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Friction reactions induced by selective hydrogenation of textured surface under lubricant conditions

Friction 2024年第1期12卷 174-184页

作者： Naizhou DU Xubing WEI Xiaowei LI Zan CHEN Shiqi LU Jiaqing DING Cunao FENG Kai CHEN Jianghao QIAO Dekun ZHANG Kwang-Ryeol LEE Tiancai ZHANG School of Materials Science and Physics China University of Mining and TechnologyXuzhou 221116China Key Laboratory of Marine Materials and Related Technologies Zhejiang Key Laboratory of Marine Materials and Protective TechnologiesNingbo Institute of Materials Technology&EngineeringChinese Academy of SciencesNingbo 315201China Computational Science Center Korea Institute of Science and TechnologySeoul 136-791Republic of Korea Technology Development Department Shipbuilding Technology Research InstituteShanghai 200032China

The passivation of hydrogen atoms and the conformation of textured surfaces under oil-lubricated conditions are effective strategies to obtain amorphous carbon(a-C)films with extremely low friction.It is critical to understanding the influence mechanism of selective surface hydrogenation on the tribological behaviors of textured a-C film under oil-lubricated conditions.In particular,the interactions of hydrogen atoms and lubricants are confusing,which is enslaved to the in situ characterization technique.The reactive molecular dynamics(RMD)simulations were conducted to analyze the friction response of textured a-C films with selective hydrogenation surfaces under oil-lubricated conditions.The results indicate that the existence of hydrogen atoms on specific bump sites significantly decreases the friction coefficient(μ)of textured a-C film,which is highly dependent on the surface hydrogen content.The repulsion between hydrogen atoms and lubricant molecules prompts the formation of a dense lubricant film on the surface of the mating material.Interestingly,with the enhancement of the surface hydrogen content,the passivation of the friction interface and the repulsion between hydrogen atoms and lubricants play dominant roles in reducing the friction coefficient instead of hydrodynamic lubrication.

关键词： textured amorphous carbon(a-C) selective hydrogenation oil lubrication friction mechanism reactive molecular dynamics(RMD)

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Synergistic effects of PtFe/CeO_(2)catalysts afford high catalytic performance in selective hydrogenation of cinnamaldehyde

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Journal of Rare Earths 2023年第2期41卷 233-239页

作者： Xia Gong Quanquan Shi Xinyu Zhang Jinmei Li Guichen Ping Hui Xu Hongjing Ding Gao Li College of Science&Key Laboratory of Soil Quality and Nutrient Resources Inner Mongolia Agricultural UniversityHohhot 010018China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

selective hydrogenation of unsaturated aldehydes remains a grand challenge in controlling chemoselectivity up to now.We synthesized a series of PtFex/CeO_(2)catalysts,which were characterized by X-ray diffraction(XRD),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS)as well as temperature-programmed-reduction by hydrogen(H2-TPR).The catalytic performance of PtFex/CeO_(2),including cinnamaldehyde(CAL)conversion and selectivity toward cinnamyl alcohol(COL),is improved remarkably by introduction of Fe species in the Pt particles in the selective CAL hydrogenation under mild conditions.XPS results indicate that the electron transfer from Fe to Pt promotes CAL adsorption,resulting in the enhanced CAL conversion.And the COL selectivity is improved by CAL adsorption via an interaction of C=O group with surface oxygen defect sites because of interaction between PtFe and CeO_(2)support.In all,this study may provide some hints to design efficient nano Pt particles for the selective hydrogenation.

关键词： PtFex/CeO_(2) Synergistic effect selective hydrogenation Cinnamaldehyde Surface oxygen defect Rare earths

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Green and selective hydrogenation of aromatic diamines over the nanosheet Ru/g-C_(3)N_(4)-H_(2) catalyst prepared by ultrasonic assisted impregnation-deposition method

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Green Energy & Environment 2022年第6期7卷 1361-1376页

作者： Huanhuan Yang Liguo Wang Shuang Xu Yan Cao Peng He Jiaqiang Chen Zheng Zheng Huiquan Li Key Laboratory of Green Process and Engineering National Engineering Laboratory for Hydrometallurgical Cleaner Production TechnologyInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China Chemical and Biochemical Engineering Technical University of DenmarkLyngby 2800 KgsDenmark Sino-Danish College University of Chinese Academy of SciencesBeijing100049China Sino-Danish Center for Education and Research University of Chinese Academy of SciencesBeijing100049China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Dalian National Laboratory for Clean Energy Dalian116023China

In this study,nanosheet g-C_(3)N_(4)-H_(2) was prepared by thermal exfoliation of bulk g-C_(3)N_(4) under hydrogen.A series of Ru/g-C_(3)N_(4)-H_(2) catalysts with Ru species supported on the nanosheet g-C_(3)N_(4)-H_(2) were synthesized via ultrasonic assisted impregnation-deposition method.Ultrafine Ru nanoparticles(selective hydrogenation performance of bi-benzene ring,i.e.,almost complete 4,40-diaminodiphenylmethane(MDA)conversion and>99%4,40-diaminodicyclohexylmethane selectivity,corresponding to a reaction activity of 35.7 mol_(MDA) mol_(Ru)^(-1) h^(-1).Moreover,the reaction activity of catalyst in the fifth run was 36.5 mol_(MDA) mol_(Ru)^(-1) h^(-1),which was comparable with that of the fresh one.The computational results showed that g-C_(3)N_(4) as support was favorable for adsorption and dissociation of H_(2) molecules.Moreover,the substrate scope can be successfully expanded to a variety of other aromatic diamines.Therefore,this work provides an efficient and green catalyst system for selective hydrogenation of aromatic diamines.

关键词： Nanosheet carbon nitride Ultrafine Ru species selective hydrogenation Aromatic diamine Alicyclic diamine

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A top–down strategy to realize the synthesis of small-sized L10 - platinum-based intermetallic compounds for selective hydrogenation

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Nano Research 2022年第10期15卷 9631-9638页

作者： Yu Jin Guomian Ren Yonggang Feng Shize Geng Ling Li Xing Zhu Jun Guo Qi Shao Yong Xu Xiaoqing Huang Jianmei Lu College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices Collaborative Innovation Center of Advanced Energy MaterialsSchool of Materials and EnergyGuangdong University of TechnologyGuangzhou 510006China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Testing&Analysis Center Soochow UniversitySuzhou 215123China

The synthesis of Pt-based nanoparticles(NPs)with ultrasmall feature and tailored structure is of great importance for catalysis yet challenging.In this work,we demonstrate a facile top–down strategy for the fabrication of small-sized Pt-based intermetallic compounds(IMCs)with L10 structure through the evaporation of Cd under high temperature.Impressively,such thermal treatment can be used as a versatile strategy for creating binary,ternary,quaternary,quinary,and senary L10-Pt-based IMCs.Moreover,the small-sized Pt-based IMCs display high stability against high temperature of 700℃,which can serve as active and selective catalyst for the selective hydrogenation of 4-nitrophenylacetylene.This work may not only provide a versatile top–down strategy for fabricating highly stable small-sized Pt-based NPs with L10 structure,but also promote their extensive applications in catalysis and beyond.

关键词： top-down strategy Pt-based intermetallic compound small-sized selective hydrogenation

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Highly efficient and anti-poisoning single-atom cobalt catalyst for selective hydrogenation of nitroarenes

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Nano Research 2022年第12期15卷 10006-10013页

作者： Yuemin Lin Renfeng Nie Yuting Li Xun Wu Jiaqi Yu Shaohua Xie Yajing Shen Shanjun Mao Yuzhuo Chen Dan Lu Zongbi Bao Qiwei Yang Qilong Ren Yiwen Yang Fudong Liu Long Qi Wenyu Huang Zhiguo Zhang Key Laboratory of Biomass Chemical Engineering of Ministry of Education Cllege of Chemical and Biological EngineeringZhejiang University38 Zheda RoadHangzhou 310027China U.S.DOE Ames Laboratory lowa State UniversityAmeslowa 50011USA Department of Chemistry Iowa State UniversityAmeslowa 50011USA College of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Department of Civil Environmentaland Construction EngineeringCatalysis Cluster for Renewable Energy and Chemical Transformations(REACT)Nano Science Technology Center(NSTC)University of Central FloridaOrlandoFL 32816USA Advanced Materials and Catalysis Group Institute of CatalysisDepartment of ChemistryZhejiang UniversityHangzhou 310028China Institute of Zhejiang University-Quzhou Quzhou 324000China

Developing non-precious metal catalysts to selectively reduce functionalized nitroarenes with high efficiency is urgently desirable for the production of value-added amines.Herein,we report a novel,efficient,anti-poisoning single-atom cobalt catalyst(Co-NAC)for the highly selective hydrogenation of the nitro to amino group for nitroarenes baring various functional groups,including vinyl,cyano,and halogen.Using a combination of structure characterization techniques,we have confirmed that the cobalt species are predominantly present in the form of four-coordinated Co single sites anchored on nitrogen-assembly carbon(NAC)as the ordered mesoporous support.Co-NAC catalysts enable the full conversion and>99%selectivity with molecular H2 as a green reductant under mild conditions(80℃,2 MPa H2).As for the selective hydrogenation of 3-nitrostyrene,Co-NAC catalyst affords high catalytic productivity(19.7 h-1),which is superior to the cobalt nanoparticles(NPs)catalysts and most of the recently reported Co-based catalysts.This is attributed to the highly accessible atomically-dispersed Co active sites,the high surface area with ordered-mesoporous morphology and the prominent high content of nitrogen dopants.Notably,Co-NAC catalyst displays resistance towards sulfur-containing poisons(20 equivalents)and strong non-oxidizing acid(8 M),showing great potential for continuous application in the chemical industry.

关键词： cobalt single-atom selective hydrogenation nitroarenes 3-nitrostyrene poisoning resistance

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Dynamically modulated synthesis of hollow metal-organic frameworks for selective hydrogenation reactions

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Nano Research 2023年第8期16卷 11334-11341页

作者： Liyun Xiao Chuanqi Cheng Zhixi Li Chaoyang Zheng Jing Du Meina Song Yue Wan Shaopeng Li Guo Jun Meiting Zhao Department of Chemistry Institute of Molecular Aggregation ScienceTianjin Key Laboratory of Molecular Optoelectronic SciencesTianjin UniversityTianjin 300072China Institute of New Energy Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300072China State Key Laboratory of Separation Membranes and Membrane Processes School of ChemistryTiangong UniversityTianjin 300387China

Hollow metal-organic frameworks(MOFs)have attracted increasing attention in the field of catalysis in recent years due to their unique cavity structure with fast mass-diffusion rates and easily accessible active sites.Here,we report the use of dynamic modulators,which are formed by the in-situ imine condensation reaction of 4-aminobenzoic acid and 4-formylbenzoic acid,to regulate the growth of MOFs to synthesize well-defined hollow thioether functionalized UiO-67(denoted as H-UiO-67-S)single crystals.After supporting Pd nanoparticles,the designed catalysts Pd@H-UiO-67-S show excellent conversion(>99.9%),selectivity(>99.9%),and stability(10 cycles)in the selective hydrogenation of nitrobenzenes with other reducible groups.Density functional theory calculations and the experimental results reveal that Pd nanoparticles not only selectively adsorb the nitro-groups on nitrobenzene,but also restrict the adsorption of the aniline product,due to the interaction of thioether with Pd in the confined pores of H-UiO-67-S,finally result in a significant increase in selectivity of nitro-hydrogenation.

关键词： hollow structure metal-organic frameworks(MOFs) dynamically modulated synthesis selective hydrogenation nitrobenzene

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AuPt bimetallic nanoalloys supported on SBA-15:A superior catalyst for quinoline selective hydrogenation in water

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Nano Research 2022年第3期15卷 1796-1802页

作者： Jianbo Zhao Haifeng Yuan Guang Yang Yingfan Liu Xiaomei Qin Zheng Chen Cheong Weng-Chon Liming Zhou Shaoming Fang School of Material and Chemical Engineering Zhengzhou University of Light IndustryZhengzhou 450001China Key Laboratory of Functional Molecular Solids Ministry of EducationAnhui Key Laboratory of Molecule-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241000China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoMacao SARChina

The structure and size of bimetallic catalysts play a crucial role in many important chemical transformations.Controlled synthesis of bimetallic nanoparticles avoiding overgrowth and aggregation can be achieved by surfactants,which are always detrimental to catalytic performances and understanding of structure-property relationship.Preparation of surface-clean bimetallic catalysts with uniform size and well-defined structure is still challenging.Herein the Au-Pt bimetallic nanoparticles immobilized on SBA-15 were prepared by facile adsorption-reduction method.Characterizations showed that Au-Pt bimetallic nanoparticles were evenly confined within the mesopores of SBA-15,possessing the uniform size of 6.0 nm and existing in the form of alloy structure.For the first time the Au-Pt bimetallic nanoalloys with Au-to-Pt molar ratio of 5:1(Au5Pt1@SBA-15)exhibited a lot higher activity than monometallic Au@SBA-15 and Pt@SBA-15 catalysts with excellent selectivity towards 1,2,3,4-tetrahydroquinoline for chemoselective hydrogenation of quinoline in water under very mild conditions.It was superior to other heterogeneous catalysts reported to date.The observed properties were related to the synergic effect between Au and Pt.The Pt sites of high electron density originated from the electron transfer between Au and Pt enhanced the ability of H_(2) dissociation and then provided a new and main approach to H_(2) splitting,while the Au sites accounted for the adsorption and activation of quinoline.This precise synthetic strategy will be very helpful to explore surface-clean gold-based bimetallic catalysts with high performance for selective hydrogenations.

关键词： gold platinum bimetallic catalyst quinoline selective hydrogenation

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Ir nanoclusters confined within hollow MIL-101(Fe)for selective hydrogenation ofα,β-unsaturated aldehyde

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Chinese Chemical Letters 2022年第1期33卷 374-377页

作者： Qinglin Liu Qian Liu Yurong Chen Yinle Li Hui Su Qinghua Liu Guangqin Li MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026China

Although the selective hydrogenation ofα,β-unsaturated aldehyde to unsaturated alcohol(UOL)is an extremely important transformation,it is still a great challenge to achieve high selectivity to UOL due to thermodynamic favoring of the C=C hydrogenation over the C=O hydrogenation.Herein,we report that iridium nanoclusters(Ir NCs)confined within hollow MIL-101(Fe)expresses satisfied reaction activity(93.9%)and high selectivity(96.2%)for the hydrogenation of cinnamaldehyde(CAL)to cinnamyl alcohol(COL)under 1 bar H;atmosphere and room temperature.The unique hollow structure of MIL-101(Fe)benefits for the fast transport of reactant,ensuring the comparable reaction activity and better recyclability of Ir@MIL-101(Fe)than the counterparts which Ir NCs were on the surface of MIL-101(Fe).Furthermore,The X-ray photoelectron spectroscopy data indicates the electropositive Ir NCs,owing to the electron transfer from Ir to MIL-101(Fe),can interact with oxygen lone pairs,and Fourier transform infrared spectrum shows the Lewis acid sites in MIL-101(Fe)can strongly interact with C=O bond,which contributes to a high selectivity for COL.This work suggests the considerable potential of synergetic effect between hollow MOFs and metal nanoclusters for selective hydrogenation reactions.

关键词： Iridium Hollow metal-organic frameworks selective hydrogenation α β-Unaturated aldehyde Heterogeneous catalysis

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Kinetics of selective hydrogenation of PAHs from FCC Slurry Extract over Ni-W/γ-Al_(2)O_(3) Catalyst

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China Petroleum Processing & Petrochemical Technology 2023年第4期25卷 31-40页

作者： Cui Wenlong Wu Fubu Chen Yulong Qian Junfeng Luo Hui Liu Yingjie Yang Jihe Jiangsu Province Key Laboratory of Fine Petrochemical Engineering Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterCNPC-CZU Innovation AllianceSchool of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China State Key Laboratory of Heavy Oil Processing China University of PetroleumQingdao 266580China

The selective hydrogenation of polycyclic aromatic hydrocarbons(PAHs)from fluid catalytic cracking(FCC)slurry extract was conducted in a batch reactor over aγ-Al_(2)O_(3)-supported bimetallic Ni-W catalyst.For the Ni-W/γ-Al_(2)O_(3) catalyst,the experiment run was divided into three processes according to the reaction conditions used:(1)the absence of hydrogenation as both temperature and pressure increased;(2)the desulfurization of FCC slurry extract under a fixed pressure as the temperature increased;and(3)the selective hydrogenation of PAHs when both pressure and temperature remained constant.The hydrogen consumption could be accurately calculated from the Redlich–Kwong equation of state.The results for the removal of PAHs with hydrogenation displayed an excellent fit to the first-order kinetics.The apparent activation energy was determined to be 20.80 kJ/mol.

关键词： selective hydrogenation kinetics PAHs FCC slurry extract

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Kinetic Model of LCO selective hydrogenation on NiMoW/Al_(2)O_(3) Catalyst

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China Petroleum Processing & Petrochemical Technology 2022年第3期24卷 1-9页

作者： Ju Xueyan Zhang Kui Xi Yuanbing Wang Zhe Nie Hong SINOPEC Research Institute of Petroleum Processing Co. Ltd.Beijing 100083

In order to investigate the hydrofining process of LCO for producing aromatics and gasoline,the selective hydrogenation of polycyclic aromatic hydrocarbons(PAHs),a major component of light cycle oil(LCO),was studied using a NiMoW/Al_(2)O_(3)catalyst.Based on the study of the reversible hydrogenation reaction,PAHs in the selective hydrogenation process could be effectively simulated by the modeled CH and CH_(2) groups,and the hydrodesulfurization and hydrodenitrogenation kinetic models could be further established in this process.The results showed that the kinetic models developed could fit the experimental data effectively and predict the content of S,N,and aromatics in the selective hydrogenation products of LCO.

关键词： LCO selective hydrogenation PAHs kinetic model CH group

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