CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhijian Xiao,Wenda Yang,Jing Wang,Shuang Cao,Jingling Yang,Mingshan Zhu
Photocatalysis is a promising technology for removing low concentrations of nitric oxide (NO) from the atmosphere. However, the unsatisfactory photocatalytic NO removal efficiency and the high selectivity for NO 2 in catalysts limit the development of this technology. In this work, we used an in-situ synthesis method to incorporate Cs 3 Bi 2 Br 9 into UiO-66 for efficient and robust photocatalytic NO removal. The Cs 3 Bi 2 Br 9 /UiO-66 catalyst exhibits a 77.6 % NO removal efficiency and low NO 2 selectivity under visible light irradiation at a WHSV of 1,650,000 mL h −1 g −1 , exceeding the efficiencies of Cs 3 Bi 2 Br 9 (36.4 %) and UiO-66 (2.3 %), as well as those of most reported MOF-based photocatalysts. The synergy of weak Lewis acid sites from Cs 3 Bi 2 Br 9 in Cs 3 Bi 2 Br 9 /UiO-66 and the strong Lewis acid sites from UiO-66 promotes the enrichment of NO on the catalyst surface and act as electron traps to induce carrier separation, thereby promoting the generation of O 2 − to achieve high efficiency. This work provides a new idea for the development of catalysts in NO elimination.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2025
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IF 2.4
Yu Lin,Yuanzhuo Ji,Yizhe Zhang,Hualiang An,Qian Zhao,Xinqiang Zhao,Yanji Wang
BACKGROUND Maleic acid (MAc) is a high value-added oxygenic hydrocarbon derivative monomer. The synthesis of MAc from biomass-based furfural is a green process and has important academic research value. Herein, selective catalytic oxidation of renewable furfural to MAc was investigated. RESULTS The effect of using different heteropoly acids as catalyst and different organic acids/H 2 O as solvent was evaluated first, and the ‘phosphomolybdic acid + acetic acid/H 2 O’ composite system with good performance was screened out. Acetate anion acted as free radical acceptor in the reaction to stabilize furfural radical and inhibit the polymerization reaction. Under optimal reaction conditions, the conversion of furfural was 97.8%, and the MAc yield and selectivity were 58.3% and 59.6%, respectively. To further improve the selectivity of MAc, different kinds of Lewis acids were introduced to construct a Brønsted–Lewis dual-acid catalytic system. When Cu(OAc) 2 was as Lewis acid, the MAc selectivity was significantly improved to 72.5% with a furfural conversion of 72.3%. The catalytic mechanism of Brønsted–Lewis dual-acid system was finally clarified. CONCLUSION In this complex system, the synergy of Cu and Mo is responsible for the outstanding catalytic efficiency, where the Mo VI /Mo V redox can be facilitated by the redox of Cu II /Cu I with the assistance of O 2 ; acetate anion can interact with furfural radicals, thereby delaying the chain reaction of free radicals. This process makes the MAc generation reaction more dominant than the polymerization reaction, thus improving MAc selectivity. © 2025 Society of Chemical Industry (SCI).
研究领域:
化学工程
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催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Liangdong Hu,Lian-hua Xu,Chenjun Yang,Longfei Hong,Kai Wu,Sheng Chu,Longlong Ma,Shurong Wang,Rui Xiao,Huiyan Zhang
Lewis acid sites (LASs) are essential for the photocatalytic isomerization of biomass into high-value platform compounds. However, transient changes in the number of LASs in a photocatalytic system have not been clearly documented, often resulting in an inaccurate understanding of their role in isomerization. To address this challenge, in this study, the molecular probes glyceraldehyde was isomerized to 1,3-dihydroxyacetone (DHA, 63.5 % yield , 3 h) and fructose (47.9 % yield , 3 h) on Pt–KC 3 N 4 , with concurrent production of H 2 (233.8 μmol g −1 ). The results of in situ NH 3 –temperature-programmed desorption (TPD) characterization demonstrated that light irradiation induced the formation of transient LASs on Pt–KC 3 N 4 , and the density of acid sites observed in this study differed significantly from that observed in offline data. Furthermore, theoretical calculations demonstrated that photothermal electron redistribution on Pt–KC 3 N 4 is the main factor driving this transient LAS formation. This report describes a unique methodology to explore transient acid sites in isomerization reactions and provides insight into potential applications in the field of photocatalytic biomass valorization.
研究领域:
化学
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可再生能源
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生物质转化
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DOI
高影响因子
MOLECULES
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2025
·Vol. 30
·期 7
·1457
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IF 4.6
Fenfen Guo,Yuxuan Wang,Zhicheng Jiang,Youjing Tu,Ruikai Li,Xingyu Zhang,Aoyi Tang,Yuan Liang,Lishi Yan,Hu Luo,Shenggang Li,Lingzhao Kong
The catalytic production of lactic acid from carbohydrates was considered a green way to efficiently utilize renewable biomass resources. In this study, an easy post-synthesis method was used to prepare a Sn-Beta catalyst for the production of lactic acid from glucose at 180 °C, 2 MPa, and 30 min. With optimized reaction time, temperature, pressure, and the ratio of raw material to catalyst, the yield of lactic acid reached an astonishingly high level of 76.0%. In addition, the catalyst characterizations were performed in-depth, revealing the intrinsic relationship between catalyst performance and structure, proving that the 2 wt% Sn was uniformly dispersed in the skeleton of Beta zeolite, which significantly increased the density of Lewis acid. Thus, the enhanced isomerization and retro-aldol condensation processes over the Lewis acid sites led to the high yield of lactic acid. This catalytic system kept stable after five cycles at mild conditions, showing high potential for industrial biomass utilization.
研究领域:
生物化学
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催化化学
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DOI
PubMed
高影响因子
DALTON TRANSACTIONS
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2015
·Vol. 44
·期 19
·9182-9192
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IF 4.197
Cholho Choe,Ling Yang,Zhanao Lv,Wanling Mo,Zhuqi Chen,Guangxin Li,Guochuan Yin
Redox-inactive metal ions can modulate the reactivity of redox-active metal ions in a variety of biological and chemical oxidations. Many synthetic models have been developed to help address the elusive roles of these redox-inactive metal ions. Using a non-heme manganese(II) complex as the model, the influence of redox-inactive metal ions as a Lewis acid on its catalytic efficiency in oxygen atom transfer was investigated. In the absence of redox-inactive metal ions, the manganese(II) catalyst is very sluggish, for example, in cyclooctene epoxidation, providing only 9.9% conversion with 4.1% yield of epoxide. However, addition of 2 equiv. of Al3+ to the manganese(II) catalyst sharply improves the epoxidation, providing up to 97.8% conversion with 91.4% yield of epoxide. EPR studies of the manganese(II) catalyst in the presence of an oxidant reveal a 16-line hyperfine structure centered at g = 2.0, clearly indicating the formation of a mixed valent di-μ-oxo-bridged diamond core, MnIII-(μ-O)2-MnIV. The presence of a Lewis acid like Al3+ causes the dissociation of this diamond MnIII-(μ-O)2-MnIV core to form monomeric manganese(IV) species which is responsible for improved epoxidation efficiency. This promotional effect has also been observed in other manganese complexes bearing various non-heme ligands. The findings presented here have provided a promising strategy to explore the catalytic reactivity of some di-μ-oxo-bridged complexes by adding non-redox metal ions to in situ dissociate those dimeric cores and may also provide clues to understand the mechanism of methane monooxygenase which has a similar diiron diamond core as the intermediate.
研究领域:
生物化学
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催化化学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jialing Shen,Guojun Lv,Juan Deng,Shihao Su,Fuxin Wang,Shengnan Xu,Lachgar Oussama,Zhongmin Liu
UiO-66 materials have the benefit of excellent stability, porosity, huge surface area, and presence of flaws, hence designing oxidative desulfurization (ODS) catalysts based on UiO-66 is very appealing. Herein, tungsten doped UiO-66 materials were synthesized with post-doping and in situ synthesis methods, and used as heterogeneous catalysts for the room-temperature oxidative desulfurization reactions. The successful doping of tungsten into the UiO-66 framework was demonstrated by FT-IR, UV–Vis, Raman and TGA characterizations. XAS characterization disclosed that tungsten element formed Zr-O-W bond on the defect sites for the tungsten doped UiO-66 materials. At the same time, the in situ synthesized W 2 @U-150 catalyst revealed the highest 98.5% of dibenzothiophene (DBT) elimination within 1h of desulfurization reaction as well as the biggest catalytic efficiency of 17727.3 h −1 mol −1 at room temperature due to its smallest band gap energy of 3.32 eV, highest tungsten content of 9.8 %, and most Lewis acid amount of 47.1 μmol/g. In addition, the synthesized W 2 @U-150 catalyst showed excellent re-usability for five cycles.
研究领域:
材料科学
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催化化学
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环境化学
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DOI
高影响因子
Scientific Reports
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2025
·Vol. 15
·期 1
·1-6
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IF 3.9
Li Wenfang,Lu Yuze,Wang Jiajun,Li Chuanbi
In this study, a novel artificial enzyme Zn(II)-SMM with simple organic structure for PNPA-directed hydrolysis is proposed. The introduction of hydrophobic quinoline and dipyridinium in Zn(II)-SMM system demonstrates high activity for the complexation of Zn 2+ and hydrolysis of PNPA, and the catalytic rate (k cat /k uncat ) exceeds 5239 times that of non-catalytic systems. The newly designed small molecule organic complex effectively binds to and catalyzes the hydrolysis of substrate PNPA in accordance with Michaelis-Menten kinetics. The mechanism with activation by single Lewis acid provides fundamental insights for the development of small molecule hydrolases.
研究领域:
生物化学
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分子生物学
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DOI
PubMed
高影响因子
FIBERS AND POLYMERS
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2025
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IF 2.3
Li Xinao,Xu Yuanyuan,Wu Jianning,Liu Zhiyong,Meng Guihua,Yang Shengchao,Guo Xuhong
Pretreatment of cellulosic materials with a Lewis acid is used to remove hemicelluloses and lower the reaction temperature of pretreatment systems. Adding Lewis acid in the pretreatment process of lignin extraction can form competitive hydrogen bonds to improve the pretreatment efficiency and the extraction rate of lignin. In this experiment, a Lewis acid (AlCl 3 ) was introduced to promote the separation of lignin by using the choline chloride/formic acid DES system. The dissolution rate of lignin was studied, as well as the effects of the molar ratio of Lewis acid/choline chloride/formic acid, reaction temperature, and reaction time on lignin structure, extraction rate, and solid residue recovery ratio. The experimental results showed that the optimal ratio of formic acid:choline chloride:AlCl 3 was 1:1:0.05. When the reaction temperature was 100 °C and the reaction time was 6 h, the solid residue recovery ratio was 33%, the extraction rate of lignin was 95.6%, and the purity was 95.0%. 2D HSQC NMR, X-ray diffraction (XRD), scanning electron microscopy (SEM), and Fourier transform infrared (FT-IR) spectroscopy were used to confirm the effect of Lewis acid on the extraction efficiency and structure of lignocellulose. The extracted lignin and commercial lignin showed similar structures, and the main structural units were G units and S units. In short, the addition of a Lewis acid improved the separation of lignin.
研究领域:
生物化学
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材料科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
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2013
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IF 4.593
Lei Dong,Yujuan Wang,Yanzong Lv,Zhuqi Chen,Fuming Mei,Hui Xiong,Guochuan Yin
Redox-inactive metal ions have been recognized to be able to participate in redox metal-ion-mediated biological and chemical oxidative events; however, their roles are still elusive. This work presents how the redox-inactive metal ions affect the oxidative reactivity of a well-investigated manganese(II) with its corresponding manganese(IV) complexes having cross-bridged cyclam ligand. In dry acetone, the presence of these metal ions can greatly accelerate stoichiometric oxidations of triphenylphosphine and sulfides by the manganese(IV) complexes through electron transfer or catalytic sulfoxidations by the corresponding manganese(II) complexes with PhIO. Significantly, the rate enhancements are highly Lewis-acid strength dependent on added metal ions. These metal ions like Al3+ can also promote the thermodynamic driving force of the MnIV–OH moiety to facilitate its hydrogen abstraction from ethylbenzene having a BDECH value of 85 kcal/mol, while it is experimentally limited to 80 kcal/mol for MnIV–OH alone. Adding Al3+ may also improve the manganese(II)-catalyzed olefin epoxidation with PhIO. However, compared with those in electron transfer, improvements in hydrogen abstraction and electron transfer are minor. The existence of the interaction between Lewis acid and the manganese(IV) species was evidenced by the blue shift of the characteristic absorbance of the manganese(IV) species from 554 to 537 nm and by converting its EPR signal at g = 2.01 into a hyperfine 6-line signal upon adding Al3+ (I = 5/2). Cyclic voltammograms of the manganese(IV) complexes reveal that adding Lewis acid would substantially shift its potential to the positive direction, thus enhancing its oxidizing capability.
研究领域:
化学
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生物化学
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DOI
PubMed
高影响因子
DESALINATION
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2024
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IF 8.3
Xiaowen Huo,Yingying Zhao,Zhaojing Jing,Jian Wang,Haitao Wang,Na Chang
One of the main approaches to improve the permeability of membranes is the preparation of PA layers with nanostructures based on metal organic framework (MOF) materials. However, the interaction between MOF additives and PIP/TMC monomers and the mechanisms affecting the interfacial polymerization process have not been elucidated. In this study, the adsorption conformation between the two-phase monomers and UiO-66 (UiO-66-TFA) was established by density functional theory (DFT) calculations based on Lewis acid-base theory. The results showed that the hydrogen bonding force between UiO-66 (UiO-66-TFA) with defect structures and PIP (−199.62 kcal/mol) was significantly stronger than that between UiO-66-TFA and TMC (−26.39 kcal/mol). Moreover, two PA layers with ridged and granular morphologies were prepared by dispersing UiO-66/UiO-66-TFA in the water/organic phase to influence interfacial polymerization, using UiO-66-TFA nanoparticles as additives. Among them, the PA layers showed more pronounced morphological transformation and excellent separation properties when UiO-66-TFA was used as an additive in the aqueous phase . The representative ridge-like nanostructured nanofiltration membrane showed a pure water flux of 27.51 L·m −2 ·h −1 and 98.8 % retention of Na 2 SO 4 . This study provides a new idea for the preparation of PA layers with different surface nanostructures based on the IP reaction of nano-additives.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Caihong Lv,Xin Zhou,Cheng Chen,Xinghai Liu,Jun Qian
Ammonia serves as a crucial indicator of food spoilage, but current sensors lack sufficient sensitivity, stability, selectivity, and automation for practical on-site and real-time monitoring. A highly sensitive and flexible ammonia sensor based on PEDOT:PSS doped with Lewis acid (FeCl 3 solution) for wireless food monitoring is proposed in this study to solve the above limitations. The intercalation effect caused by the diffusion of Fe 3+ and hydrolyzed H + in the film coordinating with SO 3 − groups present in PSS chains leads to an increased distance between adjacent PEDOT-rich domains. It enhances ammonia sensitivity by providing additional ionic carriers and carrier transport paths within the PEDOT:PSS molecule. The results demonstrated a significant enhancement in the sensitivity of PEDOT:PSS sensor doped with FeCl 3 , exhibiting a response value of about 25 % at 25 ℃ for 1 ppm NH 3 , with an impressive detection limit of 0.23 ppm and quantification limit of 0.78 ppm (1–400 ppm). Moreover, it showcases acceptable repeatability both at 1 ppm (RSD = 4.30 %) and 100 ppm ammonia (RSD = 3.61 %), along with the notable selectivity and long-term stability. XPS, Raman analysis, and the density function theory (DFT) calculations further elucidated the sensing mechanism of the sensor towards ammonia. Additionally, a portable wireless detection device was designed, which was equipped with the Bluetooth communication and the micro-controller system to detect the decay process of fresh shrimp, realizing wirelessly real-time monitoring of food freshness through a smart phone. It’s worth noting that the innovative sensing technology holds great promise for food quality monitoring.
研究领域:
食品科学
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材料科学
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传感技术
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
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IF 5.9
Md Asraful Alam,Liya Deng,Ange Douglas Potchamyou Ngatcha,Aymard Didier Tamafo Fouegue,Jingcheng Wu,Shen Zhang,Anqi Zhao,Wenlong Xiong,Jingliang Xu
Traditional two steps biodiesel production process generally involves corrosive sulfuric acid in the transesterification step, which is not environmentally benign. In this work, a novel procedure was presented for the direct production of biodiesel using Lewis acid deep eutectic solvent (LADES) to avoid using sulfuric acid. Synergy between the Lewis site of the LADES catalyst and the Brønsted site from biomass pretreated by Brønsted acidic deep eutectic (BADES) has resulted in the development of a bifunctional medium considered to be appropriate for high biodiesel formation and increase the FAMEs weight. The mechanism of biodiesel formation was anticipated through the experimental and computational studies of Lewis and/or Brönsted acid sites in the reaction process. The potential interference factors of the extraction process such as time of reaction, temperature, LADES catalyst concentration in methanol, and solvent volume were further optimized experimentally, followed by the Box–Behnken method. The highest amount (39.86 mg/g) of fatty acid methyl esters (FAMEs) was obtained from Chlorella pyrenoidosa biomass at 120 °C for 90 min, 5 mL solvent volume, and 5% concentration of LADES (ChCl-CrCl 3 .6 H 2 O) catalyst in methanol. The predominant FAMEs were C16:0 (9.47 mg/g), C18:2 (12.42 mg/g), and C18:3 (8.68 mg/g), and obtained biodiesel qualities meet international standards. The recyclability of LADES was tested, and satisfactory results of FAME weight were observed up to three cycles, and the FTIR peaks of LADES catalyst after four cycles of reusing have shown the structure of DES remain stable. Despite the existence of sustainable, efficient, and less toxic ways for microalgae transesterification, further investigation is required to assess the scalability of these methods for large-scale use.
研究领域:
生物技术
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能源科学
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环境科学
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DOI
高影响因子