Wei Jiang  Yongxin Zhang  Yingpeng Su  Xiazhen Bao  Ying Fu  Congde Huo 《中国化学》2020,38(10):1065-1069

A Cu(OAc)₂/DDQ/DTBP/Py system catalyzed oxidative dehydrogenative silylation‐alkenation tandem reaction of readily available alkyl aromatic compounds with silanes was established. A variety of functionalized alkenyl organosilicon compounds were provided in good to high yields with a total β‐(E) selectivity. The control experiments revealed that the transformation might proceed through a radical pathway.  相似文献   

    

Yangyang Zhou  Zihao Li  Yanbo Liu  Prof. Jia Huo  Chen Chen  Qiling Li  Songyang Niu  Prof. Shuangyin Wang 《ChemSusChem》2020,13(7):1746-1750

Two hydrogenation mechanisms, transfer and catalytic hydrogenation, were combined to achieve higher regulation of hydrogenation chemoselectivity of cinnamyl aldehydes. Transfer hydrogenation with ammonia borane exclusively reduced C=O bonds to get cinnamyl alcohol, and Pt-loaded metal–organic layers efficiently hydrogenated C=C bonds to synthesize phenyl propanol with almost 100 % conversion rate. The hydrogenation could be performed under mild conditions without external high-pressure hydrogen and was applicable to various α,β-unsaturated aldehydes.  相似文献   

    

Prof. Xianwei Li  Wensen Ouyang  Jianhong Nie  Prof. Shaomin Ji  Prof. Qian Chen  Prof. Yanping Huo 《ChemCatChem》2020,12(9):2358-2384

Selective functionalization of ubiquitous C−H bonds of molecules would provide novel retrosynthetic insights and powerful tools for the rapid construction of molecular complexity. In this context, Cp*Ir(III) complexes have exhibited versatile reactivity towards the selective conversion of C−H bonds, with key features that include the use of readily transformable raw materials, great selectivity (chemo-, stereo- and regio-), high efficiency, mild reaction conditions and they enable late-stage modification of complex molecules. Recently, Cp*Ir(III) catalysis has achieved a broad range of reactions such as multiple dehydrogenations and stereoselective C−X bond formations. These advancements are valuable to organometallic chemists and enable the efficient synthesis of functionalized architectures.  相似文献   

    

Dr. Yang Gao  Jianhong Nie  Dr. Yibiao Li  Guilan Liao  Yanping Huo  Dr. Xiao-Qiang Hu 《ChemCatChem》2020,12(10):2721-2725

An efficient Rh(III)-catalyzed Csp²-H amination protocol of benzoic acids with anthranils was developed for the rapid assembly of valuable anthranilic acid derivatives (AAs). The weakly coordinating carboxyl acted as a directing group and was further transformed to an ester group after facilitating the first C−H amination process. This reaction features good functional group tolerance, mild conditions and operational simplicity. The synthetic potential of this methodology was demonstrated by the synthesis of various useful heterocycles and derivatives.  相似文献   

    

Zhizhong Liu  Prof. Xuming Zhang  Dr. Hao Song  Yixuan Yang  Dr. Yang Zheng  Dr. Biao Gao  Prof. Jijiang Fu  Prof. Paul K. Chu  Prof. Kaifu Huo 《ChemCatChem》2020,12(11):2962-2966

Transition metal nitrides with Pt-like chemical properties are important electrocatalysts and tungsten nitride (WN) is a good hydrodenitrogenation and hydrodesulfurization catalyst but its catalytic activity for hydrogen evolution reaction (HER) is poor because of the unfavourable d-band electronic structure resulting in strong interactions with adsorbed hydrogen. Herein, Co doped WN nanowire arrays grown on carbon cloth are reported and the result shows that Co dopants not only act as active sites, but also increase activity of W sites by downshifting the position of d-band centre of W sites as a result of the electron transfer from W to Co. Density-functional theory (DFT) and density of states (DOS) calculations confirm that the enhanced HER performance is attributed to the modulation of the d-band center of W and introduced Co dopants both consequently facilitating the HER process. The results on electronic modulation provide insights into the design of electrocatalysts with high activity.  相似文献   

    

Xianhui Zhang  Renwu Zhou  Rusen Zhou  Maodong Chen  Jiangwei Li  Yue Sun  Qiang Chen  Size Yang  Qing Huo Liu 《Plasma Processes and Polymers》2016,13(4):429-437

  相似文献   

    

Changhong Wang  Zhengyang Liu  Tao Hu  Jingsha Li  Liuqi Dong  Feng Du  Prof. Changming Li  Prof. Chunxian Guo 《ChemSusChem》2021,14(8):1825-1829

It is of significance to design catalysts for achieving high-performance electrochemical nitrate reduction to ammonia (NRA) in mild neutral media. However, the faradaic efficiency and selectivity are still far from satisfactory. Here, the fabrication of an efficient catalyst was achieved by rationally doping Fe to Cu into a metasequoia-like nanocrystal of CuFe for NRA in neutral media. Fe doping was found to deepen energy level of the Cu 3d band, favorably tuning adsorption energies of reaction intermediates to promote the NRA. At an applied potential of −0.7 V vs. the reversible hydrogen electrode, the CuFe with approximately 2 % Fe doping content delivered a catalytic current density of 55.6 mA cm⁻², which was 2.1 times that of the Cu material. The CuFe also exhibited a faradaic efficiency up to 94.5 %, and a good selectivity of 86.8 %.  相似文献   

    

Yineng Zhao  Ni Huo  Sheng Ye  Arman Boromand  Andrew J. Ouderkirk  Wyatt E. Tenhaeff 《Advanced Optical Materials》2021,9(12):2100334

Flexible, compliant permeation barrier layers are critically needed in the optics/optoelectronics industry to protect deformable, polymer-based optical elements, such as those found in variable focus lenses. To address these needs, a transparent and deformable polymeric permeation barrier coating consisting of poly(1H,1H,6H,6H-perfluorohexyl diacrylate) (pPFHDA) is prepared by initiated chemical vapor deposition. pPFHDA is a highly crosslinked fluoropolymer, which is deposited onto temperature-sensitive elastomeric membranes at ambient temperature with high uniformity and conformality. This is believed to be the first demonstration of vapor deposition of the PFHDA monomer. Coatings with thicknesses nominally ranging from 200 to 750 nm are prepared and shown to be impermeable to high-index optical fluid (polyphenyl thioether) over 2 months at 70 °C, which translates to more than 4 year lifespan at room temperature, even after being subjected to 0.26% biaxial strain. Moreover, due to its amorphous nature, the pPFHDA is transparent from wavelengths of 300–1690 nm and also thermally stable to temperatures of 300 °C. These properties should make pPFHDA coating a particularly compelling candidate for flexible optical/optoelectronic devices requiring transparent and compliant barrier layers.  相似文献   

    

Jingxian Xiong  Yiming Sun  Liangwei Wu  Weizhe Wang  Wei Gao  Nengjie Huo  Jingbo Li 《Advanced Optical Materials》2021,9(20):2101017

The ability to detect linearly polarized light is essential in the field of angle-dependent optoelectronics and polarization optical applications. To date, most polarization-sensitive photodetectors are mainly based on single 2D anisotropic materials, which still suffer from the large dark current, from being external bias driven, and from low anisotropy ratio. To address these obstacles, we fabricated a van der Waals (vdW) GeAs/InSe heterojunction with type-II band alignment achieving a high-performance self-driven polarization-sensitive photodetector. The heterojunction exhibits excellent rectifying characteristics with a current rectification ratio exceeding 10³. By operating in photovoltaic mode at zero bias, the device shows a very low dark current of ∼0.1 picoampere, high photoresponsivity of 357 mA/W, and large photo-switching ratio of 10³, yielding a high specific detectivity of 2 × 10¹¹ Jones and photoelectric conversion efficiency (PCE) up to 8%. Benefiting from the anisotropic structure of the GeAs components, the heterojunctions also exhibit self-driven polarization-sensitive photodetection with superior anisotropic photocurrent ratio of ∼18 which surpasses state-of-the-art 2D based polarization-dependent detectors. This work proposes an effective strategy utilizing the anisotropic/isotropic vdW heterojunctions to enable self-powered and high-performance polarization-sensitive photodetectors, opening a new avenue towards the promising potential applications in polarization-resolved electronics and photonics.  相似文献   

    

Haigang Li  JingJing Huo  Dan Sun  Yong Guo  Liang Jiang  Haijuan Zhang  Xiaowei Shi  Zhilong Zhao  Jinchuan Zhou  Chunlan Hu  Chun Zhang 《Electrophoresis》2021,42(6):693-699

Polyethylene glycol-modified canine uricase (PEG-UHC) was prepared by modifying the ε-amino group of lysine residues on the canine uricase (UHC) protein to near-saturation with 5 kDa monomethoxyl-polyethylene glycol succinimide (mPEG-SPA-5k). In order to accurately determine the PEGylation uniformity of PEG-UHC, CZE, 3–8% gradient gel SDS-PAGE, and imaging CIEF (iCIEF) analyses were compared. CZE could not effectively separate PEG-UHC proteins with different degrees of modification, 3–8% gradient gel SDS-PAGE could separate PEG-UHC into seven gel bands; however, most of the gel bands were smeared or blurred, and the separation of PEG-UHC samples by iCIEF was significantly better than that by 3–8% gradient gel SDS-PAGE. Under denatured conditions, iCIEF separated 12 pI peaks, and could also accurately quantify the relative monomer PEG-UHC content. More than 85% of the total monomeric PEG-UHC was conjugated with 7–12 PEG molecules; of this 85%, approximately 40% was conjugated with 9–10 PEG molecules. These results demonstrated that iCIEF exhibits good potential for determining the PEGylation homogeneity of PEGylated protein drugs.  相似文献