Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
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IF 15.7
He Yingchun,Ma Dong-Dong,Ma Ke,Li Xiaofang,Han Lili,Wu Xin-Tao,Zhu Qi-Long
Electrochemically constructing C–N and N–C–N bonds provides an economical and sustainable alternative to conventional chemosynthesis. Herein, a hierarchically ordered open superstructure of N-doped carbon isolated with accessible three-coordinated Zn single-atom sites is explored for efficient electrocatalytic N–C–N coupling. Benefiting from the distinctive structural merits, this catalyst enables electrocatalytic preparation of N–C–N bonded compounds from methanol and amines. Notably, the Faradaic efficiency and selectivity of N,N,N’,N’ -tetramethyldiaminomethane reach up to 77% and 96% at 0.8 V, respectively. Further integrating the aminoalkylation reaction, an electro-thermo cascade synthesis is explored with the electrochemically obtained N,N,N’,N’ -tetramethyldiaminomethane serving as a unique reagent, leading to a specific set of organonitrogen compounds with (dimethylamino)methyl substituent, including topotecan hydrochloride, an anti-tumor drug, with a high yield of 95%. Furthermore, the in situ spectroscopic characterization and calculations unveil that the under-coordinated Zn-N 3 sites play a pivotal role in stabilizing the key *CH 2 O intermediate, thereby facilitating subsequent nucleophilic addition with amines.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Sarula Li,Zheyan Hu,Tianqi Wang,Fang Song,Hong Shao,Feng Li,Xiangting Dong
Triethylamine (TEA) gas is a kind of toxic gas that can lead to health problems. In this work, a novel Janus structure nanofibers (NFs) have been synthesized via a parallel electrospinning method. SnO 2 and In 2 O 3 are selected as the components of the Janus structure and different ratios of SnO 2 and In 2 O 3 in Janus structure are regulated. To investigate its TEA sensing application, gas sensors have been fabricated and the concentration of TEA gas is set at 20 ppm. The gas sensing results indicate that the optimum ratio of SnO 2 to In 2 O 3 is 1:1 and the gas sensors exhibit good sensing performances including a good response (8.45), short response time (4 s), high signal-to-noise ratio (4.45) and stable reproducibility. The improved gas sensing performances can be attributed to the n-n type Janus heterostructure interface. This research may make contributions to the development of semiconductor heterostructure sensing materials and gas sensors.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 23
·7208-7218
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IF 6.177
Wenjing Song,Yujie Wan,Yuefeng Li,Xin Luo,Weiping Fang,Quanxing Zheng,Pengfei Ma,Jianping Zhang,Weikun Lai
Low cost and high efficiency catalysts for the reductive amination of carbonyl compounds are critical to the utilization of renewable biomass. In this paper, a highly efficient N-doped porous carbon supported Ni catalyst was prepared by a template-assisted pyrolysis and impregnation method. In the presence of NH3 and H2, the as-prepared catalyst could effectively catalyze the reductive amination of various carbonyl compounds into corresponding primary amines with high yield and excellent stability. Comprehensive characterization demonstrated that the reductive amination of furfural towards furfuryl amine was linked to the formation of Ni–Nx sites and the electronic interaction of N and Ni species on the N-doped carbon surface, which promoted the reductive amination of CO bonds and significantly reduced the activation energy in reductive ammonolysis of trimers and Schiff base intermediates. This work provided a new insight into rational design of reductive amination catalysts for primary amine production.
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JOURNAL OF MEMBRANE SCIENCE
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2011
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IF 3.673
Xiao-Lin Li,Li-Ping Zhu,You-Yi Xu,Zhuan Yi,Bao-Ku Zhu
A novel method for the preparation of hydrophilic and positively charged nanofiltration (NF) membranes was developed. An active top-layer with NF characteristic was composited onto polysulfone (PSf) ultrafiltration substrate by UV-induced graft polymerization of N , N -dimethylaminoethyl methacrylate (DMAEMA) followed by quaternization cross-linking with p -xylylene dichloride (XDC). Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and atomic force microscopy were employed to monitor membrane surface chemical and morphological changes after poly(DMAEMA) grafting and quaternization cross-linking. The influences of UV irradiation time, monomer DMAEMA concentration, the cross-linker XDC concentration on the separation and permeation properties of membrane were investigated. The surface hydrophilicity of the composite membranes was evaluated by contact angle measurement. It was found that membrane hydrophilicity was obviously enhanced after UV-induced grafting and quaternization cross-linking. As the UV irradiation time and DMAEMA monomer concentration were increased, salts rejection of the composite membranes increased while water permeability decreased. Under the optimized preparing conditions, water flux and MgCl 2 rejection (1.0 g/L) of the composite membranes reached 60.3 L/(m 2 h MPa) and 93.2%, respectively. The membrane surface charge property was measured via a streaming potential method. It was found that, at pH from 4.5 to 9, the composite membranes showed positive zeta potentials. The rejections of the composite membranes to different salts followed the order Na 2 SO 4 < NaCl < MgSO 4 < MgCl 2 < CaCl 2 . Moreover, the composite NF membranes showed a good stability in water-phase filtration process.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 6
·125570
·
IF 7.5
Yan Zhang,Guannan Ren,Hongfen Zuo,Mingjia Liao,Ningrui Zhang,Zhou Xu,Genghao Gong
An interlayer regulates organosilica deposition on porous polymer supports. • A 150 nm organosilica layer was obtained after two spray cycles. • The membrane achieved a flux of about 1.0 kg m⁻² h⁻¹ for DMF dehydration. • The membrane maintained relatively stable performance over 50 h. Pervaporation dehydration of N,N-dimethylformamide (DMF) is challenging because low-viscosity organosilica sols can penetrate porous polymer supports during selective-layer deposition. In this work, a polyarylate (PAR) interlayer was introduced onto a porous poly(ether ether ketone) (PEEK) support by interfacial polymerization to regulate the deposition of a bis(triethoxysilyl)ethane (BTESE)-derived organosilica layer by ultrasonic spray coating. Cross-sectional SEM observations showed that the PAR interlayer reduced BTESE-sol penetration into the porous PEEK support and facilitated the formation of a relatively thin BTESE-derived layer. The selected membrane prepared with two spray-coating cycles exhibited a BTESE-layer thickness of approximately 150 nm. For a 90 wt% DMF/water feed at 50°C, the membrane achieved a total permeation flux of approximately 1.0 kg m⁻² h⁻¹ with a separation factor of 3–4. During 50 h of continuous operation, the permeation flux decreased initially and subsequently remained relatively stable, while the separation performance showed no pronounced deterioration under the tested conditions. Additional pervaporation experiments with NMP/water and DMAc/water mixtures showed different permeation and separation behaviors. Overall, the results indicate that the PAR interlayer can regulate BTESE-sol deposition on the porous PEEK support and facilitate the fabrication of a thin organosilica composite membrane for pervaporation dehydration under the investigated conditions. Download: Download high-res image (287KB) Download: Download full-size image
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Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 21
·5663-5672
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IF 7.779
Qixuan Qin,Asu Li,Yizhuo Fan,Xindong Zhang
In this work, Au nanoparticle-loaded ZnO/ZnFe2O4 (Au-ZnO/ZnFe2O4) microspheres were prepared using a combination of a two-step hydrothermal process and a co-precipitation method. The SEM and TEM analyses showed that the synthesized Au-ZnO/ZnFe2O4 samples were microspheres with a yolk–shell structure assembled from nanosheets. Gas-sensitive performance tests indicated that Au-ZnO/ZnFe2O4 showed the highest response to 100 ppm acetone (18.18), higher than those of ZnFe2O4 (8.4) and ZnO/ZnFe2O4 (11.6). In addition, the optimum operating temperature of Au-ZnO/ZnFe2O4 decreased from 279 to 206 °C compared to ZnFe2O4 and ZnO/ZnFe2O4. In addition, Au-ZnO/ZnFe2O4 yolk–shell microspheres exhibited fast response and recovery times (4 and 23 s, respectively). The sensor has a lower limit of acetone detection (0.7 ppm) at 85% RH and is able to effectively differentiate diabetic patients from healthy subjects by detecting acetone in their exhaled breath. The enhanced response of Au-ZnO/ZnFe2O4-based sensor is attributed not only to its high specific surface area but also to the synergistic effect of the n–n heterojunction structure of ZnO-ZnFe2O4 and the catalysis of Au nanoparticles.
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FOOD CHEMISTRY
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2025
·
IF 9.8
Zhuoning Cao,Chengqiang Li,Hong Jiang,Francesco Secundo,Xiangzhao Mao
β- N -acetylhexosaminidases garnered attention in the enzymatic synthesis of lacto- N -triose II (LNT2) as the backbone precursor of human milk oligosaccharides (HMOs). In this study, β- N -acetylglucosaminidases Hex(Sv)-2557 from Streptomyces violascens ATCC 27968 was engineered based on a stabilizing intermediate strategy to improve its transglycosylation activity for LNT2 synthesis. A mutant Hex(Sv)-2557(D297K) with a transglycosylation activity of 38.4 U/mg with p NP-GlcNAc −1.9-fold higher than that of Hex(Sv)-2557– was obtained and characterized. Instead, the hydrolase activity of the mutant was 73 % lower compared to the wild-type enzyme. Importantly, the mutant can use N -acetyl chitobiose (GlcNAc 2 ) as the donor for LNT2 synthesis. The LNT2 yield of 14.85 % was obtained when the synthetic reaction, catalyzed by the mutant Hex(Sv)-2557(D297K), started from whey powder and GlcNAc 2 -prepared from chitin by chitinase ChiA and ChiB. This study has altered the donor for the action by directed modification and promoting the high-value utilization of whey powder and chitin.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Xiaohong Shang,Qingmei Xing,Xinxin Ji,Fenghe Duan,Chuanpan Guo,Qiaojuan Jia,Shuai Zhang,Bin Hu,Zhihong Zhang
Herein, a robust photoelectrochemical (PEC) immunosensor was constructed based on an n-n heterojunction between a copper-porphyrin-based metal organic framework and Bi 2 S 3 (Bi 2 S 3 @Cu-TPyP) for efficient detection of gentamicin (GEN). The integration of Cu-TPyP features (enhanced electron transfer capability, improved photoabsorption performance, large specific surface area, and high antibody bioaffinity) with Bi 2 S 3 characteristics (narrow bandgap and visible light absorption capacity) established an efficient interfacial architecture. Enhanced separation of photogenerated electron-hole pairs and improved photoelectric conversion efficiency in the Bi 2 S 3 @Cu-TPyP heterojunction contributed to the amplified photocurrent. The immunosensor exhibited an ultralow detection limit of 0.041 fg mL −1 (1.0 fg mL −1 –1.0 ng mL −1 linear range) with high selectivity and validated applicability in analyzing GEN across diverse food matrices. This study establishes a PEC biosensing paradigm enabling ultrasensitive and rapid antibiotic monitoring in food products due to the synergistic signal amplification mechanisms without compromising specificity.
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CHEMICAL RESEARCH IN TOXICOLOGY
·
2026
·
IF 4.1
Naijie Wei,Xiaowen Yan,Mingyue Yu,Rong Li,Zhixin Xiao,Shi Chen,Limin Yang,Qiuquan Wang,Qian Liu,Guibin Jiang
N-(1,3-Dimethylbutyl)-N’-phenyl-p-phenylenediamine Quinone (6PPDQ) not only causes acute mortality in salmon but also induces toxicities in other living organisms. The electrophilic quinone moiety in the 6PPDQ molecular structure can participate in binding to the cysteine residues that ubiquitously exist in protein nucleophiles, which are responsible for its toxicities. Out of the 82 6PPDQ-bonded proteins found in the human model cell line A549 on the sulfhydryl-reactive proteomics platform, which enables the precise identification of covalent binding protein targets of a pollutant, we discovered three 6PPDQ-bonded mitochondrial proteins─NDUS6, COX5B, and ATP5PB─that are involved in mitochondrial dysfunction for the first time. They impede the function of mitochondria, as witnessed by the decreased enzymatic activities of mitochondrial respiratory chain Complexes I (27.63%) and IV (23.11%), the decreased cellular ATP content (19.94%), and the reduced mitochondrial membrane potential (3.2-fold), as well as the elevated mitochondrial ROS level (2.2-fold) under the environmentally relevant 8.9 μg/L 6PPDQ exposure compared to the controls. Our findings provide experimental evidence for elucidating 6PPDQ’s toxicities at the molecular level, and the knowledge learned will enhance the public’s awareness of the adverse impacts of environmental pollution on health.
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Journal of Environmental Sciences
·
2026
·
IF 6.3
Qi Chen,Lingjun Bu,Yangtao Wu,Shumin Zhu,Yuwei Wu,Shiqing Zhou
This study systematically investigates the behaviors and mechanisms of N,N- dichloramine decomposition in new iron pipes (NIP) and corroded iron pipes (CIP). The half-life of N,N -dichloramine in the CIP is orders of magnitude shorter than in the NIP (0.46 min vs. 35.5 h), accompanied by substantial formation of ammonia (0.27 mg/L as NH 3 -N). We demonstrate that the Fe 2+ - N,N- dichloramine complex formed in CIP is a critical factor in catalyzing the decay of N,N -dichloramine and promoting ammonia formation. Density functional calculations confirm that the coordination bond formed between Fe 2+ and N,N -dichloramine effectively lowers the energy barrier for N,N -dichloramine decomposition via the nitrile pathway, thereby promoting ammonia formation. Furthermore, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) provides molecular-level evidence for the Fe 2+ - N,N -dichloramine complex-catalyzed deamination of CHNO compounds to CHO species. These findings suggest that metal-induced decomposition of organic chloramines could trigger unforeseen ammonia release, underscoring the need to account for disinfection strategies in iron-based DWDS.
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SENSORS AND ACTUATORS B-CHEMICAL
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2020
·
IF 7.1
Qi Chen,Jun Li,Wenhui Fu,Yaohua Yang,Wenqing Zhu,Jianhua Zhang
The development of ultrasensitive and down to ppb-level gas sensors for the accurate detection of volatile organic compounds (VOCs) in environmental monitoring is still a bottleneck that urgently needed to be overcome. Here, we report a high-performance N,N -dimethylformamide (DMF) gas sensor based on electrospun InYbO nanofibers field-effect transistor (FET). Owing to the high surface area of nanofibers, the gas sensor exhibits a remarkably high sensitivity of 89–2000 ppb DMF, fast response/recovery time (36/67 s), exceedingly low detection limit of 5 ppb and outstanding selectivity towards DMF against other typical gases as well as excellent stability and reliability. In particular, the developed gas sensor can obtain low theoretical limit of detection (LOD) of 1.18 ppb. Moreover, a possible sensing enhanced mechanism is also proposed and verified utilizing the capacitance-voltage ( C–V ) analysis. This work opens a new route for the electrospun nanofibers FETs as a promising sensing platform to realize high-performance and ultralow-concentration detection gas sensors.
研究领域:
材料科学
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环境监测
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传感器技术
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纳米材料
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分析化学
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半导体器件
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JOURNAL OF MOLECULAR LIQUIDS
·
2016
·
IF 2.74
Mingwei Zhao,Mingwei Gao,Caili Dai,Mingyong Du,Yifei Liu,Chenwei Zou,Jiaping Tao,Xinke Wang,Tao Wang
In this work, we report a simple class of photo-responsive system that consists of cationic surfactant , N -methyl- N -cetylpyrrolidinium bromide (C 16 MPB), and the photoresponsive organic derivative, trans - ortho -methoxycinnamic acid ( trans -OMCA). The system is studied by UV spectra, cryo -transmission electron microscopy, and rheological measurements. C 16 MPB and trans -OMCA in basic aqueous solution can self-assemble to form viscoelastic wormlike micelles . Upon exposure to UV light , OMCA undergoes a photoisomerization from trans to cis , which results in a change of the geometry of the C 16 MPB–OMCA complexes. The wormlike micelles can transform into spherical or rodlike micelles. We hope this study may enrich the understanding of photo-responsive wormlike micelles composed by cationic surfactants and photo-sensitive additives in water.
研究领域:
软物质物理
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胶体与界面科学
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光响应材料
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表面活性剂化学
·
流变学
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