JOURNAL OF ORGANIC CHEMISTRY
·
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.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Ruotong Cui,Wenlong Xu,Feng Liu,Lei Yu,Jiming Liu,Xi Chen,Yingyun Qiao,Yuanyu Tian
The structure and reactivity of coal is the core problem of coal chemistry, and solving it at the molecular level has been an international unsolved problem. The chemical similarity-based coal chemistry group elevates the study from the macroscopic to the molecular level. However, the previous free radical mechanism lacks experimental confirmation and theoretical computational support. Here, the pyrolysis products of model compounds are first utilized to predict pyrolysis. The hydrogen-donating solvent is then used as a radical trap to confirm the reaction. Subsequently, density functional theory calculations are utilized to aid in the validation. Finally, family components are utilized to demonstrate the universality of the free radical mechanism of coal pyrolysis. This work combines radical trapping with quantum chemical calculations to analyze the radical reaction mechanism of coal pyrolysis in depth at the molecular level. This will provide a theoretical basis for coal pyrolysis and clean and efficient utilization.
研究领域:
煤化学
·
量子化学
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
材料科学
·
能源与环境化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Liang Jiang,Guangyue Xu,Yao Fu
The conversion of lignin into value-added chemicals is one of the important ways for sustainable development. Herein, phytic acid, a biomass-derived chemical, was used as the phosphorus source and pore former to synthesize the AlPyOx support. After loading Ni, the Ni/AlPyOx catalysts were found to be highly active in the catalytic conversion of lignin model compounds to high-value-added chemicals under mild conditions. The benzyl phenyl ether (α-O-4 lignin model compound) could be completely converted into toluene and phenol with near-equivalent selectivity at 30 °C and 3 MPa H2. Diphenyl ether and 2-phenoxy-1-phenylethanol were also used as 4-O-5 and β-O-4 model compounds of lignin, respectively. The unique activity of Ni/AlP0.5Ox could be attributed to metallic Ni that interacts with AlP0.5Ox and the unique adsorption of substrates on the carrier. Lignin can also be degraded over Ni/AlP0.5Ox via selective cleavage of the C–O bond, and 26.60 wt % yield of identified monomers was obtained.
研究领域:
催化化学
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生物质能
·
可持续发展
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Kun Zhou,Wei Liu,Peifang Wang,Juan Chen,Huinan Che,Bin Liu,Yanhui Ao
Rational design of piezo-assisted photocatalytic systems for simultaneously efficient ultilization of solar and mechanical energy is promising but still challenging. In this work, a novel Bi 4 Ti 3 O 12 @C (BTO@C) Schottky heterojunction with high piezo-assisted photocatalytic performance is rationaly designed, and the degradation reaction rate constant k for RhB reaches 0.092 min −1 in 30 min. Experimental results and density functional theory (DFT) calculations show that C-layer is tightly coated on the surface of BTO. Furthermore, C-O covalent bonds , which act as electron transfer channels, are formed at the interface of BTO and C-layer. Meanwhile, the presence of piezoelectric potential field of BTO@C under piezo-assisted photocatalytic conditions further promotes the transfer of photogenerated electrons from BTO to C-layer, which synergistically contributes to the performance enhancement. This work provides a new idea for the design and development of efficient piezo-assisted photocatalytic materials.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2019
·
IF 4.745
Na Li,Jinku Bai,Xiaolin Zheng,Honghua Rao
An iron-catalyzed methylene forming strategy is disclosed through sequential C–H and C–O bond functionalization of methanol with cosolvent water. This protocol provides an easy and novel access to methylene-tethered imidazo[1,2-a]pyridine and 2-aminopyridine analogues in a sustainable manner and represents a complementary approach to traditional methylene forming strategies.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL SCIENCES
·
2017
·Vol. 129
·期 3
·289-294
·
IF 1.235
LIU YAOWEN,ZHAO FEN,ZHOU HAOHUA,XIE KAI,JIANG YUBO
CuI-catalyzed selective Ullmann C–O coupling of 1,4-disubstituted 1,2,3-triazole bromides with phenols were achieved through the coordination of N(2) atom. The ortho C–Br bond in N(1) aryl can be selectively coupled with phenols, while other C–Br bonds remain inert, generating ortho aryloxyl 1,4-diaryl 1,2,3-triazoles.
CuI-catalyzed selective Ullmann C–O couplings of 1,4-disubstituted 1,2,3-triazole bromides with phenols were achieved through the coordination of N(2) atom in triazole. The ortho C-Br bond in N(1) of aryl can be selectively coupled with phenols, while other C-Br bonds remain inert, generating ortho -aryloxyl 1,4-diaryl 1,2,3-triazoles.
研究领域:
有机化学
·
药物化学
·
生物有机化学
·
催化化学
·
合成方法学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 21
·17644-17651
·
IF 3.201
Shaobo Li,Tao Zhu,Lichun Dong,Mingdong Dong
Heteroatom doping has been demonstrated to be an effective way to tune the properties of nanomaterials including chemical reactivity and electronic and optical performance. In this study, rGO/g-C3N4 and boron doped rGO/g-C3N4 (B-rGO/g-C3N4) nanocomposites were fabricated via a rapid plasma treatment method, and their photocatalytic performance under visible light radiation was examined. The results showed that the photocatalytic efficiency of B-rGO/g-C3N4 for rhodamine B degradation can be 50% higher than that of rGO/g-C3N4 at an optimum rGO loading of 5 wt%. XPS and FTIR analyses indicated the enhanced C–O–C covalent bonding between rGO and g-C3N4 in B-rGO/g-C3N4, and the optical characterization demonstrated that it could further improve the separation of the photo-generated chargers and narrow the bandgap of the nanocomposite. This work provides an idea that boron doping could be an effective way to promote the chemical interaction between different components in composite materials, which is important in designing and developing new functional nanomaterials.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Chengyao Zhao,Yiming Lin,Qiaoyan Lin,Qi Liu,Yujing Liu,Zhongqiu Liu,Anguo Ying
Aqueous zinc-ion hybrid capacitors (ZIHCs) are a promising new type of energy storage device, but there is a plight that the unsatisfactory Zn 2+ storage capability of carbonaceous cathodes limits further application. To address this issue, desolvation strategy is employed to tailor the solvation sheath of Zn 2+ in the ultra-micropores (0.59 nm) nanospheres , where H 3 PO 4 acts as phosphorus source for forming C-P bonds and enhancing C=O bonds to further reduce the desolvation energy barrier. In practical application, a quasi-solid-state flexible ZIHC is constructed, which provides a battery-level energy density (293.4 Wh kg −1 ) at a power density (180 W kg − 1 ) and a remarkable capacity retention of 93.4 % after 10 000 cycles. Electrochemical analyses, DFT calculations and structural characterization reveal that ultra-microporous is proved to be a prerequisite for C-P/C=O that are expected to further deplete solvent molecules within a Zn 2+ solvation sheath. Also, the coupling effect between the strong adsorption of Zn 2+ by C-P/C=O and the hydrophobic effect of C-P play an important role in facilitating desolvation process. This work creates a precedent for the application of ultra-microporous carbon materials in ZHICs and provides a brand-new approach for breaking the bottleneck of the low energy density and poor lifespan of ZHICs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Caitao Chen,Juan Ma,Yakun Tang,Xiaohui Li,Guangbo Liu,Hanyao Song,Yingluo He,Noritatsu Tsubaki,Lang Liu,Ting Liu
Cleaving the aromatic ether C-O bonds of lignite through catalytic hydroconversion (CHC) presents a significant challenge for producing organic chemicals and clean liquid fuels, which are vital for a sustainable future. In this study, we employed a sacrificial template-self-recovery strategy to synthesize highly dispersed and carbon-coated bimetallic catalysts MCo/C (M = Fe, Cu, Ni) for the CHC of Naomaohu coal (NMHC) and lignite-related model compounds (LRMCs). The carbon-coated NiCo bimetallic alloy catalysts, benefiting from the high dispersity of the active components and the synergistic effect between Ni and Co, exhibited excellent hydrogenolysis activity towards diphenyl ether (DPE). DPE conversion reached 100 % over Ni 3 Co 1 /C under optimal conditions (120 °C, 2 MPa H 2 , 2 h). Moreover, Ni 3 Co 1 /C significantly increased the content of arenes and alkanes while reducing the content of oxygen-containing compounds in the NMHC soluble portion (SP), demonstrating its efficient catalytic hydrogenolysis and hydrodeoxygenation capabilities. Density Functional Theory (DFT) calculations revealed that the Ni 3 Co 1 /C catalyst could activate H 2 to generate hydrogen radicals and diatomic active hydrogen, which are the primary hydrogen species involved in the reaction and affect the CHC of DPE. The experimental results can provide a reference for the conversion of lignite into clean liquid fuels.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Chuhan Zhang,Yanchang Chu,Linying Fu,Qiuyue Wang,Rui Ma,Donghai Xu,Le Yang
Lignin, a renewable resource rich in aromatic ring structures in nature, is an ideal natural source to produce aromatic compounds and cycloparaffin. Herein, we prepare MOF-derived Ni–MoxC/C and Co–MoxC/C as catalysts for the depolymerization of lignin and dimeric model compounds. Diphenyl ether (DPE) with 4-O-5 bond, benzyl phenyl ether (BPE) with α-O-4, and phenethyl phenyl ether (PPE) with β-O-4 are chosen as dimeric model compounds. Overall, Ni–MoxC/C and Co–MoxC/C show distinguished different activity toward product distribution. Ni–MoxC/C facilitates both C–O bond cleavage and hydrogenation of the benzene ring, and the main products are ethyl cyclohexane and cyclohexanol for all three model compounds. In contrast, Co–MoxC/C only facilitates C–O bond cleavage and obtains phenol and ethylbenzene as products. Similarly, for the depolymerization of lignin, cycloparaffins are obtained on Ni–MoxC/C, while phenol, guaiacol, 2,6-dimethoxyphenol, and their respective derivatives are obtained on Co–MoxC/C.
研究领域:
化学工程
·
可再生资源利用
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2013
·Vol. 27
·期 6
·337-340
·
IF 2.011
Junyu Dong,Tianbin Li,Chuan Dai,Wen Weng,Xinghua Xue,Yuyu Zhang,Qingle Zeng
A straightforward, protecting-group-free protocol for the synthesis of chiral 6-substituted and 6,6’-disubstituted binols (binol = 1,1’-bi-2-naphthol) by palladium-catalyzed hydroxylation, C–N and C–O coupling of chiral 6-bromo- and 6,6’ -dibromo-1,1’-binaphthols is developed. The protecting group free palladium-catalyzed hydroxylation, C–O and C–N cross-coupling protocol affords a straightforward and general method for the synthesis of chiral 6-substituted and 6,6’-disubstituted binols with good yields, avoiding the tedious procedures of introduction and removal of protecting groups. Copyright © 2013 John Wiley & Sons, Ltd.
研究领域:
有机化学
·
合成化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）