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Vietnam Journal of Chemistry · 2023 ·Vol. 61 ·期 2 ·204-209 · IF 0.9

Copper promoted, directed sulfenylation and phenoxylation of benzamide C−H bonds

Nguyen Van Vinh Ha,Nguyen Thi Thu Ha,Ong Ngoc Khanh,Dinh Truc Phuong,Ho Thanh Nhat,Nguyen Thanh Tung

Herein we reported a method for copper pivalate mediated, directed functionalization of ortho C−H bonds in (2-methylthio)aniline benzamides. Diaryl disulfides were used for thiolation, while successful phenoxylation was obtained with phenol as the coupling agent. Our report marks a rare example for flexible transformation of benzamide C(sp 2 )−H bonds into the corresponding unsymmetrical diaryl ethers and thioethers.

研究领域: 有机化学 · 合成化学
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JOURNAL OF ORGANIC CHEMISTRY · 2021 · IF 4.354

Iron-Catalyzed Oxidative Amination of Benzylic C(sp3)–H Bonds with Anilines

Yan-Ling Song,Bei Li,Zhen-Biao Xie,Dan Wang,Hong-Mei Sun

Iron-catalyzed oxidative amination of benzylic C(sp3)–H bonds with anilines bearing electron-withdrawing groups (EWGs) or electron-donating groups (EDGs) is realized based on simple variations of N-substituents on imidazolium cations in novel ionic Fe(III) complexes. The structural modification of the imidazolium cation resulted in regulation of the redox potential and the catalytic performance of the iron metal center. Using DTBP as oxidant, [HItBu][FeBr4] showed the highest catalytic activity for anilines bearing EWGs, while [HIPym][FeBr4] was more efficient for EDG-substituted anilines. This work provides alternative access to benzylamines with the advantages of both a wide substrate scope and iron catalysis.

CAS / MDL: 62-53-3
研究领域: 有机化学 · 催化化学
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ACS Applied Polymer Materials · 2024 · IF 4.4

Aliphatic C–H Insertion Strategies Enhancing Interactions among Waste Rubbers for Recycling

Hao-Jia Guo,Xiaodong Qiao,Ben-Xiang Hu,Shuangquan Liao,Ming-Chao Luo

The recycling of waste rubber (WR) is beneficial to the sustainable development of rubber industries. However, interactions among WR are weak, limiting the recycling of WR. In this work, our group designed bis-diazo compounds to promote interactions among WR for recycling through aliphatic C–H insertion strategies. Specifically, upon hot pressing, bis-diazo compounds produce bis-carbenes which react with C–H on the surface of WR by C–H insertions, and then we obtain recycled WR materials. As a result, stress–strain curves show that the strength of recycled WR increases steadily with the increase of bis-diazo compound loading, which has reached the level of butadiene styrene rubbers. Moreover, the introduced disulfide bonds endow recycled WR with reprocessability. Stress–relaxation experiments at different temperatures show that recycled WR with disulfide bonds have unique vitrimer viscoelastic properties. The feasibility of bis-diazo compounds to enhance interactions among WR through C–H insertions opens opportunities to recycle and reinvent industrial WR.

CAS / MDL: 107-21-1
研究领域: 材料科学 · 化学工程 · 回收技术
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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Electronic perturbation-promoted interfacial pathway for facile C–H dissociation

Zhe Wang,Chunpeng Wang,Bing Lu,Zhirong Chen,Yong Wang,Shanjun Mao

Interface has often played significant role in the behavior of metal-based catalysts during various heterogeneous reactions. Herein, we reported a novel interfacial pathway for propane dehydrogenation on Pt-GaO x dual sites. The active ensemble, composing Pt particles and Ga 2 O 3 clusters, facilitates the facile dissociation of C–H bonds (energy barrier < 0.30 eV) through H-abstraction by O sites, coupled with alkyl stabilization on the Pt surface. Notably, the electronic perturbation of the Pt slab induces higher-lying O 2 p states at the interface, accompanied by a substantial density of states around fermi level. This is in stark contrast to the O species present in Ga 2 O 3 crystals or clusters alone, leading to an exceptionally strong affinity for H and a robust ability for C–H scission. The Pt/Ga-Al 2 O 3 catalysts prepared with Pt nanoparticles decorated by Ga oxide exhibit superior performance compared to Pt/Al 2 O 3 and PtSn/Al 2 O 3 catalysts. This insight into interfacial catalysis contributes to a broader understanding of the origin of the high catalytic efficiency observed in metal-based catalysts.

研究领域: 催化化学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

NiOx(H) locked Au clusters against CO-induced aggregation for robust water-gas shift catalysis

Hui Zhao,Xin-Pu Fu,Wei-Wei Wang,Jin-Cheng Liu,Chun-Jiang Jia

Despite the supported Au demonstrating superior activity in catalyzing various reactions, their stubborn and widespread deactivation issue has long remained unsolved. Therefore, the challenge in current investigations of Au-based catalysts could be divided into two aspects: uncovering the authentic molecular induction for the deactivated evolution and fabricating interfacial structures combining efficiency and stability. In this work, by incorporating NiO x (H) adjacent to small active Au 1 /Au n species, the as-formed 0.5Au-5NiO x (H)/CeO 2 catalyst simultaneously achieved high reactivity ( r  = 5.23 mmol CO ·g Au −1 ·s −1 ) toward the water-gas shift (WGS) reaction and remarkable long-term stability with time-on-stream of 100 h at 250 °C, significantly surpassing the reference Au/CeO 2 counterpart as well as the other oxides-supported Au catalysts reported previously. Comprehensive in-situ characterizations and DFT calculations revealed that the CO molecules, rather than H 2 , H 2 O, or CO 2 molecules, are the dominant molecular driver for Au aggregation, correspondingly inducing the degraded catalytic efficiency. Specifically, on the one hand, the strong CO−Au coordination degraded the ejection barrier of Au atoms from Au-Au coordination; on the other hand, the −OH groups as intermediates from H 2 O dissociation, participating in the stabilization of Au species upon the surface, were dynamically consumed by CO molecules. For these regards, the adjacent Ni adatoms promote the sufficient generation of stable −OH groups for stabilizing Au atoms under WGS reaction. As a result, the corresponding Au−Au ejection and Au−O diffusion barriers of as-formed Au n −O(H)−Ni/CeO 2 combinations are significantly enlarged, which thereby boosts the structural stability in the CO-containing atmospheres.

研究领域: 催化化学 · 材料化学 · 表面科学 · 物理化学 · 能源化学
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2022 · IF 6.364

Densification mechanism and corrosion resistance of h-BN/ZrO2 ceramics prepared by spark plasma sintering

Mao chen,Fan Zhang,Hailong Wang,Gang Shao,Bingbing Fan,Rui Zhang,Hongxia Li,Yongqiang Chen

The dense h-BN/ZrO 2 (30 wt%) composites without additives were rapidly fabricated by spark plasma sintering . The relative density, apparent porosity, fracture toughness, flexural strength , phase composition and microstructure of h-BN/ZrO 2 composites were systematically investigated. Besides, the corrosion resistance of h-BN/ZrO 2 composites in molten steel was also studied in detail. Especially, the h-BN/ZrO 2 composites were sintered at 1800 °C exhibiting a relative density of 96.6% and the flexural strength of ≈ 157 MPa. The corrosion of h-BN/ZrO 2 composites was mainly due to the oxidative decomposition of BN, and the corrosion process was clarified by a parabolic law. The excellent corrosion resistance of the h-BN/ZrO 2 composites was attributed to ZrO 2 residual layer formed at the interface. The corrosion thickness of h-BN/ZrO 2 composites was only ∼116 µm even using the longest corrosion time (80 min). The composites could be a promising candidate material applied to fabricated thin strip continuous casting side sealing plates.

CAS / MDL: 10043-11-5 1314-23-4
研究领域: 材料科学 · 陶瓷工程
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Science of Advanced Materials · 2014 ·Vol. 6 ·期 9 ·1936-1942 · IF 2.908

A Fluorescence Assay for HIV-1 Ribonuclease H Activity and Inhibition Detection Using Graphene Oxide as Sensing Platform

Li Xiang,Ding Xuelian,Wang Gongke,Zhou Yixuan,Hou Ruipeng,Gao Shuyan,Lu Yan

In this work, we have developed a simple and highly sensitive fluorescent biosensor for the detection of HIV-1 RNase H activity and inhibition by using graphene oxide (GO) as sensing platform. In our approach, a DNA-RNA substrate was prepared which a carboxy fluorescein (FAM) was labeled at the 3 termini of single strand DNA. The FAM labeled DNA-RNA substrate preserves most of the fluorescence when mixed with GO. However, in the present of RNase H, RNase H can cleavage the RNA into fragments, resulting in the dissociation of ssDNA and mononucleotides. The fluorescence intensity was greatly quenched after the addition of GO. Because of the super quenching ability of GO, the as-proposed method provides a wide linear range from 1.0 to 26.3 units mL–1 and a low detection limit of 0.6 units mL–1 for HIV-1 RNase H activity analysis. Additionally, this approach shows potential for high-throughput screening of HIV-1 RNase H inhibitors. The method not only provides a universal platform for monitoring activity and inhibition of RNase H but also shows great potential in biological process researches, drug discovery, and clinic diagnostics.

研究领域: 生物技术 · 分子生物学 · 纳米技术 · 病毒学 · 药物发现
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Highly thermally conductive Ti3C2Tx/h-BN hybrid films via coulombic assembly for electromagnetic interference shielding

Kunpeng Qian,Qianfan Zhou,Sineenat Thaiboonrod,Jianhui Fang,Miao Miao,Hongmin Wu,Shaomei Cao,Xin Feng

With the development of electronic equipment, heat problem and electromagnetic pollution severely affect both their functions and human health, which leads to great interests in developing materials synchronously with outstanding thermal conductivity and electromagnetic interference (EMI) shielding performance. Here, ultrathin Ti 3 C 2 T x /h-BN two-dimensional (2D) heterostructure films were prepared via coulombic assembly between Ti 3 C 2 T x MXene and h-BN nanosheet through ultrasonic blending. After the addition of h-BN nanosheet as thermal conductive nanofillers, the hybrid films achieved a higher value of thermal conductivity, compared to Ti 3 C 2 T x composite film without h-BN. The higher thermal conductivity offered by h-BN enables the Ti 3 C 2 T x /h-BN films have good potential for EMI shielding applications on wearable and portable electronic devices. When the mass ratio of Ti 3 C 2 T x /h-BN is 7:3, the hybrid film with the thickness of 47.60 µm exhibited electrical conductivity of 57.67 S/cm and the maximum EMI shielding effectiveness of 37.29 dB.

研究领域: 材料科学 · 电子工程
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IEEE TRANSACTIONS ON INSTRUMENTATION AND MEASUREMENT · 2024 · IF 5.6

Lu2O3/h-BN Modified U-Shaped Fiber Optic SPR Sensor With Improved Sensitivity

Qi Wang,Hao-Yue Wang,Nuerguli Kari

Rapid and incredibly sensitive analyte detection is crucial in a variety of settings, including medical diagnostics. However, conventional surface plasmon resonance (SPR) sensors cannot effectively solve the issue of low sensitivity when assaying trace analytes. In this work, the rare Earth oxide Lu2O3 is first introduced to modify fiber optic SPR sensor. By utilizing the inherent advantages of Lu2O3, including high dielectric constant, high breakdown field strength, and high photoelectric conversion efficiency, the electric field around the sensor is effectively increased and high sensitivity detection is achieved. Experimental results show sensitivity of the sensor modified with Lu2O3 nanomaterial reaches 12133.78 nm/RIU in the interval of 1.3614–1.3756. The hexagonal boron nitride (h-BN) is subsequently introduced to further enhance electric field using the charge transfer mechanism. The sensitivity reaches 15065.92 nm/RIU, 3.96 times better than conventional U-shaped fiber SPR sensors. The sensor is compact designed with high sensitivity. There is significant potential for improving the sensitivity aspect of analyte detection.

研究领域: 生物医学工程 · 光学传感 · 材料科学
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MRS Communications · 2023 ·Vol. 13 ·期 2 ·268-275 · IF 1.9

Micro-mechanical properties of C–S–H modified by various carbon nanotubes and the correlation with the nano/micro-structures

Qiao Xinfeng,Hu Chuanlin,Yao Shun,Wang Fazhou

This study is to explore the micro-mechanical properties of C–S–H modified by various carbon nanotubes and the correlation with the nano/micro-structures. The results show that carboxyl-functionalized single-walled carbon nanotubes provide the great template for the growth of C–S–H and reduce the porosity and surface defects of C–S–H particles. The highly ordered and dense layered structure of C–S–H greatly improves its micro-mechanical properties. In addition, the functional groups (–COOH) of functionalized carbon nanotubes can combine with the Ca–O bond of C–S–H to change the interlayer spacing of C–S–H, and the effects are particularly significant at low Ca/Si. Graphical abstract

CAS / MDL: 308068-56-6 9004-32-4
研究领域: 材料科学 · 纳米技术
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SYNTHETIC COMMUNICATIONS · 2018 · IF 1.377

Pd-catalyzed regioselective C-H chlorination of disubstituted 1,2,3-triazoles

Xinyuan Ma,Qiong Mo,Jie Chang,Kai Xie

This paper mainly studied Pd-catalyzed regioselective chlorination of disubstituted 1,2,3-triazoles directed by the 1,2,3-triazole ring. A series of regioselective chlorinated products were synthesized in 47–86% yields using Pd(OAc)2 as a catalyst and CuCl2 as a chlorinated reagent. This method provides a new mean for the synthesis of 1,2,3-triazole halides which combines the formation of C-X bond with C-H activation.

研究领域: 有机化学 · 合成化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Selective Photooxidation of Benzyl Alcohol to Benzaldehyde via H-Abstraction by Bi2.15WO6 under Alkaline Conditions

Wen-Shuang Zhu,Dai Sun,Ling-Li Yu,Shao-Qi Zhi,Yu-Dong Shan,Yi-Fang Lu,Hai-Tao Ren,Song-Hai Wu,Yong Liu,Xu Han

In this study, Bi2.15WO6 with different morphologies was successfully synthesized and used for the selective photooxidation of benzyl alcohol to benzaldehyde in aqueous solutions. High conversion (85%) and selectivity (85%) can be simultaneously achieved under alkaline conditions by adding ethylenediamine to protect the produced benzaldehyde from overoxidation. In the oxidation process, ≡Bi–OO• and ≡Bi–OOH on Bi2.15WO6, instead of OH• and O2•–, are the primary oxidizing species to sequentially abstract two H (H+ + e–) from benzyl alcohol, accompanied by the formation of H2O2. Meanwhile, h+ and OH– also minorly contribute to the selective oxidation of benzyl alcohol via the H-abstraction pathway. This study enriches our understanding of the oxidizing species involved in the selective photooxidation of benzyl alcohol to benzaldehyde.

研究领域: 材料科学 · 催化化学 · 环境科学
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