Yang,Yuchuan Li,Siping Pang
Exposure to ultraviolet (UV) light is known to cause skin aging, skin damage, cancer, and eye diseases, as well as polymer material aging. Therefore, significant attention has been devoted to the research and development of UV absorbers. Considering the robust hydrogen bonding and conjugated structure present in nitrogen-containing polycyclic compounds, these compounds have been selected as potential candidates for exploring ultraviolet absorption properties. After structural optimization and the simulation of ultraviolet absorption spectra, four tris-[1,2,4]-triazolo-[1,3,5]-triazine (TTTs) derivatives, namely TTTB, TTTD, TTTJ, and TTTL, were selected as the preferred compounds and synthesized. The structure of the compound was determined using various analytical techniques, including FTIR,1HNMR,13CNMR, HRMS, and XRD. Subsequently, composite films of polyvinyl chloride (PVC) and TTTs were produced using a simple solvent casting technique. The PVC films were subjected to UV age testing by exposing them to an ultraviolet aging chamber. The age-resistant performance of the fabricated films was evaluated using an ultraviolet spectrophotometer and Fourier infrared spectrum instrument. The findings suggest that TTTs exhibit a noteworthy capacity for absorbing ultraviolet radiation. The TTTL compound exhibits a superior UV absorption performance compared to commercially available UV absorbers such as UV-0 and UV-327 in the market.
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高影响因子
MOLECULES
·
2022
·Vol. 27
·期 24
·8668
·
IF 4.927
Lilin Yang,Weilin Zhao,Daobei Wang,Yang Liu,Dongzhi Wang,Na Cui
An attempt at the treatment of the waste fiber (WF) from the wind turbine blade (WTB) was made through the modifier of dopamine hydrochloride and the compound modifier of dopamine hydrochloride and 2,5-dihydroxy terephthalic acid or 3,4-dihydroxy cinnamic acid or 3,4-dihydroxy benzonitrile, corresponding to obtain four modified waste fibers (MWF1, MWF2, MWF3, and MWF4). The MWFs samples’ microstructure properties were characterized using SEM, EDS, XPS, FTIR analyses, and water contact angle tests. The results revealed that all the MWF surfaces were wrapped by a distinct coating layer and had different elemental compositions and chemical groups, demonstrating the significant effect of the four modifications on the WF surfaces. The hydroxyl, amino, or nitrile groups were grafted onto the WF surfaces causing improvement of the hydrophilicity and reactivity. Furthermore, all the MWFs as the reinforced materials were incorporated into the industrial waste phosphogypsum (PG) to manufacture the phosphorous-building gypsum composites (PBGC). The effects on the micro-morphology and mechanical properties of the PBGC were evaluated. The results also show the improvement in flexural and compressive strength with the addition of MWFs into the PBGC, due to the enhancement of the compactness between the MWF and phosphogypsum matrix. In particular, the effects of three compound modifiers on the flexural and compressive strength are more significant. The highest flexural and compressive strength was contributed by the PBGC-MWF4 with 2% dosage using a compound modifier of dopamine hydrochloride and 3,4-dihydroxy benzonitrile, which were enhanced 61.04% and 25.97% compared with the PBG.Keywords:waste fiber;wind turbine blade;phosphogypsum;surface treatment
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Polymer Chemistry
·
2022
·Vol. 13
·期 37
·5368-5379
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IF 5.364
Chenru Tian,Haoran Feng,Yuchen Qiu,Ganggang Zhang,Tianwei Tan,Liqun Zhang
Covalent crosslinking and reinforcement are two critical issues in elastomer science and engineering. It remains challenging to achieve green crosslinked and mechanically robust elastomer materials through a facile and efficient strategy. In the present work, a facile and novel strategy for multi-crosslinking network design is proposed to prepare high-performance elastomers based on the amidoxime modification of commercial nitrile–butadiene rubber (NBR). For the first time, we found that amidoxime-functionalized NBR (AO-NBR) shows unique self-crosslinking and self-reinforcing abilities. The hydrogen bonds and metal–ligand coordination bonds arising from amidoxime groups can be formed between the AO-NBR chains. Moreover, AO-NBR could be chemically self-crosslinked based on the reaction between amidoxime groups and nitrile groups without additional additives at elevated temperature, generating the 1,2,4-oxadiazole groups. Based on the inherent properties of AO-NBR, the multi-crosslinking network structures including covalent crosslinking bonds, physical hydrogen bonds, and metal–ligand coordination bonds could be constructed by a simple hot-pressing process and the introduction of zinc ions. What's more, the hydrogen bonds and Zn-based coordination bonds as sacrificial motifs can break prior to covalent bonds with large energy dissipation and undergo reversible breaking and reforming under an external force, which endows the AO-NBR with self-reinforcing ability. Hence, the obtained elastomers show excellent mechanical properties, and their tensile strength, modulus, and toughness are improved simultaneously. Overall, we envisage that this work may open up new avenues to design high-performance elastomers based on a facile self-crosslinking and self-reinforcing strategy.
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Advanced Healthcare Materials
·
2022
·Vol. 11
·期 15
·2200467
·
IF 11.092
Wansu Zhang,Shangyu Chen,Pengfei Sun,Shuai Ye,Quli Fan,Jun Song,Pengju Zeng,Junle Qu,Wai-Yeung Wong
The luminescence of traditional phosphorescence-based hypoxia probes is limited to the visible and first near-infrared wavelength regions (<1000 nm), which has defects of higher light scattering and lower penetration depth in contrast with the second near-infrared wavelength window (NIR-II, 1000–1700 nm) for optical bioimaging. Herein, 5,15-bis(2,6-bis(dodecyloxy)phenyl)-porphyrin platinum(II) (PpyPt) with J-aggregation induced NIR-II phosphorescence is reported. J-aggregates of PpyPt are confirmed by the X-ray diffraction data in the crystalline state. Moreover, the emission and excitation spectra of PpyPt in the solid states reveal NIR-II luminescence feature of PpyPt in J-aggregates. More importantly, by preparation of water-soluble PpyPt nanoparticles (PpyPt NPs 4.76 ) with J-aggregates, it has NIR-II phosphorescent lifetime of microseconds and good oxygen-sensitivity in water. Moreover, the good biological hypoxia-sensing potential of PpyPt NPs 4.76 is demonstrated in cells and 4T1-tumor-bearing mice. This study provides an efficient strategy to design NIR-II phosphorescent probe for sensitive tumor-hypoxia detection through the construction of J-aggregates.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Baoqiang Hao,Yang Guo,Xueling Bai,Renyuan Zhang,Xiaoqing Li,Jing Li
The combined application of chlorination and UV irradiation has the potential to yield important benefits in water treatment. However, much of the fundamental chemistry that governs the behavior of UV/chlorine systems have not been well defined. Cyano-containing pesticides (CNPs) are widely used in agriculture and inevitably enter surface waters and other aquatic environments. In this study, twenty CNPs and their intermediates were investigated to evaluate the formation of disinfection byproducts under chlorination and UV/chlorine systems. It was found that UV/chlorine can significantly enhance the generation of cyanogen chloride (CNCl) and dichloroacetonitrile (DCAN) compared to chlorination alone. The CNCl and DCAN concentrations increased from an average of 0.13 and 0.12 μM during the chlorination alone to 0.85 and 0.41 μM, respectively, when UV 254 light was introduced. The maximum yields of CNCl and DCAN could reach 31.8 % and 7.7 %, respectively. Both the photo-induced • OH and • Cl played a key role in the generation of CNCl and DCAN. Additionally, higher yields of total CNX were observed in the UV/chlorine system in the presence of bromide. Similar results were obtained in the treatment of actual water samples, in which the concentrations of CNCl and DCAN increased by orders of magnitude under UV/chlorine treatment compared to the chlorination alone. The results showed that the cyano group of organic pollutants has a higher potential to be directly converted to toxic CNCl and DCAN under UV/chlorine treatment. The inclusion of this basic chemistry will deepen our understanding of UV/chorine water treatment technologies.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Geliang Xie,Guoqiang Zhu,Yifan Kang,Mingxu Zhu,Qianqian Lu,Chao He,Lujiang Xu,Zhen Fang
Realizing the recovery and valorization of waste polyethylene terephthalate (PET) plastics into value-added products have gained significant importance. This study successfully synthesized aromatic nitriles , specifically terephthalonitrile (TPN), from waste polyethylene terephthalate (PET) plastic through in situ catalytic pyrolysis with urea and γ-Al 2 O 3 catalyst. Based on distributed activation energy model, positive interaction between waste PET and urea is responsible for improved thermal decomposition kinetics. The dosage of urea and pyrolysis temperature significantly influenced TPN production. TPN yield reached 32.5% with ca. selectivity of 85% at 550 °C and equivalent urea dosage. Density functional theory calculations validated the role of active ammonia in reducing energy barriers and thus facilitating PET depolymerization . The study highlights the feasibility of recycling waste PET into valuable aromatic nitriles through in situ catalytic pyrolysis with urea and enhances the understanding of the pyrolysis process.
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ACS Applied Bio Materials
·
2020
·
IF 0
Faming Wang,Pengfei Ren,Katrien V. Bernaerts,Yifu Fu,Wanjun Hu,Naizhen Zhou,Tianzhu Zhang
As one of the nonenzymatic cell-harvesting technologies, a thermal-responsive surface based on poly(2-oxazoline)s has achieved initial success in supporting the adhesion and thermal-induced detachment of animal cells. However, because of the laborious preparation procedure, this technique was only limited to research purposes. In this work, through using poly(glycidyl methacrylate) (PGMA) as the anchor layer, poly(2-propyl-2-oxazoline)s (PPOx) were grafted onto glass wafers through a facile two-step coating and annealing procedure for nonenzymatic cell harvesting. In the first step, the piranha solution-activated glass wafers were immersed into the chloroform solution of PGMA and then annealed for a given period of time to immobilize PGMA onto the glass wafers through the bonding between epoxy groups and hydroxyl groups. In the second step, the PGMA-coated glass wafers were further immersed into the chloroform solution of carboxyl-functionalized PPOx. After annealing, PPOx were immobilized onto the PGMA layer through the bonding between carboxyl groups and the residual epoxy groups. Atomic force microscopy, X-ray photoelectron spectroscopy, and ellipsometry were used to characterize the modified glass wafers. The results of cytocompatibility evaluation showed that the PPOx-coated glass wafers were almost nontoxic and were able to support the adhesion and proliferation of L929 cells well. By lowering the temperature to 8 °C, L929 and Vero cells were successfully detached from the PPOx-coated glass wafers without any enzymatic treatment. Further cultivation has demonstrated that the cooling procedure had little effect on cell viability, and the cells still retained good viability after harvesting.
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PubMed
Materials
·
2020
·Vol. 13
·期 7
·1513
·
IF 3.057
Jialing Kang,Mengjia Wang,Chenbao Lu,Changchun Ke,Pan Liu,Jinhui Zhu,Feng Qiu,Xiaodong Zhuang
Due to the growing demand for energy and imminent environmental issues, hydrogen energy has attracted widespread attention as an alternative to traditional fossil energy. Platinum (Pt) catalytic hydrogen evolution reaction (HER) is a promising technology to produce hydrogen because the consumed electricity can be generated from renewable energy. To overcome the high cost of Pt, one effective strategy is decreasing the Pt nanoparticle (NP) size from submicron to nano-scale or even down to single atom level for efficient interacting water molecules. Herein, atomically dispersed Pt and ultra-fine Pt NPs embedded porous carbons were prepared through the pyrolysis of Pt porphyrin-based conjugated microporous polymer. As-prepared electrocatalyst exhibit high HER activity with overpotential of down to 31 mV at 10 mA cm−2, and mass activity of up to 1.3 A mgPt−1at overpotential of 100 mV, which is double of commercial Pt/C (0.66 A mgPt−1). Such promising performance can be ascribed to the synergistic effect of the atomically dispersed Pt and ultra-fine Pt NPs. This work provides a new strategy to prepare porous carbons with both atomically dispersed metal active sites and corresponding metal NPs for various electrocatalysis, such as oxygen reduction reaction, carbon dioxide reduction, etc.Keywords:platinum;atomically dispersed active site;nanoparticle;porous carbon;hydrogen evolution reaction
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Analytical Methods
·
2021
·Vol. 13
·期 30
·3414-3423
·
IF 2.896
Qingyu Xu,Hongju Chen,Shaoqing Ye,Yongming Zeng,Hongmei Lu,Zhimin Zhang
Raman spectroscopy can provide structural fingerprints to identify molecules by means of spectral library searching. However, it is difficult to share the spectral library between different Raman spectrometers because of the nonlinear displacement in Raman shift. In this study, we propose a Raman spectra Standardization method using Variable Penalty dynamic time warping (RS-VPdtw), which can synchronize the nonlinear displacement between spectra acquired with different spectrometers. We have compared the standardization performance of RS-VPdtw and MWFFT on the spectra of 13 real samples acquired with 6 different spectrometers. The mean spectral similarity of RS-VPdtw and MWFFT increased from 0.79 to 0.97 and 0.91 respectively. Results show that RS-VPdtw is significantly better than MWFFT in Raman spectra standardization. The Raman spectra acquired with different spectrometers can be standardized by RS-VPdtw to search the same spectral library, which can avoid the time-consuming and labor-intensive reestablishment of spectral libraries for different spectrometers. This means that RS-VPdtw is a promising and valuable method to solve the spectra standardization problem in large-scale applications of Raman spectroscopy.
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JOURNAL OF MOLECULAR CATALYSIS B-ENZYMATIC
·
2013
·
IF 2.823
Xiaolin Pei,Lirong Yang,Gang Xu,Qiuyan Wang,Jianping Wu
Microbial nitrile hydratases (NHases) are important industrial catalysts to produce valuable amides. However, only some NHase genes have been reported and studied at the molecular level. In this study, we developed a genome mining method to discover Fe-type NHases from GenBank. The putative NHase gene from Pseudomonas putida F1 was cloned and functionally expressed in Escherichia coli BL21 (DE3) by assisting of a putative activator gene adjacent to β-subunit region. Three recombinant plasmids containing NHase gene or the activator gene were designed and constructed. Maximal enzyme activity was obtained when the structural and activator genes were transcribed as one unit in plasmid pCDFDuet-1 at 18 °C. However, the expressed product did not show any NHase activity when the downstream activator gene was ignored, and the product completely existed in insoluble inclusion body. The activator gene might be involved in protein folding of the α- and β-subunits of NHase. In addition, the Fe-type NHase exhibited broad substrate specificity. The enzyme can efficiently hydrate aromatic nitriles, such as 3-cyanopyridine, 4-cyanopyridine, and benzonitrile, asides from aliphatic nitriles preferentially. Therefore, the recombinant NHase shows potential applications in some amides preparation.
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