RSC Advances
·
2015
·Vol. 5
·期 85
·69854-69860
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IF 3.84
Suyun Tian,Jing Sun,Siwei Yang,Peng He,Shengju Ding,Guqiao Ding,Xiaoming Xie
Rapid thermal exfoliation/reduction of graphite oxide is a fast and easy method among the oxidation–reduction approaches for graphene synthesis. In this research, we firstly demonstrated that graphene can be obtained with a surface area of 550 to 700 m2 g−1 and a yield of approximately 50% through one-step rapid thermal treatment in air from 450 to 550 °C, without vacuum or protective gas through a self-protection process. Then, we further demonstrated the effective two-step thermal annealing to significantly improve the C/O ratio from ca. 7.3 to 25.9 in air at the relatively low temperature of 600 °C. The smart self-protecting and enhanced-oxygen-removal mechanisms were discussed.
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JOURNAL OF ORGANIC CHEMISTRY
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2023
·
IF 3.6
Benqiang Cui,Ye Tian,Yongchao Gao,Shaoyi Hua,Yanhui Shi,Changsheng Cao
Direct introduction of silyl radicals to forge C–Si bonds is of central importance in organic synthesis, owing to the formidable potential of silyl groups as coupling partners for further derivatization reactions to achieve more valuable compounds. Cleavage of heteroaromatic endocyclic carbon–heteroatom bonds to assemble C–Si bonds is scarce. Here, we demonstrate a dearomatization silylation of benzofurans and furopyridines via silyl radical addition and C(2)–O bond scission under metal-catalyst-free and mild conditions. Preliminary mechanistic experiments suggest that these transformations involve radical/single-electron transfer and [1,5]-Brook rearrangement processes. This protocol for the total synthesis of Doxepin and oxyresveratrol derivatives is carried out. The silylated products in several transformation reactions have proven to be useful as synthetic intermediates.
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Catalysts
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2022
·Vol. 12
·期 10
·1278
·
IF 4.501
Ying Wang,Huilin Xie,Kunming Liu,Jinhui Li,Jin-Biao Liu
Herein, we report a copper-catalyzed C-O cross-coupling of N-methoxy amides and arylboronic acids for the synthesis of aryl-N-methoxy arylimides. The fully selective O-arylation of the N-methoxy amides is found to be greatly prompted by the inexpensive and commercially available CuI. The reaction conditions tolerate a variety of functional groups and promote different reactivities depending on the electronic and steric properties of the distorted substrates.Keywords:copper catalyzed;N-methoxy amides;selective C-O cross-coupling;aryl-N-methoxy arylimides
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CHINESE JOURNAL OF CATALYSIS
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2026
·
IF 17.2
Chongzheng Xu,Haoping Di,Fengyue Sun,Wenjing Bao,Yanwei Ju,Dengwei Yan,Changle Yue,Yiyuan Xu,Yunxiu Zhao,Shuo Wang,Jiqian Wang,Yukun Lu
Sulfided NiMo catalysts can effectively hydrogenate oxygen-rich bio-oils into high quality hydrocarbon fuels. However, precisely controlling the cleavage of C−O bonds remains challenging. Here, we synthesized an oil-soluble precursor NiMo 6 -DODA by encapsulating the polyoxometalates (POMs) (NH 4 ) 4 [NiMo 6 O 24 H 6 ] (NiMo 6 ) with surfactants, followed by in-situ construction of an ultra-dispersed monolayer NiMoS catalyst. The “surfactant shell” of the precursor ensured its homogeneous dispersion in the oil phase, while gradually sacrificing and decomposing during the sulfidation to mitigate the aggregation of the MoS 2 nanosheets. Meanwhile, the well-defined “POMs core” established an atomic-level Ni-Mo proximity, ensuring the dominance of the Ni-promoted MoS 2 active phase. This design not only altered the adsorption configuration of esters on the NiMo catalyst but also introduced abundant edge sulfur vacancies to promote oxygen atom adsorption and accelerate C−O bond cleavage. The results showed that NiMo 6 -DODA achieved 100% conversion of methyl palmitate and 100% alkane selectivity under low catalyst loading conditions. Notably, the selectivity for n -hexadecane reached 94.2%, significantly surpassing that obtained with a commercial oil-soluble precursor (69.8%). Furthermore, the catalyst maintained high activity across multiple reaction cycles and in the solvent-free conversion of real bio-oils. This strategy of pre-assembly combined with sacrificial sulfidation provides a simple and effective route for designing hydrodeoxygenation catalysts that enable precise control over ester C−O bond cleavage.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2023
·
IF 8.7
Chen Yang,Jian Yang,Shuangshuang Liu,Mingxue Zhao,Xu Duan,Hongli Wu,Lang Liu,Weizao Liu,Jiangling Li,Shan Ren,Qingcai Liu
Owing to its feasibility, efficiency in light-harvesting and effectiveness in the interfacial charge transfer between two n-type semiconductors, constructing heterojunction photocatalysts have been identified as an effective way for enhancing the photocatalytic properties. In this research, a C–O bridged CeO 2 /g-C 3 N 4 (cCN) Step-scheme (S-scheme) heterojunction photocatalyst was constructed successfully. Under visible light irradiation, the cCN heterojunction exhibited the photocatalytic degradation efficiency of methyl orange, which was about 4.5 and 1.5 times higher than that of pristine CeO 2 and CN, respectively. The DFT calculations, XPS and FTIR analyses demonstrated the formation of C–O linkages. And the calculations of work functions revealed the electrons would flow from g-C 3 N 4 to CeO 2 due to the difference in Fermi levels , resulting in the production of internal electric fields . Benefiting from the C–O bond and internal electric field, the photo-induced holes in the valence band of g-C 3 N 4 and the photo-induced electrons from conduction band of CeO 2 would be recombined when exposed to visible light irradiation, while leaving the electrons with higher redox potential in the conduction band of g-C 3 N 4 . This collaboration accelerated the separation and transfer rate of photo-generated electron-hole pairs, which promoted the generation of superoxide radical (•O 2 − ) and improved the photocatalytic activity .
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Catalysts
·
2022
·Vol. 12
·期 11
·1328
·
IF 4.501
Liang-Qiu Huang,Zhi-Jun Diao,Bo Chen,Qing-Pan Du,Kai-Yang Duan,Si-Jia Zhao
Efficient depolymerization of C–O linkages is essential for converting lignin into fuels and higher value-added chemicals. In this work, CoRuP/SiO2, an amorphous Ru-Co phosphide composite, was fabricated for the efficient hydrogenolysis of ether linkages. The 4–O–5 andα–O–4 linkages containing lignin-related compounds, such as diphenyl ether, benzyl phenyl ether, 3-methyl diphenyl ether, and dibenzyl ether, are selected as representatives of linkages in lignin. Under mild conditions, Ru-containing metallic phosphides have high-performance for the catalytic depolymerization of C–O linkages. Compared with other catalysts, CoRuP/SiO2shows an outstanding selectivity for benzene and excellent efficiency in depolymerizing diphenyl ethers, yielding only a small amount of by-products. Furthermore, the total acidity shows a linear relationship with the hydrogenolysis reactivity in cleaving aromatic ether bonds. The mechanisms for the catalytic hydrogenolysis of 4–O–5 andα–O–4 bonds over CoRuP/SiO2are proposed. Moreover, two-dimensional heteronuclear single quantum coherence nuclear magnetic resonance spectroscopic analysis demonstrates that CoRuP/SiO2could effectively depolymerize C–O bonds of lignin. These dominant hydrogenolysis products from lignin have excellent potential in the production of high value-added drugs or pharmaceutical intermediates. The hydrogenolysis of lignin can be a highly efficient alternative to the existing method of lignin utilization.Keywords:hydrogenolysis;C–O linkages;metallic phosphides;reaction pathway
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Hong Li,Xinzhu Wen,Feng Shao,Shiwei Xu,Chao Zhou,Yafei Zhang,Hao Wei,Nantao Hu
Rational materials design is critical to develop advanced electrodes for high-performance sodium-ion battery. In this work, a well-designed structure with interlayer-expanded molybdenum disulfide (MoS 2 ) vertically anchored on graphene substrates (v-MoS 2 /rGO) is achieved by one-pot hydrothermal synthesis . The vertical anchored MoS 2 and high conductivity graphene sheets provide a good path for electrons/ion transfer. More importantly, the direct linkage of O from functional group on graphene oxide (GO) with edge S of MoS 2 (C-O-S) is constructed, which can maintain the stability of the v-MoS 2 /rGO electrode and enhance its electrons transport rate for the high-rate performance and long cycle life. The assembled sodium-ion battery shows high rate performance (129.2 mAh g −1 at 10 A g −1 ) and long cycling stability (251.2 mAh g ‐1 −1 at 2 A g −1 after 1000 cycles with an ultra-low degradation of 10.9 μAh g −1 per cycle). The excellent performance makes the designed structure a fascinating anode for sodium battery.
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MACROMOLECULES
·
2020
·
IF 5.918
Fan Zhang,Tiantian Li,Wanting Chen,Xiaoming Yan,Xuemei Wu,Xiaobin Jiang,Yang Zhang,Xiaozhou Wang,Gaohong He
As critical triggers, both the electron-withdrawing links and neighboring cationic groups induce and accelerate the aryl ether cleavage in the widely used aryl ether containing anion exchange membranes (AEMs). Herein, a novel alkaline stable polyelectrolyte is proposed by converting the electron-withdrawing C═O links in the widely used poly(aryl ether ketone) backbone into the electron-donating C–NH2 links, and then grafting faraway para-type cations by Leuckart-Menshutkin reaction without using noble metal catalysts. Contributions of the elimination of electron-withdrawing C═O links and graft of para-type cations to the excellent alkaline stability of the aryl ether containing polyelectrolytes are demonstrated through density functional theory, as the increasing electron cloud density on the ether-connected carbon atom elevates the activation energy barrier to OH– initiated aryl ether cleavage, and the para-type cation is more stable than the conventional ortho-type cation due to the sterical protection and low electrophilicity to benzylic carbon. By converting C═O to C–NH2 groups and then tuning the quaternization degree, the remaining C–NH2 groups in the polymer backbone could form hydrogen bonding networks to reinforce the membranes. The novel quaternized poly(aryl ether amine) membrane exhibits high conductivity (92.2 mS cm–1 at 80 °C), excellent mechanical properties (48.2 MPa, 51.3%), and suppressed swelling ratio (12.8% at 80 °C). Excellent alkaline stability is also confirmed experimentally with no polymer backbone degradation even in harsh conditions (4 M KOH, 80 °C, 400 h), which is at the top level among the state-of-the-art side chain and aryl ether-free types of AEMs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Hongping Li,Tianxiao Zhu,Yuan Zhang,Jie Yin,Jinrui Zhang,Linhua Zhu,Hua Wei,Huaming Li
Adsorbents with high adsorption capacity and selectivity have long been the pursuit of researchers in the field of adsorptive desulfurization. In this study, a novel single-atom adsorbent comprised of iron (Fe) integrated into C, O co-doped hexagonal boron nitride (Fe-BNCO) has been successfully synthesized. This unique material demonstrates outstanding adsorption capabilities, boasting an adsorption capacity of 49.7 mg S/g and excellent selectivity for adsorptive desulfurization. Notably, this adsorption capacity is 48.6 % higher than that of pure BNCO. The incorporation of the Fe element into boron nitride materials induces a reduction in crystallinity and an increase in specific surface area, resulting in a higher number of available adsorption sites. Combining experimental analysis with theoretical calculations, we propose that the exceptional adsorption performance of Fe-BNCO can be attributed to the formation of S-Fe coordination interaction, while maintaining the existing π-π interactions. This study advances our understanding of adsorbents with high adsorption capacity and selectivity, providing valuable insights for the field of adsorptive desulfurization.
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ACS Applied Polymer Materials
·
2022
·
IF 4.855
Yue Yao,Baolong Wang,Feng Zhao,Zhen Hu,Yudong Huang
The extensive use of unsaturated polyester resins and their composites has resulted in an increasingly aggravating problem of waste materials which are difficult to remold or degrade endowed by their highly crosslinked network. A simple and facile recovery method to fully degrade resins remains challenging so far. Here, a hindered C–O bond with a carbonyl group in the β-position of steric ester was introduced into the design and preparation of a dimethacrylate monomer and its self-polymerized unsaturated polyester resin. The obtained resin with good thermal, mechanical, and solvent-resistance properties could be efficiently degraded within 3.5 h at 90 °C at an 80% concentration of aqueous hydrazine hydrate. Selective cleavage of the hindered bond due to steric and electronic effects was activated by the prior addition of the introduced carbonyl group. Degradation products rich in benzene and carboxyl/carboxylate groups respectively could be separated readily according to the water solubility, being expected to be reused as a flocculant and other functional additives. This work provides a promising strategy for the facile recycling of unsaturated polyester resins.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Zhuoran Song,Daohu Sheng,Siyao Cheng,Mengmeng Zhang,Aming Xie
The development of two-dimensional (2D) metal composite materials for electromagnetic wave (EMW) absorption is hindered by complex fabrication processes, high raw material costs, and insufficient absorption performance. We ingeniously integrate a multi-metal doping strategy with the oxygen-rich two-dimensional structure of p(C₃O₂)ₓ to successfully construct a defect-rich two-dimensional metal composite microwave absorber. Spectroscopic analysis reveals that multi-metal doping and oxygen release during pyrolysis generate abundant heterogeneous interfaces (oxides/alloys) and induce pronounced electron delocalization, promoting lattice distortions and defect formation. This synergistic effect significantly enhances both local dipole and interfacial polarization, boosting dielectric response. Consequently, the optimized OC-FeMnCuCo sample achieves exceptional EMW absorption with a minimum reflection loss (RL min ) of –55.0 dB and a broad effective absorbing bandwidth (EAB) of 6.8 GHz at an ultra-thin thickness of 1.9 mm. CST simulations further confirm its practical applicability. This work provides a simple, cost-effective strategy for designing advanced 2D absorbers.
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INDUSTRIAL CROPS AND PRODUCTS
·
2026
·
IF 6.4
Zheyuan Ding,Juncheng Zhao,Jiaming Zhang,Junzhong Xie,Kunye Zhang,Cenkai Zhao,Jikun Xu,Yu Wang,Xuepin Liao,Xiao Xiao,Bi Shi
A 100% lignin β -O-4 model conversion with 93.1% monomer selectivity and a high TON was obtained. • The interplay between Ru particle and single atom contributed to the high performance. • Favorable stability under high-temperature heating and high-pressure with reusability > 97%. Catalytic hydrogenolysis is a promising strategy for converting lignin into valuable aryl platform chemicals, contingent upon the availability of high-performance catalysts. The philosophy for the catalyst rational design towards high conversion and selectivity was rarely reported to the best of our knowledge. We illustrate the synergistic interplay between Ru particles and single atoms, contributing to the high catalytic performance. The N-doped carbon-supported Ru catalyst is designed by combining collagen fiber-immobilized tannin adsorption with carbonization (TNC). The Ru is finely dispersed on the TNC support in the form of both single atoms and nanoparticles at a low metal loading of 0.91 wt% (noted as Ru/TNC). It achieved a 100% conversion with a 93.1% aromatic monomer yield in the catalytic hydrogenolysis of lignin β –O–4 model 2-phenoxy-1-phenylethanol (PPE) at 260 °C and 2 MPa H 2 . The primary products of this reaction included ethylbenzene, cyclohexanol, and ethylcyclohexane, and a high turnover number (TON) of 955 was obtained, which surpassed most reports. Specifically, the Ru particle sites facilitate efficient H 2 dissociation, while the single-atom sites provide a weakly adsorbing environment for reaction intermediates due to electron-rich isolated Ru atoms, thereby effectively suppressing over-hydrogenation. This work offers a promising catalyst rational design principle for selective hydrogenation for efficient C–O bond cleavage of lignin, demonstrating significant potential in transforming lignin into value-added platform chemicals. Download: Download high-res image (151KB) Download: Download full-size image Possible reaction pathway on Ru/TNC catalyst consisting of Ru particle and Ru single atom. The intermediates easily desorbed over Ru single atom site due to the weak adsorption. Purple ball: Ru atom, red ball: N atom, white ball: H atom where Ru particles serve as H* species supply pump due to H spillover.
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