Journal of Energy Storage
·
2026
·
IF 10.7
Binbin Liu,Xiaorui Yang,Jian Ren,Meng Yang,Xiaodong Shen,Yong Kong
Silicon oxycarbide (SiOC)-based materials hold significant potential as anodes of lithium-ion batteries (LIBs) due to their high theoretical capacity, low volume expansion, and excellent electrochemical stability. However, they exhibit low initial Coulombic efficiency (ICE) and poor cycling stability. In this study, carbon/silicon oxycarbide (C/SiOC) composites were synthesized using a facile sol-gel method followed by ambient pressure drying and thermal treatment. The phase composition of SiOC was tuned by the oxygen content of precursors to achieve a high content of reversible phase for Li storage. Among four organosilanes including trimethylethoxysilane (TMES), 1,3,5,7-tetramethylcyclotetrasiloxane (TMCTS), methyltriethoxysilane (MTES), and tetraethoxysilane (TEOS), TMCTS leads to the highest content of SiO 3 C and SiO 2 C 2 phases owing to moderate oxygen content, which are responsible for Li storage. Hence, the C/SiOC composite with TMCTS as precursor exhibits significantly higher initial Coulombic efficiency (70.53%) than those with TMES, MTES, and TEOS as precursors (68.86%, 43.85%, and 33.11%), which this value exceeds the typical ICE range of 50–60% reported for other SiOC-based materials. It was demonstrated that a higher oxygen content of the precursor promotes the generation of Li 2 O during the lithiation process, which acts as a robust structural buffer to enhanced structural stability. TMCTS-derived C/SiOC composite exhibited excellent cyclic stability over long-term cycling, retaining 601.87 mAh·g −1 after 100 cycles at 0.1 A·g −1 . The results verify the critical role of phase composition of SiOC as anodes of LIBs, providing a new strategy to design SiOC-based materials with high electrochemical performance by tuning phase composition of SiOC from its precursor.
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ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Kexuan Jing,Weizong Wang,Shijie Wang,He Ma,Ran Song,Kang Liang,Shujun Cai,Yurong Ren,Jianbin Li,Zhengping Ding
With high lithium storage performance and low intercalation/deintercalation potentials, silicon-based anode is one of the most promising anode materials for the development of high-energy density lithium-ion batteries (LIBs). Despite the considerable advances made by Si/C negative electrodes in the commercial field, there remains scope for enhancement in terms of their low-temperature performance. In this work, we put forward a novel additive, which is tetrakis(trimethylsilyl)silane (TTS). Theoretical calculations and differential capacity curves demonstrated that the additive is able to preferentially carbonate solvents for decomposition and that the chemical bonds formed by the breakage facilitated the formation of surface films. The incorporation of O-Si-C-rich structures into solid electrolyte interface (SEI) film allows for the attainment of better mechanical properties and high ionic conductivity. The particular SEI is capable of tolerating significant alterations in the volume of Si/C anode particles, thereby preventing the irreversible depletion of lithium ions and electrolytes. Thus, the Si/C half-cell with TTS additive exhibits higher reversible capacity (582.1 mAh g -1 at room temperature, 212.3 mAh g -1 at -20°C), high-rate performance (440.3 mAh g -1 at 2 C), and excellent capacity retention (76.2% after 150 cycles at room temperature, 77.9% after 200 cycles at -20°C). Furthermore, our research explores the impact of TTS on the formation of amorphous silicon. On the one hand, the formed SEI containing O-Si-C structure has better mechanical properties and ionic conductivity, which inhibit the fragmentation of Si/C particles and reduce the irreversible consumption of Li + . On the other hand, an increase in Li + concentration can increase the amorphous silicon content in the lithiation process. Specifically, the introduction of TTS promotes the formation of the amorphous silicon (a-Si) phase, and the content of the a-Si phase is closely related to the reversible capacity and cycling stability of the silicon anode. The unique phase-regulation mechanism is the key to the ability of TTS modification to enhance the low-temperature electrochemical performance of Si/C anode. This work provides an effective method for the development of materials suitable for operation at low-temperature.
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JOURNAL OF CATALYSIS
·
2017
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IF 6.844
Min Wang,Jianmin Lu,Lihua Li,Hongji Li,Huifang Liu,Feng Wang
Selective oxidative cleavage of C C bond is pivotal for producing functionalized molecules, useful for organic synthesis and biomass utilization. We herein report the oxidative C(OH) C bond cleavage of secondary alcohols to acids over a copper/1, 10-phenanthroline complex with molecular oxygen as the oxidant. A wide range of secondary alcohols are converted into acids with up to 98% yields. More interestingly, it is effective for breaking up lignin model systems into acids, which is rarely achieved in previous studies. Density functional theory (DFT) calculations indicate a copper-oxo-bridged oxygen dimer is the active species for the C H bond cleavage which is the rate-determining step for C C bond.
研究领域:
有机化学
·
催化化学
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GREEN CHEMISTRY
·
2026
·
IF 10.6
Yuguo Dong,Puyan Bai,Hongyu Yang,Lin Dong,Xiaoli Gu,Changle Zhao,Zupeng Chen
Photocatalytic depolymerization of lignin into aromatic compounds is of great significance but extremely challenging, hindered by the stable interunit C-C bonds with high dissociation energies. Herein, we develop a novel oxidation acetalization strategy for the phtocatalytic cleavage of C-C bond in lignin model compounds while simultaneously reducing aldehyde condensation. Phosphorus-doped carbon nitride (Px-CN) was synthesized for the selective cleavage of Cα-Cβ bonds under visible light at room temperature. This approach achieves a nearly complete conversion (>99.9%) of 2-phenoxy-1phenylethanol, along with high yields of benzaldehyde dimethyl acetal (91.1%) and benzyl formate (56.3%). Mechanistic investigations reveal that the activation of the Cβ-H bond by photogenerated holes is crucial for the transformation to occur.Meanwhile, the introduction of phosphorus accelerates the separation efficiency of charge carriers, thereby enhancing the photocatalytic performance of the Px-CN. This work demonstrates the potential of phosphorus-doped carbon nitride for the high-selectivity photocatalytic cleavage of the C-C bond in lignin to aromatic chemicals.
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JOURNAL OF PHYSICS D-APPLIED PHYSICS
·
2022
·Vol. 55
·期 44
·444008
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IF 3.409
Jian Cao,Xiaoli Jin,Zhaoyu Ma,Huiqing Wang,Yixue Xu,Yuwei Guo,Haiquan Xie,Junying Zhang
Graphitic carbon nitride (g-C3N4) is gaining more and more attentions as a promising metal-free photocatalyst for H2 production. Nevertheless, from the perspective of practical applications, the photocatalytic performance over g-C3N4 in visible-light region needs a further improvement. In this work, C doping and C quantum dots (QDs) are co-integrated in g-C3N4 by a one-step thermal polymerization method to obtain an advanced C QDs/C doped g-C3N4 photocatalyst. The synergistic effects of C doping and C QDs modification promote the photocatalytic activity of g-C3N4 significantly. The optimal C QDs/C doped g-C3N4 exhibits a significant improvement on visible-light-driven photocatalytic hydrogen production (205 μmol g−1 h−1) with an apparent quantum yield (AQE) at 420 nm reaching 1.24%, which is approximately nine-fold enhancement than that of pristine g-C3N4. The increased photocatalytic activity mainly benefits from the enhanced visible light absorption and carrier separation efficiency. This study may open a new perspective for the design and fabrication of C-modified g-C3N4 for photocatalytic hydrogen production.
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ACS Sustainable Chemistry & Engineering
·
2022
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IF 9.224
Jiayuan Sun,Shanshan Shao,Xinggang Hu,Xiaohua Li,Huiyan Zhang
The aqueous fraction of bio-oil from biomass fast pyrolysis mainly contains low-molecular-weight oxygenates such as carboxylic acids, ketones, aldehydes, phenols, and furans. In this study, the full components of aqueous bio-oil are directionally converted into carbonyl groups such as aldehydes and ketones, and then the oxygen-containing precursors of aviation fuel are prepared through coupling, focusing on exploring the mechanism of carbonylation and C–C coupling. Studies have revealed that propionic acid, furfural, and phenol can be directionally converted into ketones, in which reaction 3-pentanone, cyclopentanone, and cyclohexanone were formed via ketonization and hydrogenation in the aqueous phase. Then the two components of 3-pentanone, cyclopentanone, cyclohexanone, acetone, and acetaldehyde were subjected to aldol condensation to explore the C–C coupling mechanism in the preparation of the C7–C18 precursor of aviation fuel. The mechanism in the high-quality utilization of all components of the aqueous phase bio-oil fraction was explored, which was favorable for the synthesis of biomass-based aviation fuel.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
·
2019
·
IF 2.338
Li-ping RAN,Fei RAO,Ke PENG,Huan YIN,Mao-zhong YI
Ultrahigh-temperature ceramics were added to C/C composites to meet their application requirement in a high-temperature oxidizing environment. C/C−ZrB 2 −SiC composites were fabricated by high-solid-loading slurry impregnation with polymer infiltration and pyrolysis. The dispersion and rheological behavior of ZrB 2 slurry and the microstructural, mechanical, and ablation properties of the C/C−ZrB 2 −SiC composites were investigated. Results indicated that a well-dispersed and low-viscosity ZrB 2 slurry was obtained using 0.40 wt.% polyethyleneimine as a dispersant at pH 5. Ceramics were uniformly distributed in the short-cut fiber layer and needle-punched area. The flexural strength of the C/C−ZrB 2 −SiC composites was 309.30 MPa. The composites exhibited satisfactory ablation resistance under the oxyacetylene flame of 2500 °C, and the mass and linear ablation rates were 0.40 mg/s and 0.91 μm/s, respectively. A continuous and compact ZrO 2 layer, which could effectively reduce the diffusion rate of oxygen and protect the composites from being ablated, was formed.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
·
IF 4.2
Qifeng Yang,Yiming Mo
Selective oxidation of high-energy C–H bonds to produce carbonyl compounds is a fundamental transformation in fine chemical synthesis. Despite tremendous efforts, the development of green and safe strategies often suffers from harsh reaction conditions and uses homogeneous transition-metal catalysts. Herein, we present an electrochemical oxidation strategy that is green and safe for the direct oxidation of benzylic C–H bonds using La2O3 nanoparticles supported on a carbon paper (La2O3/CP) anode. La2O3/CP can selectively oxidize indane to indanone in 83% yield with 73% Faraday efficiency at room temperature. It also can oxidize different kinds of compounds with benzyl C–H bonds to produce the corresponding ketones with moderate-to-excellent yields. The oxygen source was confirmed to be water by an oxygen isotope (18O) tracer experiment. Additionally, the La2O3@C/CP composite electrode was reconfigured through carbonizing oleic acid to stabilize La2O3 on CP, resulting in an improved stability due to the reinforced catalyst embedding on CP, and retaining 81% initial activity after five cycles.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2023
·
IF 6.1
Wenwen Yang,Xiaoping Zhang,Jun Zhang,Guoshuan Wang,Hailong Liang,Xinglei Zhang,Konstantin Chingin,Huanwen Chen
The positions of C═C bonds in unsaturated fatty acids (FAs) are one of the main factors determining the quality of food flavor. Herein, we developed an approach for the determination of C═C bonds of FAs by online epoxidation reaction with water dimer radical cations. The limit of detection for octenoic acid isomers was ∼9 μg/L. The positions of C═C bonds in trans-2/3-hexenoic acid, trans-2/3-octenoic acid, oleic acid, linoleic acid, and linolenic acid in black tea or olive oil samples were directly determined by the established method. These results indicate that the established method allows the rapid determination of unsaturated FAs in black tea and olive oil. The advantages of this approach include the analysis speed (∼1 min per sample), simple device, and no need for complex pretreatment. This study not only provides a strategy for the determination of C═C positions but also offers new possibilities for applications in the field of food chemistry.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Junjie Xu,Wei Sun,Xiang Xiong,Hongbo Zhang,Lingkun Yang
To improve the mechanical properties and ablation resistance of Cf-reinforced ceramic-based materials, ZrC–W cermet composites (C/C–ZrC–W) were prepared in C/C preforms using slurries and low-temperature reactive melt infiltration , and their microstructure, formation mechanism, and mechanical and ablation properties were investigated. The obtained results revealed that the formation of C/C–ZrC–W composites involved the dissolution–precipitation and C diffusion processes. Owing to the precipitation of W nanoparticles in the ZrC phase and interdiffusion of W/ZrC, the fabricated C/C–ZrC–W composites exhibited superior mechanical properties with a flexural strength of 280.65 ± 12.84 MPa and fracture toughness of 13.87 ± 0.56 Mpa.m 1/2 . The formation of a Zr–W–O dense oxide layer resulted in the excellent ablation performance of the C/C–ZrC–W composites in oxyacetylene flame with a temperature of 2200 °C, and their mass ablation rate and linear ablation rate were 1.14 mg/s and 2.42 µm/s, respectively. The described method can be potentially used for preparing high-strength, high-toughness, and ablation-resistant materials at low temperatures.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Junjie Yan,Xiumei Wu,Qidong Liu,Yunping Li,Shu Yu
Silicon oxycarbide (SiOC) coatings were prepared through isothermal chemical vapor co-deposition by using two precursors of hexamethyldisilane (HMDS) and tetraethyl orthosilicate (TEOS). The microstructure, composition and the protectiveness on C/C composite against oxidation of the coatings prepared at temperatures ranging from 1423 K to 1563 K and pressures ranging from 500 Pa to 1200 Pa were investigated, respectively. After oxidation, cracks and defects were formed in the coatings of all conditions due to the volume shrinkage of amorphous SiO 2 crystallization and the mismatch of thermal expansion coefficient (CTE) between SiOC coatings and substrate. The most oxidation-resistant SiOC coating was obtained at 1563 K and 500 Pa, which exhibited the lowest weight loss rate of 4.87 % after 12 h of oxidation at 1673 K in air condition.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Yingying Zhou,Jia-jia Jiao,Huang Huang,Yong Dong Liu,Rugang Zhong,Xin Yang
Dichloroacetonitrile (DCAN) as one of the potentially prioritized regulated DBPs has drawn great attention; however, understanding its formation, especially the C–C bond cleavage mechanisms, is limited. In this study, DCAN formation mechanisms from long-chain primary amines, amino acids, and dipeptides during chlorination were investigated by a combined computational and experimental approach. The results indicate that nitriles initially generate for all of the above precursors, then they undergo β-C-hydroxylation or/and α-C-chlorination processes, and finally, DCAN is produced through the Cα–Cβ bond cleavage. For the first time, the underlying mechanism of the C–C bond cleavage was unraveled to be electron transfer from the O– anion into its attached C atom in the chlorinated nitriles, leading to the strongly polarized Cα–Cβ bond heterocleavage and DCAN– formation. Moreover, DCAN molar yields of precursors studied in the present work were found to be determined by their groups at the γ-site of the amino group, where the carbonyl group including −CO2–, −COR, and −CONHR, the aromatic group, and the −OH group can all dramatically facilitate DCAN formation by skipping over or promoting the time-consuming β-C-hydroxylation process and featuring relatively lower activation free energies in the C–C bond cleavage. Importantly, 4-amino-2-hydroxybutyric acid was revealed to possess the highest DCAN yield among all the known aliphatic long-chain precursors to date during chlorination. Additionally, enonitriles, (chloro-)isocyanates, and nitriles can be generated during DCAN formation and should be of concern due to their high toxicities.
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PubMed
高影响因子
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