ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Mei Ma,Jia-qi Bai,Huangfei Liu,Ben Liu,Zhangkai Qian,Suiqin Li,Jingshuai Chen,Mengdie Cai,Song Sun
The preparation of methyl-substituted amines by direct N-methylation of amines with CO2/H2 is an important reaction for CO2 utilization and organic synthesis. However, the design and construction of effective and stable non-noble-metal catalysts for this reaction remain challenging. Here, a cheap non-noble-Cu-based catalyst was prepared and applied in the direct N-methylation reaction of N-methylaniline with CO2 and H2. 5%Cu-ZnO(3.75%)/TiO2 showed 98.8% yield with an initial TOF of 7.7 h–1 after 24 h under 453 K, 1.5 MPa CO2, and 4.5 MPa H2, which was superior to 5%Cu/TiO2, 5%Cu/ZnO, and reported Cu-based catalysts. Furthermore, 5%Cu-ZnO(3.75%)/TiO2 can be reused at least four times and applied to the direct N-methylation of various amines with excellent selectivity. The various characterizations and experimental results showed that Cu0 was the active site, and 5%Cu-ZnO(3.75%)/TiO2 exhibited the largest surface Cu0 amount, thereby contributing to superior catalytic performance. The reaction mechanism of the direct N-methylation reaction of N-methylaniline with CO2 and H2 was proposed based on spectroscopic studies, kinetic studies, and control experiments. The reaction proceeded with the HCHO and N-methylformanilide intermediates, and the formation of HCHO from H2 and CO2 was the rate-determining step.
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ACS Nano
·
2024
·
IF 15.8
Jixi Zeng,Jing Wang,Jinzhao Wang,Jia Li,Jiwen Chen,Feng Wei,Jing Zhang,Weijie Song,Xi Fan
Flexible tin–lead (Sn–Pb) mixed perovskite solar cells (PSCs) are among the promising flexible photovoltaics, owing to the narrow bandgap (NBG) of Sn–Pb perovskites, flexible and wearable features, and their role as a critical component in all-perovskite tandem photovoltaics. However, the flexible Sn–Pb PSCs suffer from a low power conversion efficiency, no higher than 18.5%, along with limited stability. Herein, we reported an efficient and stable flexible NBG Sn–Pb PSC via an N,N′-carbonyldiimidazole (CDI) passivation strategy. CDI, with strong adsorption energy, preferentially binds to Sn2+ compared with oxygen (O2), thus effectively inhibiting the adsorption of O2 on perovskite surfaces. The transfer of electron density around Sn2+ dramatically decreased, thus suppressing Sn2+ oxidation. The CDI treatments endowed the Sn–Pb mixed films with fewer defects, improved crystallinity, better morphology, and matched energy-level alignment. The flexible Sn–Pb devices exhibited a high PCE of 21.02%. Besides, the devices showed enhanced stability and promoted flexibility. This work provides a pathway to visibly increase the efficiency and stability of the flexible Sn–Pb mixed photovoltaic cells.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xin Wang,Yubing Xu,Yuzhu Pan,Shunjie Chai,Jie Wu,Jingda Zhao,Yuwei Li,Zhiwei Zhao,Qing Li,Jun Wu,Jing Chen,Byung Seong Bae,Jianming Zhou,Ying Zhu,Wei Lei,Xiaobao Xu
Solution-processed lead halide perovskite single crystals (LHPSCs) are believed to have great potential in gamma-ray spectroscopy. However, obtaining low-defect LHPSCs from a solution at low temperatures is difficult compared to obtaining Bridgman single crystals such as CdTe and Si. Herein, noise from the intrinsic defects of LHPSCs is considered as the main problem hindering their gamma-ray detection performance. By isolating the defect-induced holes in LHPSCs via energy barriers, we show that NIN photodiodes based on three types of LHPSCs, i.e., MAPbBr3 (MA = CH3NH3), MAPbBr2.5Cl0.5, and cascade LHPSCs, have demonstrated good energy resolution in the range of 6.7–10.3% for 662 keV 137Cs gamma-ray photons. The noise for >10 mm3 devices is low, in the order of 340–860 electrons, and the electron collection efficiency reaches 23–43%. These results pave the way for obtaining low-cost, large, high energy-resolution gamma-ray detectors at room temperature (300 K).
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
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
·
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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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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FOOD CHEMISTRY
·
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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CRYSTENGCOMM
·
2013
·Vol. 15
·期 32
·6368-6373
·
IF 3.879
Shuling Xu,Lei Wang,Haibo Li,Qiaoli Yue,Rui Li,Jifeng Liu,Xiaohong Gu,Shuqiu Zhang
Novel three-dimensional Ag nanoflowers (3DAN) were successfully synthesized through a facile Cu2+ mediated solution method using N,N-dimethylformamide (DMF), which serves as both a reducing agent and a solvent at room temperature. It was found that the introduction of a trace amount of Cu2+ could greatly slow the rate of the Ag+ reaction and thus this process effectively reduced the growth speed of Ag nanoparticles allowing 3DAN to be formed. The mechanism underlying the self-assembly process and shape evolution of 3DAN were systematically investigated by varying reaction time. X-Ray powder diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM) and high-resolution transmission electron microscopy (HRTEM) were used to characterize the structure and morphology of the obtained products. X-Ray photoelectron spectroscopy (XPS) was used to assess the chemical state and surface composition of the 3DAN. UV-vis absorption spectra of the products collected from the reaction solution at various stages were taken to study their optical properties. In the measurement of surface-enhanced Raman scattering using rhodamine 6G (R6G) as the probe, the 3DAN exhibited a significant enhancement factor, indicating their potential applications in biosensing and nanodevices.
研究领域:
纳米医学
·
生物传感
·
材料科学
·
胶体化学
·
分子影像学
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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
·
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
·
环境监测
·
传感器技术
·
纳米材料
·
分析化学
·
半导体器件
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