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Energy & Environmental Science · 2024 · IF 32.4

Harnessing trace water for enhanced photocatalytic oxidation of biomass-derived alcohols to aldehydes

Wenhua Xue,Jian Ye,Zhi Zhu,Reeti Kumar,Jun Zhao

The photocatalytic conversion of biomass into valuable chemicals offers a more energy-efficient and low-carbon alternative to traditional thermal catalysis, representing a promising strategy for fine chemical production without relying on fossil fuels. While most studies have focused on catalyst design to improve efficiency, the precise tuning of solvents has been neglected. This study examines the conversion of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) as a representative biomass alcohol oxidation reaction, revealing a novel strategy for enhancing photocatalytic efficiency through solvent fine-tuning. The introduction of minute quantities of water into an acetonitrile solvent matrix during the HMF oxidation reaction was observed to engender pronounced enhancements in catalytic performance, with the degree of effect contingent on precise water concentration. Trace water is an active participant in the catalytic cycle, diminishing the activation energy barrier for bond cleavage and averting catalyst deactivation. This mechanism also proved applicable to other photocatalysts and various alcohol substrates, highlighting the potential of this strategy for enhancing photoenergy utilization and reaction efficiency.

研究领域: 化学工程 · 可再生能源 · 催化科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

Highly crystalline covalent organic frameworks for ratiometric fluorescent sensing of trace water in honey and N2 gas

Cong Guan,Jiaming Cai,Xiaotao Liu,Liangqia Guo

The detection of trace water (H 2 O) content is important and challenging in food and food-related industries. Herein, highly crystalline two-dimensional covalent organic frameworks (TAPT-BTCA-COF) with yellow-green fluorescence were prepared by using 1,3,5-tris(4-aminophenyl)triazine (TAPT) and 1,3,5-benzenetricarboxaldehyde (BTCA) as precursors. The fluorescence of TAPT-BTCA-COF is sensitive to the solvent polarity due to the intermolecular charge transfer (ICT) effect and can be quenched by trace H 2 O due to the block of ICT effect by H 2 O. On this base, TAPT-BTCA-COF is applied for sensing of trace H 2 O in common organic solvents such as DMF, acetonitrile , THF and acetone with fast response and high sensitivity. The limits of detection for H 2 O in DMF, acetonitrile, THF and acetone are 0.082 wt%, 0.0053 wt%, 0.0091 wt% and 0.0061 wt%, respectively. Furthermore, a ratiometric fluorescent sensor is proposed by using TAPT-BTCA-COF as the signal probe and red fluorescent tris(2,2′-bipyridyl)ruthenium(II) dichloride as the reference and successfully applied for quantitatively and semi-quantitatively sensing of trace H 2 O in honey sample and the moisture in N 2 gas.

CAS / MDL: 1314-56-3
研究领域: 材料科学 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Dependence of ε-caprolactone selectivity on diffusion performance over Sn-Beta zeolite catalyst for Baeyer-Villiger oxidation of cyclohexanone

Xiaolong Liu,Jiahe Sun,Shuo Li,Kaixuan Yang,Ting Su,Hongying Lü,Zhiguo Zhu

Sn-containing zeolite catalysts exhibit the unique feature of selectively activating carbonyl groups in organic compounds, which demonstrate relatively high activity and selectivity in the Baeyer-Villiger (B V) oxidation of aldehydes or ketones using H 2 O 2 as the oxidant. However, the influence of diffusion property and trace water on the ε-caprolactone selectivity as targeted product in the cyclohexanone's B V oxidation system with the green oxidant of aqueous H 2 O 2 remains unclear. To address this, three kinds of Sn-Beta zeolites are prepared by interzeolite transformation, structural reconstruction, and post-synthesis method to establish structure-property relationships. The physicochemical property and Sn coordinated state are investigated in detail. The existence of trace water in the reaction system negatively affects the conversion and product selectivity by competitive adsorption of water with reaction substrates and facilitated hydrolysis of ε-caprolactone, respectively. DFT calculation implies that kinetics dominates the conversion of cyclohexanone → ε-caprolactone → 6-hydroxycaproic acid. The structure-property relationship indicates that the cyclohexanone conversion and ε-caprolactone selectivity are closely related to the adsorption amounts of substrates and the diffusion performance of products, respectively, over Sn-Beta zeolite catalysts. Finally, the reusability and deactivation mechanism are analyzed. This study aims to provide guidance for designing efficient stannosilicate zeolite catalysts for B V oxidation through precisely modulating the zeolite's diffusion property.

CAS / MDL: 112-40-3 12125-01-8
研究领域: 催化化学 · 材料科学 · 有机化学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Ultrafast Visual Detection of a Trace Amount of Water by Highly Efficient Hybrid Manganese Halides

Jie Zhang,Meng-Ping Ren,Man Xu,Zhonghui Zhang,Mingxue An,Yang Lu,Xiao-Wu Lei,Zhongliang Gong,Cheng-Yang Yue

A quantitative water detection method is urgently needed in storage facilities, space exploration, and the chemical industry. Although numerous physical techniques have been widely utilized to determine the water content, they still suffer from many disadvantages such as highly expensive special instruments, complicated analysis processes, etc. Hence, a convenient, rapid, and sensitive water analysis method is highly desirable. Herein, we developed a visual fluorescence sensing technology for water detection based on reversible PL off-on switching of organic–inorganic hybrid zero-dimensional (0D) manganese halides. In this work, a family of hybrid manganese halides were synthesized through a facile solution method, namely, [NH4(18-Crown-6)]2MnBr4, [Ca(18-Crown-6)·3H2O](18-Crown-6)MnBr4, [NH4(dibenzo-18-Crown-6)]2MnBr4, and [Ca(dibenzo-18-Crown-6)·2H2O]MnBr4. Excited by UV light, these highly crystalline manganese halides exhibit strong green light emissions from the d–d electron transition of Mn2+ with near-unity photoluminescence quantum yield and submillisecond lifetime. Benefiting from the dynamic and weak ionic bonding interactions, these 0D manganese halides display reversible water-response on/off luminescence switching but fail in any other aprotic solvents. Therefore, these 0D hybrid manganese halides can be explored as ultrafast visual fluorescence probes to detect the trace amount of water in organic solvents with multiple superiorities of rapid response time (< 2 s), ultralow detection limit (9.71 ppm), excellent repeatability, etc. The reversible water-response luminescent on/off switching also provides a binary optical gate with advanced applications in anticounterfeiting and information security, etc.

研究领域: 材料科学 · 化学工程
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DYES AND PIGMENTS · 2019 · IF 4.018

An AIE dye based smartphone and LDA integrated portable, intelligent and rapid detection system as trace water indicator and cyanide detector

Linfeng Chen,Xike Tian,Yong Li,Chao Yang,Liqiang Lu,Zhaoxin Zhou,Yulun Nie

Portable, rapid, accurate and on-site detection of analysis target has always been the goal of continuous efforts in the field of analysis. In this work, a novel intelligent and rapid detection system based on an AIE dye (TPA-DCV) was established for portable and on-site detection of trace water in organic solvents and CN − in water by integrating the smartphone and linear discriminant analysis (LDA). The TPA-DCV displayed remarkable solvatochromism effect and showed different fluorescence colors to different water contents of different solvents, with the minimum detection limit of 54 ppm. In addition, TPA-DCV also exhibited specific response to CN − , and showed significant fluorescence changes to different amounts of CN − . With the assist of this detection system, these different fluorescence color signals could be accurately classified in canonical score plot. What's more, the classification and distribution of fluorescence color in canonical score plot showed regular change with the target concentration, which could be used to quantify the trace water and CN − . The rationality and practicability of this detection system were preliminary verified by a large number of real sample analyses. This detection system greatly simplifies the analysis process, which is in the proof of intelligent and rapid detection just using a simple color analysis without any instrument test, which may be a big step forward.

研究领域: 分析化学 · 环境科学 · 生物医学工程
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DYES AND PIGMENTS · 2021 · IF 4.889

Room-temperature phosphorescence based on chitosan carbon dots for trace water detection in organic solvents and anti-counterfeiting application

Yeyan Ni,Pingyan Zhou,Qiwen Jiang,Qi Zhang,Xingyu Huang,Yi Jing

Trace water is known to be an impurity in organic solvents , having an adverse effect on the chemical reaction or environmental safety. Developing a green, facile and non-toxic method for detecting trace water in various organic solvents is still a challenge. Distinct form conventional fluorescent probes , room-temperature phosphorescence (RTP) test paper (TP) has aroused wide concern owing to its characteristic optical performance, including long afterglow and non-background interference. Herein, we fabricated a new kind of RTP-TP on the basis of chitosan carbon dots (CDs). The anchoring effect of polyvinyl alcohol (PVA) promoted the restriction of vibration/rotation and hindered the non-irradiative quenching of CDs by forming intermolecular hydrogen bonds . However, water molecules could interrupt these hydrogen bonds and therefore the RTP phenomenon would be disappeared. Further, the RTP-TP was used to detect trace water in various organic solvents with high efficiency, excellent stability, and reliability. In addition, the CDs-PVA solution can be also used as anti-counterfeiting ink via various printing methods.

研究领域: 材料科学 · 分析化学 · 环境科学
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Nano Research · 2020 ·Vol. 13 ·期 10 ·2803-2811 · IF 8.183

Construction of self-sensitized LiErF4: 0.5% Tm3+@LiYF4 upconversion nanoprobe for trace water sensing

Zhang Ling,Li Xiaodan,Wang Wang,Zhao Xu,Yan Xu,Wang Chenguang,Bao Haoqiang,Lu Yang,Kong Xianggui,Liu Fengmin,Liu Xiaomin,Lu Geyu

LiErF 4 was commonly used as a dipolar-coupled antiferromagnet, and was rarely considered as a luminescent material. Herein, we achieved the strong red upconversion emission of LiErF 4 simply by an inert shell coating, i.e., LiErF 4 @LiYF 4 . Owing to the unique and intrinsic ladder-like energy levels of Er 3+ ions, this LiErF 4 core-shell nanostructures present red emission (∼ 650 nm) under multi-band excitation in the near-infrared (NIR) region (∼ 808, ∼ 980, and ∼ 1,530 nm). A brighter and monochromic red emission can be further obtained via doping 0.5% Tm 3+ into the LiErF 4 core, i.e., LiErF 4 : 0.5% Tm 3+ @LiYF 4 . The enriched Er 3+ ions and strong monochromic red emission natures make LiErF 4 : 0.5% Tm 3+ @LiYF 4 nanocrystals very sensitive for trace water probing in organic solvents with detection limit of 30 ppm in acetonitrile, 50 ppm in dimethyl sulfoxide (DMSO), and 58 ppm in N , N -dimethylformamide (DMF) under excitation of 808 nm. Due to their superior chemical and physical stability, these nanoprobes exhibit excellent antijamming ability and recyclability, offering them suitable for real-time and long-term water monitoring.

CAS / MDL: 1310-65-2
研究领域: 材料科学 · 分析化学 · 纳米技术
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2018 · IF 2.88

Colorimetric and fluorometric dual sensing of trace water in methanol based on a Schiff Base-Al3+ ensemble probe

Jia Feng,Li Xin Duan,Zhuo Bin Shang,Jian Bin Chao,Yu Wang,Wei Jun Jin

A new julolidine based Schiff base receptor (L) was synthesized and characterized. L forms a 1:1 complex with Al 3+ in methanol, resulting in an immediate color change from chartreuse to orange and a remarkable enhancement in its emission intensity along with a bathochromic shift from 540 nm to 570 nm. Addition of trace amounts of water significantly quenches the fluorescence emission , where a decomplexation of Al 3+ from the L-Al 3+ complex takes place. The significant quenching effect indicated that the L-Al 3+ ensemble system can be used to detect trace water in commercial methanol. From the fluorescence titration, the detection limit for sensing water in methanol was estimated to be 0.0047%. We have also made an easy-to-prepare test strip of L-Al 3+ to detect water in methanol through naked-eye observation, which is possible to realize in situ monitoring.

CAS / MDL: 5351-69-9
研究领域: 分析化学 · 材料科学
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ANALYST · 2018 ·Vol. 143 ·期 13 ·3068-3074 · IF 3.864

Ratiometric fluorescence detection of trace water in organic solvents based on aggregation-induced emission enhanced Cu nanoclusters

Shanliang Song,Yuping Zhang,Yizhou Yang,Chuanxi Wang,Ying Zhou,Chuan Zhang,Yueqi Zhao,Minghui Yang,Quan Lin

A fast, sensitive, and convenient dual-emission water detector was robustly fabricated. This detector was prepared with blue fluorescent carbon dots (CDs) and red fluorescent Cu nanoclusters (NCs), and showed two well-resolved and intensity-comparable fluorescence peaks under a single excitation wavelength. Moreover, it showed strong red fluorescence in organic solvent due to the aggregation-induced emission enhancement (AIEE) properties of the Cu NCs, but the red fluorescence was gradually quenched with an increasing amount of water, whereas the blue fluorescence remained constant. The differences in response result in a continuous fluorescence color change from red to blue that can be clearly observed by the naked eye. Thus, as-prepared Cu NC-based dual-emission nanomaterials can be used for ratiometric fluorescence detection of trace amounts of water in organic solvents by taking advantage of the water sensitivity of their fluorescence intensity ratios (red/blue) and their low detect limits (<0.02% v/v). These studies demonstrate that a novel and sensitive dual-emission ratiometric water detector has been found, which shows promise for application in environmental monitoring, food inspection, and life science.

研究领域: 分析化学 · 材料科学 · 环境科学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Detection of Trace Water Based on Electro-oxidation of Molybdenum Disulfide Nanomaterials to Form Molybdenum Oxysulfide

Di Liu,Yixuan Bian,Zhiwei Zhu,Yuanhua Shao,Meixian Li

Molybdenum disulfide nanomaterials nowadays are very popular in electrocatalysis field due to their outstanding catalytic performance toward many electrochemical reactions. However, the electrochemical oxidation reaction of molybdenum disulfide nanomaterials in the range of positive potential has not been studied thoroughly. Herein, we have investigated electro-oxidation of molybdenum disulfide nanomaterials and put forward a new reaction mechanism: molybdenum disulfide nanomaterials are electro-oxidized with water to form molybdenum oxysulfide (MoOS2) and hydrogen ions, leading to the release of hydrogen on the counter electrode. Various characterization methods such as contact angle measurement, scanning electron microscope (SEM), transmission electron microscope (TEM) with energy dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), X-ray absorption near edge structure (XANES) spectroscopy, time-of-flight secondary ion mass spectrometry (ToF-SIMS), and gas chromatography (GC) were applied to attest the doping of oxygen and the generation of hydrogen. Based on this reaction, we constructed a novel ultrasensitive electrochemical sensor for detecting trace water with the minimum detectable content of 0.0010% (v/v) in various organic solvents and ionic liquids, which is comparable to the Karl Fischer titration, but with much simpler reagent.

研究领域: 材料科学 · 分析化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Multi-functional lanthanide coordination polymers for multi-modal detection of nitroaromatics and trace water in organic solvents

Yong-Mei Wang,Ying Xu,Zhong-Rui Yang,Xinxin Zhang,Ying Hu,Rusen Yang

Multifunctional materials used for multimodal sensors are of great significance both for enriching variety of materials and overcoming the shortcomings of traditional single signal sensors. This work reports the ultrafast preparation of multifunctional coordination polymer (CP) spheres with metalloligand Ru (II)[4,4′-(COOH) 2 -bpy] 3 ▪Cl 2 ( L ) and Gd 3+ ions. Gd- L CPs were used for multi-modal detection of nitroaromatic explosives and trace water in organic solvents with their red fluorescence and magnetic resonance response. The red fluorescence was derived from the ligand, which is electron-rich because of the bipyridine rings. There were different emission behaviors when Gd- L CPs reacted with nitroaromatic explosives that have various electron-deficient properties through electron transfer donor–acceptor mechanism. The changes in the emission depended closely on the nitroaromatic explosives ability to withdraw electrons. Gd- L CPs also showed magnetic resonance response with r 1 of 12.1 mM −1 s −1 due to the integration of the paramagnetic property of Gd 3+ ions. Smart sensing of trace water in organic solvents was achieved by magnetic signals. The fluorescence of Gd- L CPs was enhanced and there was a tiny blue-shift in protonic solvents with increased polarity. The fluorescence sensor used in detecting trace water had a consistent result like the MR response. Thus, Gd- L CPs enabled the use of fluorescence and magnetic resonance sensors simultaneously for the first time to overcome the shortcoming of single modal sensor and expand the application of magnetic resonance relaxation.

CAS / MDL: 13450-84-5
研究领域: 材料科学 · 化学传感 · 环境监测
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Multifunctional luminescent switch based on a porous PL-MOF for sensitivity recognition of HCl, trace water and lead ion

Xin Xu,Huijun Li,Zhouqing Xu

The development of multifunctional luminescent switch for the detection of different targets is highly desirable because of the complexity of the environment. In this paper, novel porous fluorescent Metal–Organic Framework (HPU-23), which can visually detect gaseous hydrogen chloride (HCl) and trace water from organic solvents through the fluorescence quenching phenomena, are designed. Besides, after the fluorescence of HPU-23 quenching by HCl, HPU-23 can be reopened by gaseous triethylamine (TEA) treatment. HPU-23 also could detect trace water from organic solvents. Although the quenching of fluorescence is also observed, the sensor after sensing H 2 O cannot be regenerated by any treatment. Besides, another Pb 2+ sensor is obtained when a new luminophore, i.e., tris(2,2′-bipyridine) dichlororuthenium(II) hexahydrate (Ru(bpy) 3 2+ ), is added into an aqueous system containing HPU-23. Therefore, our strategy is a promising broadcast for the development of multifunctional sensors.

研究领域: 材料科学 · 分析化学
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