GREEN CHEMISTRY
·
2024
·
IF 9.3
Qi Zhu,Bo Gong,Shuquan Huang,Yangxin Jin,Shengqin Liu,Shan Shao,Yuwei Yang,Taren Cataldo,Nicholas M. Bedford,Jason Chun-Ho Lam
The electrochemical selective oxidative transformation of lignin feedstocks into valuable oxygenated aromatics is essential to establish a sustainable biorefinery. In this study, we used a rhombohedral ZnIn2S4 (R-ZIS) electrocatalyst to realise the efficient anodic cleavage of C–O bonds in benzyl phenyl ether (BPE), an α-O-4 lignin model compound, to a series of industrially relevant oxygenated mono-aromatics. The reaction occurred at +2 VAg/AgCl, 65 °C, and atmospheric pressure. In optimised conditions, the reaction achieved over 99% conversion rate with a Faraday efficiency of 51.6% at 91.3% conversion of BPE, that is greater than most known electrocatalytic oxidative cleavage examples. The ZnIn2S4 electrocatalyst was deposited on a carbon cloth support, and its structural properties and surface morphology were extensively investigated. Systematic potential controlled electrolysis coupled with 18O isotopic labelling confirmed that C–O scission occurred exclusively between the benzylic carbon and phenolic oxygen. Furthermore, substrate competition studies were conducted to compare the electrocatalytic performance of the R-ZIS catalyst with that of its structural analogue, hexagonal ZnIn2S4, in terms of BPE and mono-aromatics conversion. The experimental results were supported by density functional theory calculations. The substrate scoping study revealed the suitability of the R-ZIS induced electrocatalytic system for a variety of substituted α-O-4/β-O-4 model dimers. Overall, this work demonstrates an efficient anodic process that can enable the atom-efficient valorisation of lignin to produce oxygenated aromatics. The proposed approach can complement the numerous existing reductive lignin cleavage methods.
研究领域:
化学工程
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可再生资源利用
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电化学催化
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Entong Ye,Zheng Chen,Yongyong Shi,Dan Zhang,Wenfei Li,Hong Qin,Ziming Luo,Quansheng Wu,Qian Lin,Hongyan Pan,Keliang Wang
Although a high-activity yield of hydrogen peroxide (H 2 O 2 ) can be achieved by direct synthesis from hydrogen and oxygen, developing an extreme catalyst with high activity and stability is still very challenging, which limits its industrial application. Here, we reported a catalyst Pd/SPE with polyelectrolyte membranes SPE as an electronic acceptor to anchor Pd, which achieves H 2 O 2 selectivity of 90.1% and productivity of 5764.4 mmol∙g Pd -1 ∙h −1 . The results of TEM, XRD and ICP-MS, XPS, CO-DRIFT, O 2 -TPD, synchrotron radiation and density functional theory (DFT) simulations reveal that the electrons of Pd are transferred into polyelectrolyte membranes and Pd clusters are strongly chemisorbed on SPE, which is beneficial for O 2 adsorption and inhibits the dissociation of O-O bond, leading to significantly enhanced H 2 O 2 productivity and selectivity.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 20
·11508-11518
·
IF 3.43
Jing Chen,Hanling Yang,Hongquan Fu,Hongyan He,Qiang Zeng,Xuehui Li
Electrochemical oxidation is a promising and effective method for lignin depolymerization owing to its selective oxidation capacity and environmental friendliness. Herein, the electrooxidation of non-phenolic alkyl aryl ether monomers and β-O-4 dimers was experimentally (by cyclic voltammetry, in situ spectroelectrochemistry, and gas chromatography-mass spectroscopy) and theoretically (by DFT calculations) explored in detail. Compared to the reported literature (T. Shiraishi, T. Takano, H. Kamitakahara and F. Nakatsubo, Holzforschung, 2012, 66(3), 303–309), 1-(4-ethoxyphenyl)ethanol showed a distinguishable oxidation pathway, where the resulting carbonyl product surprisingly underwent a bond cleavage on alkyl–aryl ether to ultimately produce a quinoid like compound. In contrast, β-O-4 dimers, like 2-phenoxy-1-phenethanol and 2-phenoxyacetophenone also demonstrated electrochemical oxidation induced by Cβ–O and Cα–Cβ bond cleavages. For the oxidation products, the presence of the Cα-hydroxyl group in dimers was the key to selectively generate aldehyde-containing species under mild electrochemical conditions, otherwise it produces alcohol-containing products following a different mechanism compared to the CαO containing dimers.
研究领域:
林产化学
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环境科学
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有机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Ziwen Yao,Jing Li,Shuai Nie,Yuan Wang,Xitao Yin,Yunxia He
Utilizing p-n composite materials for the fabrication of metal-oxide semiconductor (MOS) gas sensors represents a promising strategy to achieve exceptional selectivity in detecting reducing gases such as hydrogen (H₂) and carbon monoxide (CO). However, previous studies have typically achieved this selectivity under fixed operating temperatures and single molar ratios. This study presents the successful synthesis of n-In₂O₃/p-Co₃O₄ nanoparticles, featuring a p-n heterojunction structure, using a simple composite preparation method. The gas-sensing properties, crystal structure, morphology, and chemical states were comprehensively characterized using an electrochemical workstation, XRD, TEM, HRTEM, and XPS. Experimental results show that the gas sensor responses of the n-In₂O₃/p-xCo₃O₄ composites (with x = 10.5, 15, 18, 21), annealed at 500°C within an operational temperature range of 350°C to 400°C, exhibit distinct behaviors for CO and H₂ gases. This addresses the challenge of achieving selective detection across varying conditions. Notably, the n-In₂O₃/p-18Co₃O₄ composites display opposing response characteristics for both gases across a broad temperature range of 200°C to 400°C. At 350°C, the n-In₂O₃/p-18Co₃O₄ sensor demonstrates optimal selectivity, significantly minimizing cross-sensitivity and improving detection accuracy and reliability. The sensor also shows excellent stability, with consistent responses under repetitive exposure conditions. By improving both sensor selectivity and stability, this research advances gas detection technologies, with potential applications in sustainable energy and public health monitoring.
研究领域:
材料科学
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传感器技术
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Fekadu Tadesse Bekena,Dong-Hau Kuo,Worku Lakew Kebede
Wastewater treatment becomes an important part to improve environmental quality and protect water resources. Thus, developing a new photocatalyst is a key solution for environmental issues. Herein, universal, highly efficient, and novel Bi 2 (O,S) 3 /Mo(O,S) 2 nanocomposite photocatalyst was fabricated by a facile method and the crystal structure, morphology, composition, and optical properties of the as-prepared catalysts were characterized in details. The photocatalytic performance of the catalysts was evaluated by the photodegradation of methyl orange (MO), rhodamine B (RhB), methylene blue (MB), and neutral red (NR), the results showed that 20% Bi-MoOS nanocomposite had excellent photodegradation activity towards all dyes. 96.0% of MO, 96.6% of RhB, 98.8% of MB and 91.3% of NR dyes were removed after 180 min, 40 min, 20 min, and 25 min visible light irradiation, respectively. The photodegradation of these dyes was further confirmed with HPLC. The excellent photocatalytic activity of the nanocomposites was due to the efficient separation and transport of photogenerated charge carriers induced by the fabricated binary heterostructures. The photodegradation fitted well the pseudo-first-order kinetics. The active species capture experiment study showed that, OH, O 2 − and h + all took parts in the degradation of dyes. The stability of the catalyst and reaction mechanism also explained in this work.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Zhuang Li,Zi-Chun Fan,Xiang Bai,Xian-Yong Wei,Yierxiati. Dilixiati,Qian-Qian Kong,Ji Zhao,Yong-Hui Feng,Jun-Long Wang,Xing Fan,Xiao-Yan He,Hai-Xu Zou,Zhi-Min Zong
MY zeolites with mesopores were prepared by hydrothermal method using functionalized SiO 2 (F-SiO 2 ) as a silica source, and hydrophobic bifunctional Ru/MY- O catalysts were obtained by deposition precipitation method and silylation treatment. This work aims at obtaining polycyclic alkane (PCA) based high-density hydrocarbon fuels (HDHFs). We focused on the catalytic hydroconversion (CHC) of 2-phenoxy-1-phenylethanol (PP-ol) and oxydibenzene (ODB), two typical lignin-related model compounds (LRMCs), over Ru/MY- O . The effects of different reaction conditions and catalysts on the product distribution in PP-ol and ODB were investigated. The partial hydrogenation of ODB was found to be a necessary step before achieving C-O ether bond cleavage and C-C bond coupling. The balance of metal/acidic sites is critical for maximizing PCA yields. Changes in the metal/acid ratio had a greater effect on PCA yield in PP-ol than in ODB. Poor stability of cycloalkyl cations and partial hydrogenation of ODB hinder the generation of C-C coupling products. The incorporation of mesopores and hydrophobic treatment were found to weaken the negative effects of C-C bond coupling products and water on the catalyst. The conversion of Ru 3 /MY- O was improved by nearly 10% compared to Ru 3 /Y in the fifth cycle reaction. This work provided a theoretical basis for the generation of HDHFs from lignin.
研究领域:
化学工程
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催化
·
可再生能源
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-17
·
IF 15.7
Liu Qiannan,Lu Xiaoyan,Deng Yao,Zhang Han,Wei Rumeng,Li Hongrui,Feng Ying,Wei Juan,Ma Fang,Zhang Yan,Zou Xia
Protein O-glycosylation plays critical roles in sperm formation and maturation. However, detailed knowledge on the mechanisms involved is limited due to lacking characterization of O-glycoproteome of testicular germ cells. Here, we performed a systematic analysis of site-specific O-glycosylation in mouse testis, and established an O-glycoproteome map with 349 O-glycoproteins and 799 unambiguous O-glycosites. Moreover, we comprehensively investigated the distribution properties of O-glycosylation in testis and identified a region near the N-terminal of peptidase S1 domain that is susceptible to O-glycosylation. Interestingly, we found dynamic changes with an increase Tn and a decrease T structure from early to mature developmental stages. Notably, the importance of O-glycosylation was supported by its effects on the stability, cleavage, and interaction of acrosomal proteins. Collectively, these data illustrate the global properties of O-glycosylation in testis, providing insights and resources for future functional studies targeting O-glycosylation dysregulation in male infertility.
研究领域:
生殖生物学
·
蛋白质组学
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Su Wang,Qifang Sun,Chen Li,Dongge Wang,Yue Ma,Hongzhou Zhang,Xixi Shi,Lianqi Zhang,Dawei Song
Given the high combustion or explosion potential of liquid electrolyte, polymer electrolytes have attracted intensive attention due to high safety, compatible interface and flexible processability. However, the related low ionic mobility remains an issue for related wide application. Herein, a crosslinked polymer electrolyte (abbreviated as PMEP) comprising abundant oxygen-contained groups (C-O-C/C=O) is developed. With the crosslinking agent of ethoxylated trimethylolpropane triacrylate (ETPTA), a high transference number ( t Li + =0.69) is obtained since C-O/C=O are conducive to the transfer of Li ions. Specifically, C=O group exists in individual monomers in order to be applicable to high voltage cathode, therefore, a criss-cross network containing abundant sites conducive to ion transport is constructed and rapid ion transfer as well as enhanced mechanical strength can be realized even in high potential system. With the coordination effect of C-O and C=O, PMEP exhibits rapid Li ion transfer and a wide electrochemical stability window of 5.1 V. As for Li//Li symmetrical cell, a stable voltage profile with slight polarization of 60 mV is displayed for over 550 h at 1 mA cm −2 . After assembled with LiNi 0.8 Co 0.15 Al 0.05 O 2 cathode, a high discharge specific capacity of 190.6 mAh g −1 is delivered and the capacity retention reaches 86 % at 0.1C for 100 cycles. This work provides a promising method for designing high-performance polymer electrolytes for lithium metal batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
BMC Chemistry
·
2019
·Vol. 13
·期 1
·1-15
·
IF 0
Guo J.,Ma Yu L.,Yu Jia Y.,Gao Yu J.,Ma Ning X.,Wu Xiao Y.
Herein, 2-(2-methoxyphenoxy)-1-phenylethanol (β- O -4), 2-methoxyphenyl anisole (α- O -4) and 4-phenoxyphenol (4- O -5) were selected as typical lignin model compounds. Given the effectiveness of traditional acid–base catalysts for lignin depolymerisation, a novel Ni/CaO–H-ZSM-5(60) catalyst was prepared to investigate the difficulty level of C–O bond of three model compounds cleavage in ethanol. It was observed that Ni/CaO–H-ZSM-5(60) had prominent performance on the C–O bond cleavage at very mild conditions (140 °C, 1 MPa H 2 ). Among them, the C–O bond of α- O -4 and β- O -4 could be completely cleaved within 60 min. Although the C–O bond of 4- O -5 had high bond energy, 41.2% of conversion was occurred in 60 min. The introduction of CaO could regulate the acidity of H-ZSM-5 to enhance the ability to break C–O bonds. Moreover, the possible pathways of C–O ether bonds in three lignin model compounds cleavage were proposed in order to selectively obtain target products from the raw lignin degradation.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
Nanomaterials
·
2020
·Vol. 10
·期 3
·438
·
IF 4.324
Jianian Hu,Jian Zhang,Guoqiang Luo,Yi Sun,Qiang Shen,Lianmeng Zhang
This research presents an approach for C-O grain boundary strengthening of Al composites that used an in situ method to synthesize a C-O shell on Al powder particles in a vertical tube furnace. The C-O reinforced Al matrix composites (C-O/Al composites) were fabricated by a new powder metallurgy (PM) method associated with the hot pressing technique. The data indicates that Al4C3was distributed within the Al matrix and an O-Al solution was distributed in the grain boundaries in the strengthened structure. The formation mechanism of this structure was explained by a combination of TEM observations and molecular dynamic simulation results. The yield strength and ultimate tensile strength of the C-O/Al composites, modified by 3 wt.% polyvinyl butyral, reached 232.2 MPa and 304.82 MPa, respectively; compared to the yield strength and ultimate tensile strength of the pure aluminum processed under the same conditions, there was an increase of 124% and 99.3%, respectively. These results indicate the excellent properties of the C-O/Al-strengthened structure. In addition, the strengthening mechanism was explained by the Hall–Petch strengthening, dislocation strengthening, and solid solution strengthening mechanisms, which represented contributions of nearly 44.9%, 15.9%, and 16.6% to the total increased strength, respectively. The remaining increment was attributed to the coupled strengthening of the C and O, which contributed 20.6% to the total increase.
研究领域:
材料科学
·
力学
·
纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2015
·
IF 4.169
Kexin Hou,Fengli Chen,Yuangang Zu,Lei Yang
An efficient method for the extraction of vitexin , vitexin-4″- O -glucoside, and vitexin-2″- O -rhamnoside from Phyllostachys edulis leaves comprises heat treatment using an ionic liquid–lithium salt mixture (using 1-butyl-3-methylimidazolium bromide as the solvent and lithium chloride as the additive), followed by ultrasound-assisted extraction. To obtain higher extraction yields, the effects of the relevant experimental parameters (including heat treatment temperature and time, relative amounts of 1-butyl-3-methylimidazolium bromide and lithium chloride, power and time of the ultrasound irradiation, and the liquid–solid ratio) are evaluated and response surface methodology is used to optimize the significant factors. The morphologies of the treated and untreated P. edulis leaves are studied by scanning electron microscopy. The improved extraction method proposed provides high extraction yield, good repeatability and precision, and has wide potential applications in the analysis of plant samples.
研究领域:
植物化学
·
分析化学
✓ 已验证
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Zehong Zhu,Qingxin Wu,Xueying Wang,Haiyang Zhang,Jian Li,Yanzhao Dong,Yongsheng Xu,Yunsheng Dai,Jinli Zhang
Here, the spiral mesoporous hydrothermal carbonaceous nanospheres (SMHNs) were designed and fabricated from pentose precursors to enhance gas diffusion in acetylene hydrochlorination. Through the optimization of hydrothermal conditions, the optimized SMCNs-800 material showcased the highest catalytic activity with an acetylene conversion of 77 % under the condition of GHSV (C 2 H 2 ) = 30 h −1 . The structural analysis indicated that the material with helical structure could provide larger pore sizes and abundant defect sites, exposing more active sites. The structure-activity relationship among acid-base properties of the catalyst surface, the adsorption-desorption capacity for the reactants and the catalytic activity jointly demonstrated that pyridine-N and -C=O could provide abundant basic sites for the adsorption and activation of H-Cl, thus accelerating the process of acetylene hydrochlorination reaction.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）