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Access to High-Molecular-Weight Polyethylenes through High Temperature Ethylene Polymerization Catalysed by Ethylene-Bridged ansa-(3-R-Cyclopentadienyl)(Fluorenyl) Zirconocene Complexes

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Chinese Journal of Polymer Science 2024年第1期42卷 42-51,I0007页

作者： Bo Li Haiyan Ma Jiling Huang Shanghai Key laboratory of Functional Materials chemistry and laboratory of Organometallic chemistry School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

A series of C1-symmetric ethylene-bridged ansa-(3-R-cyclopentadienyl)(fluorenyl) metallocene complexes(Zr: 1-5;Hf: 6) have been synthesized, characterized and investigated as catalyst precursors for the high temperature ethylene polymerization. Using methylaluminoxane(MAO) as the cocatalyst, zirconium complexes 1-5 bearing a bulky substituent on the 3-position of the cyclopendienyl ring showed high catalytic activities up to 1.48×10^(7) g PE·mol_(Zr)^(-1)·h^(-1) toward the polymerization of ethylene and afforded polyethylenes with high molecular weights(1.49×10^(5)-6.31×10^(5) g/mol), meanwhile exhibting great thermal stability at high temperatures up to 120 ℃ together with a long catalytic life time up to 2 h. By adopting low Al/Zr ratios, such as 125, polyethylenes with ultra high molecular weights up to 2.86×106 g/mol were obtained. It is worthy of noting that zirconium complexes 1-4 bearing a substituent with an aryl pendant showed temperature-dependent activities, which increased rapidly with the increase of polymerization temperature, thus weak interaction of the pendent aryl group with the cationic active center is proposed to account for the very low activities displayed at low temperatures. In contrast to zirconocene complexes 1-5, hafnocene complex 6 only displayed very low catalytic activities toward the polymerization of ethylene and afforded polyethylenes with molecular weights ten times smaller than those obtained by zirconocene complexes 1-5. Zirconocene complexes 1-5 were also able to catalyse the polymerization of propylene at high temperatures, but only afforded waxes with low molecular weights.

关键词： ansa-Metallocene Ethylene Propylene Polymerization High temperature

Third-order nonlinear wavelength conversion in chalcogenide glass waveguides towards mid-infrared photonics

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Chinese Physics B 2024年第10期33卷 269-274页

作者： Fengbo Han Jiaxin Gu Lu Huang Hang Wang Yali Huang Xuecheng Zhou Shaoliang Yu Zhengqian Luo Zhipeng Dong Qingyang Du Fujian Key laboratory of Ultrafast laser Technology and Applications Xiamen UniversityXiamen 361005China Zhejiang laboratory Hangzhou 311100China

The increasing demand in spectroscopy and sensing calls for infrared(mid-IR)light ***,we theoretically investigate nonlinear wavelength conversion of Ge_(28)Sb_(12)Se_(60)chalcogenide glass waveguide in the mid-IR spectral *** waveguide dispersion engineering,we predict generation of over an octave wavelength(2.8μm-5.9μm)tuning range Raman soliton self-frequency shift,over 2.5 octaves wavelength cover range supercontinuum(1.2μm-8.0μm),as well as single soliton Kerr comb generated in suspended Ge_(28)Sb_(12)Se_(60)*** findings evidenced that Ge_(28)Sb_(12)Se_(60)chalcogenide glass waveguides can simultaneously satisfy the generation of Raman soliton self-frequency shift,supercontinuum spectrum,and Kerr frequency comb generation through dispersion engineering towards mid-IR on chip.

关键词： chalcogenide glass Raman soliton self-frequency shift supercontinuum soliton Kerr comb

Recent progress on the functionalization of white phosphorus in China

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National Science Review 2024年第06期11卷 308-320页

作者： Xinlei Huangfu Zhongzhen Wang Yu Chen Junnian Wei Wei Liu Wen-Xiong Zhang Beijing National laboratory for Molecular Sciences(BNLMS) State Key Laboratory of Rare-Earth Materials Chemistry and Applications & Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular Engineering Peking University

Direct synthesis of organophosphorus compounds from white phosphorus represents a significant but challenging subject, especially in the context of ongoing efforts to comprehensively improve the phosphorus-derived chemical industry driven by sustainability and safety concerns. China is the world's largest producer of white phosphorus, creating a significant demand for the green transformation of this crucial feedstock. This review provides an overview of advancements in white phosphorus activation by Chinese research teams, focusing on the direct construction of P–C/N/O/S/M bonds from white phosphorus. Additionally, we offer some insights into prospective directions for the activation and transformation of white phosphorus in the future. This review paper aims to attract more researchers to engage in this area, stimulating follow-up exploration and fostering enduring advances.

关键词： white phosphorus organophosphorus compound activation selectivity efficiency

Electric-field-controlled highly regioselective thiocyanation of N-containing heterocycles

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Science China chemistry 2024年第4期67卷 1263-1269页

作者： Ming Gong Qian Wu Jung Keun Kim Mengmeng Huang Yabo Li Yangjie Wu Jong Seung Kim Henan Key laboratory of Chemical Biology and Organic chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesCollege of ChemistryZhengzhou UniversityZhengzhou 450052China Department of chemistry Korea UniversitySeoul 02841Korea

Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting *** electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional ***,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their *** this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)*** approach led to moderate to good yields of the corresponding C7-thiocyanation *** calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction ***,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE *** work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.

关键词： electric fields reaction-axis rule electric double layer C7-thiocyanation C-S bond formation

Performance enhancement and active sites identification of Cu-Cd bimetallic oxide derived catalysts for electrochemical CO_(2) reduction

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Journal of Energy chemistry 2024年第4期91卷 50-58页

作者： Cai Wang Xin Hu Bairong Chen Houan Ren Xiaoyu Wang Yilin Zhang Xinyu Chen Yuping Liu Qingxin Guan Wei Li State Key laboratory of Elemento-Organic chemistry Key Laboratory of Adv.Energy Mater.Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China

The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great ***-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of ***,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 ***,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such *** results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.

关键词： CO_(2)reduction Cu-Cd bimetallic Real active sites CO production

Highly sensitive CO_(2)-LITES sensor based on a self-designed low-frequency quartz tuning fork and fiber-coupled MPC

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Chinese Optics Letters 2024年第7期22卷 105-110页

作者： Jinfeng Hou Xiaonan Liu Yahui Liu Ying He Weijiang Zhao Yufei Ma National Key laboratory of Science and Technology on Tunable laser Harbin Institute of TechnologyHarbin 150001China

A highly sensitive carbon dioxide(CO_(2))sensor based on light-induced thermoelastic spectroscopy(LITES)utilizing a selfdesigned low-frequency quartz tuning fork(QTF)and a fiber-coupled multipass cell(MPC)is reported in this *** QTF with a low resonant frequency of 8675 Hz and a high Q factor of 11,675.64 was used to improve its energy accumulation time and the sensor’s signal *** MPC with the fiber-coupled structure and optical length of 40 m was adopted to significantly increase the gas absorbance and reduce the optical alignment difficulty as well as improve the robustness of the sensor system.A distributed feedback(DFB),near-infrared diode laser with an emission wavelength of 1.57μm was used as an excitation *** experimental results showed that this CO_(2)-LITES sensor had an excellent linear response to CO_(2) *** minimum detection limitation(MDL)of this CO_(2)-LITES sensor was obtained to be 445.91 ppm,and it could be improved to 47.70 ppm(parts per million)when the integration time of the system reached 500 *** improvement methods for the detection performance of such sensors were also discussed.

关键词： carbon dioxide quartz tuning fork multipass cell light-induced thermoelastic spectroscopy

Impact of Pd single-site coordination structure on catalytic performance for semihydrogenation of acetylene

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Nano Research 2024年第9期17卷 8243-8249页

作者： Yu Zeng Minqi Xia Fujie Gao Changkai Zhou Xueyi Cheng Liwei Liu Liu Jiao Qiang Wu Xizhang Wang Lijun Yang Yining Fan Zheng Hu Key laboratory of Mesoscopic chemistry of MOE and Jiangsu Provincial laboratory for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Semihydrogenation of trace acetylene in an ethylene gas stream is a vital step for the industrial production of polyethylene,in which Pd single-site catalysts(SSCs)have great ***,two Pd SSCs with different coordination structures are prepared on hierarchical nitrogen-doped carbon nanocages(hNCNC)by regulating the nitrogen species with or without using *** using dicyandiamide,the obtained Pd1-Ndicy/hNCNC SSC features the coordinated Pd by two pyridinic N and two pyrrolic N(PdN^(py)_(2)N^(pr)_(2)).Without using dicyandiamide,the obtained Pd1/hNCNC SSC features the coordinated Pd by pyridinic N and C(PdN^(py_(x)C_(4-x)),x=1-4).The former exhibits an 18-fold increase in catalytic activity compared to the *** results reveal the abundant unoccupied orbital states above the Fermi level of moiety,which can facilitate the activation of substrate molecules and dynamics of acetylene hydrogenation as supported by the combined theoretical and experimental *** addition,PdN^(py)_(2)N^(pr)_(2)the moiety presents a favorable desorption of ***,the Pd1-Ndicy/hNCNC SSC exhibits high C2H2 conversion(99%)and C2H4 selectivity(87%)at 160℃.This study demonstrates the impact of Pd single-site coordination structure on catalytic performance,which is significant for the rational design of advanced Pd SSCs on carbon-based supports.

关键词： coordination structure hierarchical nitrogen-doped carbon nanocages palladium semihydrogenation of acetylene singlesite catalysts

Chiral multiple-resonance thermally activated delayed fluorescence materials based on chiral spiro-axis skeleton for efficient circularly polarized electroluminescence

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Science China chemistry 2024年第7期67卷 2257-2264页

作者： Shi-Quan Song Xiao Han Zhong-Zhong Huo Ching-Fai Yip Xian-Fang Hong Meng-Ning Ding You-Xuan Zheng State Key laboratory of Coordination chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Key laboratory of Mesoscopic chemistry of Ministry of Education School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chiral luminescence materials have potential applications in the field of three-dimensional displays due to their circularly polarized luminescence(CPL)***,the further development of circularly polarized organic light-emitting diodes(CP-OLEDs)needs to meet the requirements of high efficiency,high color purity,low cost,and high dissymmetry factor(gPLor gEL),chiral multiple resonance thermally activated delayed fluorescence(MR-TADF)materials are considered as candidates in these ***,based on a pair of chiral spirofluorene precursors,two pairs of high-performance chiral MR-TADF emitters((R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB)are developed,which exhibit strong emissions peaking at 491 and 502 nm in toluene with full-width at half-maximum values of 25 and 33 nm,*** addition,small singlet–triplet energy gaps of 0.15 and 0.10 eV with high absolute photoluminescence efficiencies of 95.0%and 96.7%are observed for p-Spiro-DtBuCzB and m-Spiro-DtBuCzB molecules,*** based on p-Spiro-DtBuCzB and m-Spiro-DtBuCzB display high maximum external quantum efficiencies of 29.6%and 33.8%,*** importantly,CP-OLEDs present symmetric circularly polarized electroluminescence spectra with|gEL|factors of 3.36×10^(-4)and 7.66×10^(-4)for devices based on(R/S)-p-Spiro-DtBuCzB and(R/S)-m-Spiro-DtBuCzB enantiomers,respectively.

关键词： chiral spiro-axis skeleton-based material multiple resonance thermally activated delayed fluorescence circularly polarized electroluminescence dissymmetry factor external quantum efficiency

Structure regulating of metal clusters in carbonized metallic organic frameworks for high-efficient microwave absorption via tuning interaction strength between metals and ligands

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Nano Research 2024年第3期17卷 1699-1709页

作者： Chang Sun Kun-Yan Zhao Ming-Lu Huang Cheng-Long Luo Xu-Dong Chen Ming Wang School of chemistry and Chemical Engineering Chongqing Key Laboratory of Soft-Matter Material Chemistry and Function ManufacturingSouthwest UniversityChongqing 400715China Jieyang Branch of chemistry and Chemical Engineering Guangdong laboratory(Rongjiang laboratory) Jieyang 515200China

Carbonized metallic organic frameworks(CMOF)have been attracting attention in microwave absorption(MA)research area because of their diverse structures,tunable compositions,and rich ***,structure regulation on metal clusters in CMOF is achieved by tuning the interaction strength between metals and ligands to enhance microwave absorption *** to relatively weak interaction among copper cations and ligands,copper nanoclusters(CuNC)can be uniformly formed and embedded within the cobalt/zinc(Co/Zn)***,copper cations are added to the Co/Zn bimetallic zeolitic imidazolate frameworks(ZIFs).Secondly,the CMOF composite particles with CuNCs(CuNCs/CoZn-CMOF)were developed by a pyrolysis *** CuNCs/CoZn-CMOF with an appropriate amount of CuNCs can harmonize both dielectric and magnetic *** a result,the minimum reflection loss(RLmin)reaches–45.1 dB at a matching thickness of 2.30 mm and the effective absorption bandwidth(EAB)is 8.80 GHz at a thickness of 3.10 *** broadband response to electromagnetic waves is attributed to interfacial polarization at CuNCs surface and heterogeneous interfaces,impedance matching and multiple scattering of electromagnetic *** study provides a feasible method to develop CMOF microwave absorption materials with high EAB values.

关键词： heterogeneous interface carbonized metallic organic frameworks microwave absorption interfacial polarization