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Enhancing alkyne semi-hydrogenation through engineering metal-support interactions of Pd on oxides

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Nano Research 2024年第5期17卷 3707-3713页

作者： Yuefeng Wu Xiaotong lu Pengfei Cui Wenyu Jia Jun Zhou Yuan Wang Hussain Zahid Yuxin Wu Muhammad Umer Rafique Xiong Yin Baoshan Li Leyu Wang Guolei Xiang State Key Laboratory of chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

Supported Pd catalysts show superior activities for olefin productions from alkynes through semi-hydrogenation reactions,but over-hydrogenation into alkanes highly decreases olefin *** phenylacetylene semi-hydrogenation as a model reaction,here we explore the optimization approaches toward better Pd catalysts for alkyne semi-hydrogenation through investigating support effect and metal-support *** results show that the states of Pd with supports can be tuned by varying oxide reducibility,loading ratios,and *** our system,0.06 wt.%Pd on rutile-TiO_(2) nanorods shows the highest activity owing to the synergistic effects of single-atoms and *** reducibility can change the filling degrees of Pd 4d orbitals through varying interfacial bonding strengths,which further affect catalytic activity and selectivity.

关键词： alkyne semi-hydrogenation support effect metal-support interaction Pd catalyst single-atom catalyst

Tuning the product selectivity of dimethyl oxalate hydrogenation over WO_(x) modified Cu/SiO_(2) catalysts

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Journal of Energy Chemistry 2024年第10期97卷 128-138,I0004页

作者： Zheng Li Zhuo Ma Yihui Li Ziang Zhao Yuan Tan Ziyin Liu Xingkun Chen Nian Lei Huigang Wang Wei lu Hejun Zhu Yunjie Ding Hangzhou institute of Advanced Studies Zhejiang Normal UniversityHangzhou 311231ZhejiangChina dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Shaanxi Key Laboratory of Clean Energy Technology Utilization Yulin BranchDalian National Laboratory For Clean EnergyCASYulin 719199ShaanxiChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Product selectivity and reaction pathway are highly dependent on surface structure of heterogeneous *** vapor-phase hydrogenation of dimethyl oxalate(DMO),"EG route"(DMO→methyl glycolate(MG)ethylene glycol(EG)→ethanol(ET))and"MA route"(DMO→MG→methyl acetate(MA))were proposed over traditional Cu based catalysts and Mo-based or Fe-based catalysts,***,tunable yield of ET(93.7%)and MA(72.1%)were obtained through different reaction routes over WO_(x) modified Cu/SiO_(2) catalysts,and the corresponding reaction route was further proved by kinetic study and in-situ DRIFTS *** studies demonstrated that H_(2) activation ability,acid density and Cu-WO_(x) interaction on the catalysts were tuned by regulating the surface W density,which resulted in the different reaction pathway and product ***'s more,high yield of MA produced from DMO hydrogenation was firstly reported with the H_(2) pressure as low as 0.5 MPa.

关键词： Ethanol Dimethyl oxalate Selective hydrogenation Methyl acetate WCu/SiO_(2)catalyst

Unleashing the Power of Bio-based Thermotropic Liquid Crystal Modifiers:Toughening and Reinforcing Petroleum-based Epoxy Resin without Compromising Other Properties

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Chinese Journal of Polymer Science 2024年第8期42卷 1093-1102页

作者： Qing-Yun lu Hong-Wei Gu Jia-Hui Li Qian-Qian Fan Bei-Tao Liu Yan Kou Xi-Gao Jian Zhi-Huan Weng State Key Laboratory of Fine chemicals Frontiers Science Center for Smart MaterialsLiaoning Technology Innovation Center of High Performance Resin MaterialsDepartment of Polymer Science&EngineeringDalian University of TechnologyDalian 116024China Thermochemistry Laboratory Liaoning Province Key Laboratory of Thermochemistry for Energy and MaterialsDalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Toughening the petroleum-based epoxy resin blends with bio-based modifiers without compromising their modulus,mechanical strength,and other properties is still a big challenge in view of the *** this study,a bio-based liquid crystal epoxy resin(THMT-E P)with an s-triazine ring structure was utilized to modify a petroleum-based bisphenol A epoxy resin(E51)with 4,4'-diaminodiphenylsulfone(DDS)as a curing agent,and the blended systems were evaluated for their thermal stability,mechanical properties,and flame *** results showed that the impact strength of the blended system initially increased and then decreased with the increase in THMT-EP content,and it reached the a maximum value of 26.5 kJ/m^(2)when the THMT-EP content was 5%,which was 31.2%higher than that of E51/***,the flexural strength,modulus,and glass transition tem perature of the blended system were all simultaneously improved with the addition of *** the same time,the addition of THMT-EP enhanced the flame retardancy of the system by increasing the char yield at 700℃and decreasing the peak heat release rate and total heat release *** work paves the way for a more sustainable improvement in the comprehensive performance of epoxy resin.

关键词： Epoxy resin Toughening Bio-based Thermotropic liquid crystal

Highly stable side-chain-type cardo poly(aryl ether ketone)s membranes for vanadium flow battery

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Chinese chemical Letters 2024年第3期35卷 167-170页

作者： Ziming Zhao Qing Dai Sihan Huang Wenjing lu Yaohan Chen Jifu Zheng Suobo Zhang Shenghai Li Xianfeng Li Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Vanadium flow batteries(VFBs)have drawn considerable attention as an emerging technology for largescale energy storage systems(ESSs).One of the pivotal challenges is the availability of eligible ion exchange membranes(ICMs)that provide high ion selectivity,proton conductivity,and stability under rigorous ***,a‘side-chain-type’strategy has been employed to fabricate highly stable phenolphthalein-based cardo poly(arylene ether ketone)s(PAEKs)membrane with low area resistance(0.058Ωcm^(2)),in which flexible alkyl spacers effectively alleviated inductive withdrawing effect from terminal ion exchange groups thus enabling a stable *** assembled VFBs based on PAEKs bearing pendent alkyl chain terminated with quaternary ammonium(Q-PPhEK)demonstrated an energy efficiency above 80%over 700 cycles at 160 mA/cm^(2).Such a remarkable results revealed that the side-chain-type strategy contributed to enhancing the ICMs stability in strong oxidizing environment,meanwhile,more interesting backbones would be woken with this design engaging in stable ICMs for VFBs.

关键词： Vanadium flow battery Energy storage technology Ion exchange membrane Ion transport mechanism Poly(arylene ether ketone)s(PAEKs)

A review of ultra-high temperature heat-resistant energetic materials

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Defence Technology（防务技术） 2024年第8期38卷 33-57页

作者： Rongzheng Zhang Yuangang Xu Feng Yang Pengcheng Wang Qiuhan Lin Hui Huang Ming lu School of Chemistry and chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China institute of chemical Materials China Academy of Engineering PhysicsMianyang 621900China

Heat-resistant energetic materials refer to a type of energetic materials that possess a high melting point,high stability and operational safety. By studying the structures of these energetic materials has showed that the thermal stability can be enhanced by introducing amino groups to form intra/inter-molecular hydrogen bonds, constructing conjugate systems and designing symmetrical structures. This article aims to review the physical and chemical properties of ultra-high temperature heat-resistant energetic compounds and provide valuable theoretical insights for the preparation of ultra-high temperature heatresistant energetic materials. We also analyze the selected 20 heat-resistant energetic materials with decomposition temperatures higher than 350℃, serving as templates for the synthesis of various highperformance heat-resistant energetic materials.

关键词： Heat-resistant energetic materials Organic synthesis Conjugated Hydrogen bond Symmetrical structure Stabilization

Multidimensional hollow SiO_(2)/C nanofibers modified by magnetic nanocrystals for electromagnetic energy conversion and lithium battery storage

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Nano Research 2024年第8期17卷 7301-7314页

作者： Chen Han Qi Zheng Juncheng Jin Jiajia Zhang Wen-Qiang Cao Kun Xiang Min Zhang Mao-Sheng Cao Anhui Provincial Laboratory of Biomimetic Sensor and Detecting Technology College of Materials and Chemical EngineeringWest Anhui UniversityLu’an 237012China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081China Department of physics Beijing Technology and Business UniversityBeijing 100048China

Multifunctional materials are powerful tools to support the advancement of energy conversion *** with prominent electromagnetic and electrochemical properties can realize the conversion of electromagnetic energy and solve the subsequent storage ***,an electrospinning-thermal reduction method is employed to construct ultrafine nickel nanoparticle modified porous SiO_(2)/C(Ni-SiO_(2)/C)hollow nanofibers as promising materials for applications in both electromagnetic wave absorption(EMA)and lithium-ion ***,when used as an EMA material,the reflection loss(RL)of Ni-SiO_(2)/C can reach−47.8 dB at 15.8 GHz with a matching thickness of 2.2 *** excellent microwave absorption performance can be attributed to the enhanced conduction loss,polarization relaxation,synergistic magnetic loss,and preferred impedance matching,which result from multi-component magnetic/dielectric synergy and the unique interconnected multidimensional hollow ***,the electronic conductivity and electrochemical activity of the samples are significantly enhanced due to the uniform distribution of ultrafine Ni nanoparticles in the amorphous SiO_(2)/C ***,the hierarchical hollow porous structure provides sufficient free space for volume change during lithiation/delithiation ***,the Ni-SiO_(2)/C nanocomposite exhibits a high reversible capacity of 917.6 mAh·g^(−1)at 0.1 A·g^(−1).At a high current density of 2 A·g^(−1),a capacity of 563.9 mAh·g^(−1)can be maintained after 300 *** energy conversion-storage device is designed to store waste electromagnetic energy in the form of useful electrical *** work inspires the development of high-performance bifunctional materials.

关键词： Ni-SiO_(2)/C nanofiber electromagnetic absorption lithium-ion storage electrospinning multidimensional structure

Interlayer Magnetic Interaction in the CrI_(3)/CrSe_(2) Heterostructure

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Chinese physics Letters 2024年第5期41卷 85-89页

作者：王秋皓倪美燕李淑静郑法伟路洪艳张平 School of physics and Physical Engineering Qufu Normal UniversityQufu 273165China Center for Quantum physics Key Laboratory of Advanced Optoelectronic Quantum Architecture and MeasurementSchool of PhysicsBeijing Institute of TechnologyBeijing 100081China Beijing Key Lab of Nanophotonics and Ultrafine Optoelectronic Systems School of PhysicsBeijing Institute of TechnologyBeijing 100081China College of Mathematics and physics Beijing University of Chemical TechnologyBeijing 100029China institute of Applied physics and Computational Mathematics Beijing 100088China

Based on first-principles calculations, we systematically study the stacking energy and interlayer magnetic interaction of the heterobilayer composed of CrI_(3) and CrSe_(2) monolayers. It is found that the stacking order plays a crucial role in the interlayer magnetic coupling. Among all possible stacking structures, the AA-stacking is the most stable heterostructure, exhibiting interlayer antiferromagnetic interactions. Interestingly, the interlayer magnetic interaction can be effectively tuned by biaxial strain. A 4.3% compressive strain would result in a ferromagnetic interlayer interaction in all stacking orders. These results reveal the magnetic properties of CrI_(3)/CrSe_(2) heterostructure, which is expected to be applied to spintronic devices.

关键词： strain stacking interlayer

Atomically Precise Design of PtSn Catalyst for the Understanding of the Role of Sn in Propane Dehydrogenation

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Precision Chemistry 2024年第6期2卷 245-255页

作者： Hui Ye Lina Cao Minghui Gu Han Nie Qingqing Gu Bing Yang Yunxing Bai Qinxue Nie Weixin Huang Junling lu institute of Advanced Technology Key Laboratory of Precision and Intelligent ChemistryDepartment of Chemical PhysicsHefei National Research Center for Physical Sciences at the MicroscaleKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesUniversity of Science and Technology of ChinaHefei 230026P.R.China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsThe Chinese Academy of SciencesDalian 116023P.R.China

Propane dehydrogenation(PDH),an atom-economic reaction to produce high-value-added propylene and hydrogen with high efficiency,has recently attracted extensive *** severe deactivation of Pt-based catalysts through sintering and coking remains a major challenge in this high-temperature *** introduction of Sn as a promoter has been widely applied to improve the stability and selectivity of the ***,the selectivity and stability of PtSn catalysts have been found to vary considerably with synthesis methods,and the role of Sn is still far from fully *** gain in-depth insights into this issue,we synthesized a series of PtSn/SiO_(2)and SnPt/SiO_(2)catalysts by varying the deposition sequence and Pt:Sn ratios using atomic layer deposition with precise *** found that PtSn/SiO_(2)catalysts fabricated by the deposition of SnO_(x)first and then Pt,exhibited much better propylene selectivity and stability than the SnPt/SiO_(2)catalysts synthesized the other way *** demonstrate that the presence of Sn species at the Pt-SiO_(2)interface is of essential importance for not only the stabilization of PtSn clusters against sintering under reaction conditions but also the promotion of charge transfers to Pt for high *** the above,the precise regulation of the Sn content is also pivotal for high performance,and the excess amount of Sn might generate additional acidic sites,which could decrease the propylene selectivity and lead to heavy coke *** findings provide deep insight into the design of highly selective and stable PDH catalysts.

关键词： Propane dehydrogenation PtSn catalysts sintering coke formation acidity

Structure,electronic,and nonlinear optical properties of superalkaline M_(3)O(M=Li,Na)doped cyclo[18]carbon

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Chinese physics B 2024年第2期33卷 311-317页

作者：刘晓东卢其亮罗其全 School of physics and Material Science Anhui UniversityHefei 230601China institute of Physical Science and Information Technology Anhui UniversityHefei 230601China Department of chemical physics University of Science and Technology of ChinaHefei 230026China

Cyclo[18]carbon has received considerable attention thanks to its novel geometric configuration and special electronic *** have low ionization *** a superalkali in cyclo[18]carbon is an effective method to improve the optical properties of the system because considerable electron transfer *** this paper,the geometry,bonding properties,electronic structure,absorption spectrum,and nonlinear optical(NLO)properties of superalkaline M_(3)O(M=Li,Na)-doped cyclo[18]carbon were studied by using density functional theory.M_(3)O and the C_(18) rings are not *** C_(18) ring still exhibits alternating long and short *** charge transfer between M_(3)O and C_(18) forms stable[M_(3)O]+[C_(18)]-ionic complexes.C_(18)M_(3)O(M=Li,Na)shows striking optical nonlinearity,i.e.,their first-and second-order hyperpolarizability(βvec andγ||)increase considerably atλ=1907 nm and 1460 nm.

关键词： superalkaline doped cyclocarbon structure and electronic properties nonlinear optical properties density functional theory(DFT)