Nature Communications
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2024
·Vol. 15
·期 1
·1-11
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IF 14.7
Jia Shunhan,Zhang Libing,Liu Hanle,Wang Ruhan,Jin Xiangyuan,Wu Limin,Song Xinning,Tan Xingxing,Ma Xiaodong,Feng Jiaqi,Zhu Qinggong,Kang Xinchen,Qian Qingli,Sun Xiaofu,Han Buxing
Nitrogen oxides (NO x ) play important roles in the nitrogen cycle system and serve as renewable nitrogen sources for the synthesis of value-added chemicals driven by clean electricity. However, it is challenging to achieve selective conversion of NO x to multi-nitrogen products (e.g., N 2 H 4 ) via precise construction of a single N-N bond. Herein, we propose a strategy for NO x -to-N 2 H 4 under ambient conditions, involving electrochemical NO x upgrading to NH 3 , followed by ketone-mediated NH 3 to N 2 H 4 . It can achieve an impressive overall NO x -to-N 2 H 4 selectivity of 88.7%. We elucidate mechanistic insights into the ketone-mediated N-N coupling process. Diphenyl ketone (DPK) emerges as an optimal mediator, facilitating controlled N-N coupling, owing to its steric and conjugation effects. The acetonitrile solvent stabilizes and activates key imine intermediates through hydrogen bonding. Experimental results reveal that Ph 2 CN* intermediates formed on WO 3 catalysts acted as pivotal monomers to drive controlled N-N coupling with high selectivity, facilitated by lattice-oxygen-mediated dehydrogenation. Additionally, both WO 3 catalysts and DPK mediators exhibit favorable reusability, offering promise for green N 2 H 4 synthesis.
研究领域:
化学工程
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环境科学
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材料科学
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DOI
PubMed
高影响因子
ChemistrySelect
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2024
·Vol. 9
·期 18
·e202304772
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IF 1.9
Chenghao Tang,Chaoyang Song
Graphical Copper encapsulated N-rich carbon material derived from porous organic polymer was found to be highly active heterogeneous catalyst for solvent-free coupling of acyl chlorides with alkynes. Copper promoted Sonogashira coupling has recently emerged as an attractive route for synthesizing α, β-Acetylenic ketones (ynones). In this study, a porous organic polymer based on [2,6-Bis(1,2,3-triazol-4-yl)pyridine] (BTP) was prepared through oxidative coupling. By incorporating copper salt and subsequent pyrolysis, copper encapsulated N-doped carbon materials were obtained. The resulting copper/carbon materials exhibited excellent catalytic performance for the coupling of acyl chlorides and alkynes due to their large surface area, abundant mesopores, and uniformly distributed metal nanoparticles. The reaction proceeded efficiently, yielding ynones with good to excellent yields at room temperature within a short reaction time (4 h) using only 0.4 mol % catalyst. Compared to previously reported copper nanocatalysts, the N-doped carbon materials supported copper catalyst demonstrated higher catalytic activity and operated at lower reaction temperatures. Additionally, the catalyst displayed reliable recyclability without any significant loss in catalytic activity.
研究领域:
化学
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材料科学
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高影响因子
INORGANIC CHEMISTRY
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2021
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IF 5.165
Heng-Zhi Liu,Bo Li,Haiqiang Luo,Xiaohang Qiu,Jian-Gong Ma,Peng Cheng
Metal–organic frameworks (MOFs) represent an ideal platform for the construction of highly active composite catalysts. However, loading metastable and/or multicomponent metal compounds into MOFs remains a synthetic bottleneck due to the great challenge of keeping the guest and matrix intact during the preparation of a composite. In this work, we develop a new impregnation reduction surface modification (IRSM) strategy to give a new composite catalyst CuCl@MIL-101(Cr), which is successfully postmodified by in situ construction of CuII defects on the surface of loaded CuCl inside MOF pores, leading to the new composite material CuII/CuI@MIL-101(Cr). The new dual-component composite catalyst exhibits a hierarchical structure and superior catalytic activity in C–C homocoupling of arylboronic acids under green conditions. This study presents a facile strategy for improving the catalytic activity by constructing defects on the surface of MOF-based catalysts as well as for forming multiple-component composite materials.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
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2017
·Vol. 44
·期 4
·2289-2303
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IF 1.369
Li Jianhui,He Shaopo,Fu Haiqing,Chen Xin,Tang Min,Zhang Dela,Wang Bo
Presented here is an efficient one-pot and catalyst-free procedure for the synthesis of amides starting from carboxylic acids and amine/ammonium salts using 2,2-dichloro-1,3-diisopropylimidazolidine-4,5-dione as the coupling agent. Reactions can proceed smoothly even with those bearing thermosensitive group(s) at ambient temperature, and the corresponding products of primary, secondary and tertiary amides can be afforded in moderate to excellent yields of up to 96%.
研究领域:
有机化学
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合成化学
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DOI
高影响因子
Nanoscale
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2025
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IF 5.1
Mohammadreza Rostami,Biao Yang,Xiaochuan Ma,Sifan You,Jin Zhou,Meng Zhang,Xuefeng Cui,Haiming Zhang,Francesco Allegretti,Bing Wang,Lifeng Chi,Johannes Barth
n-Armchair graphene nanoribbons (nAGNRs) are promising components for next-generation nanoelectronics due to their controllable band gap, which depends on their width and edge structure. Using non-metal surfaces for fabricating nAGNRs gives access to reliable information on their electronic properties. We investigated the influence of light and iron adatoms on the debromination of 4,4”-dibromo-p-terphenyl precursors affording poly(para-phenylene) (PPP as the narrowest GNR) wires through the Ullmann coupling reaction on a rutile TiO2(110) surface, which we studied by scanning tunneling microscopy and X-ray photoemission spectroscopy. The temperature threshold for bromine bond cleavage and desorption is reduced upon exposure to UV light (240-395 nm wavelength), but the reaction yield could not be improved. However, in the presence of codeposited iron adatoms, precursor debromination occurred even at 77 K, allowing for Ullmann coupling and PPP wire formation at 300-400 K, i.e., markedly lower temperatures compared to the conditions without iron adatoms. Furthermore, scanning tunneling spectroscopy data reveal that adsorbed PPP wires feature a band gap of ≈ 3.1 eV.
研究领域:
材料科学
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表面化学
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DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2020
·Vol. 22
·期 11
·6222-6230
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IF 3.43
Xiao Yan,Yafei Luo,Wei Liu,Li Liang,Ya Gan,Zhongzhu Chen,Zhigang Xu,Hua Wan,Dianyong Tang,Hubing Shi,Jianping Hu
Unveiling the reaction mechanism is significant for developing high-performance catalysts. In this paper, a series of precisely controlled PdxM147−x (M = Cu, Pt, Au, Rh, Ru) dendrimer encapsulated nanoparticles (DENs) has been successfully synthesized. The mechanisms of PdxM147−x as catalysts for Suzuki cross-coupling reactions were investigated by combining experimental and theoretical methods. The experimental results indicate that Pd74Cu73 DEN shows similar activity to Pd147 DEN and excellent substrate adaptability under mild reaction conditions. Moreover, the Cu component can play an important role in tuning the catalytic activity of PdxCu147−x DEN. Density functional theory (DFT) calculations illustrate that the similar activities of the Pd147 and Pd74Cu73 DENs originate from the comparable energy barriers of the rate-determining steps. The partial density of states (PDOS) and electron density differences demonstrate that Cu decreases the intensities of the valence orbitals of the top and edge Pd atoms and weakens orbital interactions between the intermediates and Pd74Cu73 DEN, leading to low desorption energies of the products. This work can provide a promising strategy to reduce the cost of Pd catalysts in Suzuki cross-coupling reactions.
研究领域:
化学
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材料科学
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催化反应机制
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DOI
PubMed
高影响因子
JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY
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2024
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IF 1.3
Li Ziling,Shi Chundiao,Xiang Shengchang,Liu Chulong,Zheng Ximing
As an oral Janus kinase 1 inhibitor, upadacitinib shows good activity in the treatment of rheumatoid arthritis, especially for other drug-resistant and refractory rheumatoid arthritis patients. A key step in the synthesis of upadacitinib is the introduction of ethyl on the pyrroline ring. Here, a FeCl3/p-aminophenol catalyst system was used to increase the ethyl introduction for synthesis of pyrroline building blocks of upadaticinib. This catalytic system allows milder reaction conditions and increases the yield of this step by 25% compared to the existing reports, and the scale-up experiment is still effective. In addition, a possible FeII/FeIV catalytic mechanism for this reaction was also proposed.
研究领域:
有机化学
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药物化学
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催化反应机制
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
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2014
·Vol. 28
·期 9
·673-677
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IF 2.017
Limin Ren,Wenyi Chu,Dinghui Guan,Yanjun Hou,Man Wang,Xiaobin Yuan,Zhizhong Sun
A simple and efficient route for the preparation of terphenyl derivatives via palladium-catalyzed sequential directed C―H arylation/Suzuki–Miyaura cross-coupling in ‘one-pot’ has been developed. 4,4′-(Cyclohexane-1,1-diyl)diphenol is an essential ligand. This reaction can tolerate a series of functional groups and provides the terphenyl derivatives in moderate to good yield. Copyright © 2014 John Wiley & Sons, Ltd.
研究领域:
有机化学
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合成化学
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DOI
高影响因子
CATALYSIS COMMUNICATIONS
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2014
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IF 3.32
Xuanduong Le,Zhengping Dong,Zhicheng Jin,Qingqing Wang,Jiantai Ma
In this study, a novel Pd(II) complex functionalized core–shell magnetic mesoporous catalyst (Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II)) was synthesized by a simple cost effective procedure. It was characterized by transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, vibrating sample magnetometer, and nitrogen physical adsorption. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst offered high surface area and exhibited excellent activity towards Suzuki–Miyaura cross-coupling reaction of halides with aryl boronic acids in ethanol in air. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst was stable, reusable, and conveniently recovered by applying an external magnetic field. Moreover, it provided 91% conversion after the sixth catalytic run. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst examined in this study combined both the efficiency of a homogeneous catalyst and the durability of a heterogeneous catalyst. The results revealed that the Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst is promising as a candidate for various Pd-based catalytic applications.
研究领域:
化学
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材料科学
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DOI
高影响因子
JOURNAL OF CHEMICAL RESEARCH
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2019
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IF 0.67
Wanyun Liu,Xiuming Zhou,Ping Huo,Jingbo Li,Guangquan Mei
A green synthesis of variously substituted biphenyl carboxylic acids was achieved through Suzuki–Miyaura cross-coupling of a bromobenzoic acid with an aryl boronic acid using a water-soluble fullerene-supported PdCl2 nanocatalyst (C60-TEGs/PdCl2). Yields of more than 90% were obtained at room temperature in 4 h using 0.05 mol% catalyst and 2 equiv. K2CO3.
研究领域:
有机化学
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催化化学
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环境化学
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DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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2025
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IF 3.6
Yang Zhu,Guisheng Deng
The I2-catalyzed reaction of 1-(2-hydroxyphenyl)-propargyl alcohols with indoles and subsequent treatment with K2CO3 provided (benzofuran-3-yl)-1H-indoles in good to excellent yields with high regioselectivity. This one-pot and two-step strategy proved to be suitable for a wide range of substrates except for aliphatic alkynyl alcohols as well as the indoles bearing N-protected groups such as the Ts group possessing strong electron-withdrawing feature. The reaction procedure involved a cross-coupling and the construction of a benzofuran framework via 5-exo-dig cyclization.
研究领域:
有机化学
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合成化学
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产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
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2025
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IF 4.9
Haoye Tian,Chennan He,Haiping Zhang,Xia Dong,Jinxin He,Jinfang Zhang,Qiangqiang Zhao
Phloxine B (PHB) demonstrates strong catalytic performance in cross-dehydrogenative coupling (CDC) reactions, yet its light-harvesting efficiency remains limited. Dye-supported nanofiber photocatalysts were developed via electrospinning, integrating polyvinyl alcohol (PVA), polydimethyldiallyl ammonium chloride (PDADMAC), and the Förster resonance energy transfer (FRET) pair: AY184 (donor) and PHB (acceptor). Four strategies—electrospinning-adsorption, blending-electrospinning, co-electrospinning from a single nozzle, and co-electrospinning from separate nozzles—were explored to optimize dye distribution and FRET efficiency. Among the synthesized nanofibers, the NF-TZ, co-electrospun from a single nozzle, showed the highest FRET efficiency at 59 %. The blended-electrospinning nanofibers (NF-GH) exhibited exceptional catalytic activity, achieving nearly 90 % conversion of N-phenyltetrahydroisoquinoline (N-phenyl-THIQ) within 4 hours under the visible light (1 W), and the reaction rate constant is 1.8-fold faster than that for fiber with PHB alone. For NF-GH, the conversion of N-phenyl-THIQ retained to 85 % with reused 7 times, demonstrating robust recyclability and photostability. This finding provides new insight into the construction of recyclable FRET-enhanced photocatalysts with broad spectral response and high energy conversion efficiency for organic photochemical reactions.
研究领域:
材料科学
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有机化学
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光催化
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）