FUEL
·
2020
·
IF 5.578
Tianjin Li,Hongfei Lin,Xinping Ouyang,Xueqing Qiu,Zechen Wan,Tao Ruan
The selective cleavage of C–O bond in lignin is the key to convert them into aromatic compounds and then to produce liquid fuels and chemicals. N-doped carbon nanosheets were obtained by direct pyrolysis of glucosamine hydrochloride (GAH) and melamine. Highly-dispersed and small-sized Ru nanoparticles (NPs) supported N-doped carbon by impregnation method, which can efficiently convert lignin to obtain 40.70% aromatic monomers. It was 2.3 times than that of the commercial catalyst (Ru/C) and the catalyst could be used at least five runs with an insignificant loss in the yield of aromatic monomers. The morphology, specific surface area, nitrogen species and content of supports could be tuned by controlling the weight of melamine. The results showed that the melamine and GAH were condensed to form layered graphitic carbon nitride (g-C 3 N 4 ) and a carbon skeleton at 600 °C, respectively. Then, the produced N from the decomposition of g-C 3 N 4 at high temperature (>700 °C) could improve nitrogen concentration, increase the specific area and result in the graphene-like wrinkled morphology. The presence of pyridinic N not only served as metal coordination sites to stabilize and disperse Ru NPs but also enhanced the proportions of Ru 0 through the electronic interactions. The DFT calculations implied that the pyridinic N contributed to the highest adsorption energy for 2-phenoxy-1-phenethanol (PPE) and a reduction of the disassociation energy for C alkyl –O bond compared with graphite N and pure C.
研究领域:
化学工程
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 10
·e202300067
·
IF 8.4
Wenhao Liu,Xuanpeng Wang,Jinshuai Liu,Changyuan Guo,Fan Qiao,Xiaoling Ding,Xiaobin Liao,Chunhua Han
To better satisfy the increasing demands for electric vehicles, it is crucial to develop fast-charging lithium-ion batteries (LIBs). However, the fast-charging capability of commercial graphite anodes is limited by the sluggish Li + insertion kinetics. Herein, we report a synergistic engineering of uniform nano-sized T-Nb 2 O 5 particles on graphite (Gr@Nb 2 O 5 ) with C−O−Nb heterointerfaces, which prevents the growth and aggregation of T-Nb 2 O 5 nanoparticles. Through detailed theoretical calculations and pair distribution function analysis, the stable existence of the heterointerfaces is proved, which can accelerate the electron/ion transport. These heterointerfaces endow Gr@Nb 2 O 5 anodes with high ionic conductivity and excellent structural stability. Consequently, Gr@10-Nb 2 O 5 anode, where the mass ratio of T-Nb 2 O 5 /graphite=10/100, exhibits excellent cyclic stability and incredible rate capabilities, with 100.5 mAh g −1 after 10000 stable cycles at an ultrahigh rate of 20 C. In addition, the synergistic Li + storage mechanism is revealed by systematic electrochemical characterizations and in situ X-ray diffraction. This work offers new insights to the reasonable design of fast-charging graphite-based anodes for the next generation of LIBs. Graphical Bond together : Benefiting from the C−O−Nb heterointerfaces that can effectively enhance the structure stability and facilitate electron/ion transport, composite of T-Nb 2 O 5 particles decorated on graphite exhibits low interfacial resistance, high Li + diffusion coefficient (nearly 34 times higher than graphite), and a high discharge capacity of 100.5 mAh g −1 after 10000 cycles at 20 C.
研究领域:
材料科学
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电化学
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能源存储
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纳米材料
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锂离子电池
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Feng Chen,Xuebin Lin,Wei Chen,Na Wen,Yanqiao Jin
The design of a highly active Cu-Co catalyst for catalytic transfer hydrogenolysis of lignin without the use of external hydrogen remains highly challenging. In this work, Cu 2 O was initially encapsulated in ZIF-67, and subsequently Cu 2 O@ZIF-67 was utilized as a precursor and sacrificial template to prepare the unique double core–shell hollow nanocage CuO@Co 3 O 4 . Co and Cu, serving as Lewis acid sites and dehydrogenation sites for the hydrogen-donor solvent isopropanol, respectively, exhibited synergistic enhancement, further increasing the catalytic activity. Under the optimal conditions of 220 °C, 1 MPa N 2 , and 4 h, the catalyst achieved 100 % conversion of 2-phenoxy-1-phenylethanol and 100 % yield towards cyclohexanol and ethylbenzene. Furthermore, the catalyst remained stable and reusable after 5 cycles, providing a practicable guidance for the value-added conversion of lignin.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
HIGH PERFORMANCE POLYMERS
·
2015
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IF 1.286
Yewei Xu,Yi Sun,Yonglin Lei,Jichuan Huo,Lin Zhang
This article presents a convenient polymerization route to synthesize poly(arylene ether)s containing N-arylenebenzimidazolyl groups. The novel polymers were prepared by a catalyst-free nucleophilic substitution reaction, in which the N–H and O–H sites were removed from 2-(2-hydroxyphenyl)-1H-benzimidazole with different activated difluorides containing carbonyl groups in sulfolane. The reaction was carried out in the presence of anhydrous potassium carbonate at 210°C. The structures of the polymers were characterized using Fourier transform infrared spectroscopy, proton nuclear magnetic resonance spectroscopy, and elemental analysis. The results show good agreement with the proposed structure. All resulting polymers show essentially amorphous patterns. Moreover, differential scanning calorimetry and thermogravimetric measurements show that the polymers have high glass transition temperatures (>209°C), good thermostability, and high decomposition temperatures (>425°C). Furthermore, the polymers also exhibit excellent solubility in common organic solvents.
研究领域:
材料科学
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高分子化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Tingting Xiao,Jingrong Li,Jian Li,Qihang Gong,Peikai Luo,Xinluona Su,Haiyang Cheng,Chao Zhang,Fengyu Zhao
The hydrogenolysis of cellulose-derived 5-hydroxymethylfurfural is essential for the production of fuels and chemicals from biomass. Herein, we fabricated a phosphorus-doped Pd/P-TiO2 catalyst for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran. A large number of defects and electron-deficient Ti4+ sites (dTi4+) were formed by doping phosphorus into the TiO2 support, which could promote hydrogen spillover and reactant adsorption. Moreover, the spilled active hydrogen induced the formation of P–O(H)-dTi4+, which acted as a “Brønsted acidic site” to promote the activation of C–O bonds. Consequently, the Pd/P-TiO2 catalyst exhibited superb activity for the hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran at mild conditions of 150 °C under 1 MPa H2.
研究领域:
催化化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
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
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
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催化科学
✓ 已验证
DOI
ChemSusChem
·
2025
·
IF 6.6
Zixuan Tan,Yihong Cai,Bo Yang,Hao Huang,Haijun Guo,Min Zhuang,Hui Luo,Qingwei Meng,Shaoqu Xie
Graphical Monohydric alcohols are a potential fuel, and herein, monohydric alcohols have been selectively synthesized from multicarbon sugars by modulating the electron distribution of Ru and enhancing the hydrodeoxygenation process of biomass. Ru-based catalysts are widely used in catalytic reactions, but the electron-deficient nature promotes strong decarbonylation, leading to complete deoxygenation during the conversion of polyhydroxy biomass. Despite extensive research, effectively suppressing this decarbonylation activity remains challenging. Herein, electron-rich Ru and electron-deficient Ni formed due to the electron migration of Ni → Ru have a synergistic catalytic effect, controlling the precise cleavage of C N bonds by Ru 0 and retaining most of the C O bonds. The amorphous Al 2 O 3 is sufficiently bound to the substrate to promote rapid hydrogenation. This modification effectively suppresses the intrinsic decarbonylation activity of Ru and improves selectivity for hydrodeoxygenation. Using carbohydrates as substrates, the Ru–Ni bimetallic catalysts preferentially promote the hydrodeoxygenation pathway, resulting in a significant increase in C3+ monohydric alcohol yields. This work presents a new strategy for modulating reaction pathways via electronic structure engineering, offering valuable insights into the potential of Ru–Ni systems for biomass conversion and sustainable alcohol synthesis.
研究领域:
催化化学
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材料科学
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化学工程
·
生物质转化
·
可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 6
·1748-1754
·
IF 5
Shaoyuan Guo,Xinli Tong,Lingwu Meng,Guobao Yang
Selective oxidative C–C and C–O bond cleavage is of significance to the efficient utilization of biomass and biomass-derived platform compounds. In this work, the selective oxidative cleavage of C–C and C–O bonds has been developed with an iron-based catalyst (Fe–N–C) in the presence of molecular oxygen. Specifically, the β-O-4 lignin model compound was successfully converted to phenol and methyl benzoate in a methanol solvent, where the substrate conversion was 95.0% and the yields of phenol and methyl benzoate were 94.9% and 63.7%, respectively, when the reaction was performed with the Fe–N–C-850 catalyst at 120 °C for 4 h. Also, the oxidative transformations of other lignin models to phenols and methyl benzoates were achieved. Further investigations showed that the existence of the Fe3C phase in the catalyst plays an important role in the aerobic oxidative cleavage of C–C and C–O bonds in the β-O-4 lignin model.
研究领域:
生物质化学
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催化化学
✓ 已验证
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
TETRAHEDRON
·
2014
·
IF 2.817
Dazhuang Miao,Xuesong Shi,Guozhen He,Yao Tong,Zengqiang Jiang,Shiqing Han
N -(2-Chloro-phenyl)-2-halo-benzamides (halo=I/Br/Cl) as substrates were used for the one-pot synthesis of 2-arylbenzoxazole derivatives via copper-catalyzed intermolecular C–N/intramolecular C–O couplings with primary amines . This aryl amination offers clean reaction conditions and easy work-up in good yields by using CuI as catalyst, readily available 8-hydroxyquinoline as ligand, K 3 PO 4 as base, DMF as solvent.
研究领域:
有机化学
·
合成化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jingjing Tang,Hongchao Li,Xuan Zhang,Jieshu Qian,Bingcai Pan
Fe-based metal–organic frameworks (MOFs) have garnered significant attention as catalysts for heterogeneous Fenton reactions, while the limited efficiency of the Fe(III)/Fe(II) redox cycle hinders their widespread use in wastewater treatment. Herein, we successfully incorporated carbon nanotubes (CNTs) into MIL-101(Fe) to modulate the coordination environment of Fe for achieving better catalytic activity. The MIL-101(Fe)/CNTs/H 2 O 2 system shows outstanding performance in degrading various pollutants, with the catalytic activity of the MIL-101(Fe)/CNTs composites (98.8%) significantly surpassing that of MIL-101(Fe) alone (26.4%) or CNTs alone (3.5%). Multiple experimental findings suggest that this synergistic effect is primarily attributed to the C-O-Fe bridge bonds resulting from the interaction of surface carboxyl groups on CNTs with Fe in MIL-101(Fe). This unique coordination structure accelerates the redox cycle of Fe(III)/Fe(II), thereby promoting the generation of hydroxyl radicals (HO • ). Furthermore, the MIL-101(Fe)/CNTs composites demonstrate excellent reusability and stability, maintaining effectiveness over a wide pH range from 3.0 to 6.5. This study provides new insights into regulating the microstructure of Fe-based MOFs to enhance their Fenton catalytic activity.
研究领域:
环境科学
·
材料科学
✓ 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）