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Nano-sized stationary phase packings retained by single-particle frit for microchip liquid chromatography

Chinese Chemical Letters 2024年第4期35卷 486-489页

作者： Wangyan Hu Ke Li Xiangnan Dou Ning Li Xiayan Wang Center Excellence for Environmental Safety and Biological Effects Beijing Key Laboratory for Green Catalysis and SeparationDepartment of ChemistryBeijing University of TechnologyBeijing 100124China Center for Environmental Metrology National Institute of MetrologyBeijing 100029China

Modern chromatography is increasingly focused on miniaturization and integration. Compared to conventional liquid chromatography, microfluidic chip liquid chromatography(microchip-LC) has the potential due to its zero-dead volume connection and ease of integration. Nano-sized packings have the potential to significantly enhance separation performance in microchip-LC. However, their application has been hindered by packing difficulties. This study presents a method for packing nano-sized silica particles into a microchannel as the stationary phase. The microchip-LC packed column was prepared by combining the weir and the porous silica single-particle as frit to retain the packing particles. A surface tensionbased single-particle picking technique was established to insert porous single-particle frit into glass microchannels. Additionally, we developed a slurry packing method that utilizes air pressure to inject nano-sized packing into the microchannel. Pressure-driven chromatographic separation was performed using this nano-packed column integrated into a glass microchip. The mixture of four PAHs was successfully separated within just 8 min using a 5 mm separation channel length, achieving high theoretical plates(10~6plates/m). Overall, these findings demonstrate the potential of utilizing nano-sized packings for enhancing chromatographic performance in microchip systems.

关键词： Nano-size packing Single-particle frit Packed column Microchip LC Chromatographic separation

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Revealing the specific role of sulfide and nano-alumina in composite solid-state electrolytes for performance-reinforced ether-nitrile copolymers

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Journal of Energy Chemistry 2024年第4期91卷 628-636页

作者： Haoyang Yuan Changhao Tian Mengyuan Song Wenjun Lin Tao Huang Aishui Yu Department of Chemistry Collaborative Innovation Center of Chemistry for Energy MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsInstitute of New EnergyFudan UniversityShanghai 200438China Laboratory of Advanced Materials Fudan UniversityShanghai 200438China

Composite solid-state electrolytes represent a critical pathway that balances the interface compatibility and lithium-ion conductivity in all-solid-state *** quest for stable and highly ion-conductive combinations between polymers and fillers is vital,but blind attempts are often made due to a lack of understanding of the mechanisms involved in the interaction between polymers and ***,we employ in-situ polymerization to prepare a polymer based on an ether-nitrile copolymer with high cathode stability as the foundation and discuss the performance enhancement mechanisms of argyrodite and *** 1%content of sulfide interacting with the polymer at the two-phase interface,the local enhancement of lithium-ion migration capability can be achieved,avoiding the reduction in capacity due to the low ion conductivity of the passivation layer during *** capacity retention after 50cycles at 0.5 C increases from 83.5%to 94.4%.Nano-alumina,through anchoring the anions and interface inhibition functions,eventually poses an initial discharge capacity of 136.8 m A h g^(-1)at 0.5 C and extends the cycling time to 1000 h without short-circuiting in lithium metal *** the combined action of dual fillers on the composite solid-state electrolyte,promising insights are provided for future material design.

关键词： Composite solid-state electrolytes Lithium metal anode Dual fillers Interfacial ionic conduction Inert nano-alumina

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Oxidative Dehydrogenation of Propane over Supported Nickel Single-Atom Catalyst

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Chinese Journal of Chemistry 2024年第4期42卷 370-376页

作者： Qian Zhang Xunzhu Jiang Yangyang Li Yuanlong Tan Qike Jiang Xiaoyan Liu Botao Qiao CAS Key Laboratory of Science and Technology on Applied catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023 China University of Chinese Academy of Sciences Beijing100049 China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianLiaoning116023 China

Oxidative dehydrogenation of propane has been an ever-growing field for propylene production due to its exothermic properties,of which overoxidation is the major drawback,with CO and even CO_(2) as undesired *** the purpose of getting higher propylene selectivity as well as yield,herein,we report Ni single atoms supported on calcium aluminate as an efficient catalyst candidate for propane oxidative *** from higher valence states of Ni1 species,it shows 2—3 times as much propylene selectivity as that of Ni *** 14.2%C_(3)H_(6) yield with 47.3%propylene selectivity has been achieved on Ni single atom catalyst and a good stability during 20 h test can be obtained as well.

关键词： Oxidative dehydrogenation/Nickel Single-atom catalysts Propane Propylene selectivity

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Interfacial assembly of 2D polydopamine/graphene heterostructures with well-defined mesopore and tunable thickness for high-energy planar micro-supercapacitors

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Chinese Chemical Letters 2024年第7期35卷 439-444页

作者： Jieqiong Qin Zhi Yang Jiaxin Ma Liangzhu Zhang Feifei Xing Hongtao Zhang Shuxia Tian Shuanghao Zheng Zhong-Shuai Wu College of Science Henan Agricultural UniversityZhengzhou 450002China State Key Laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China Mechanical and Electrical Engineering institute Zhengzhou University of Light IndustryZhengzhou 450002China

Two-dimensional(2D)mesoporous pseudocapacitive polymer/graphene heterostructures combine the advanced merits of 2D materials and mesoporous materials,possessing unique nanosheet structure,large specific surface area(SSA),abundant oxygen/nitrogen-containing groups,desirable electrical conductivity and admirable electrochemical redox activity,and hold great potential for constructing high-performance planar micro-supercapacitors(MSCs).Herein,we demonstrate the interfacial assembly of 2D mesoporous polydopamine/graphene(mPDG)heterostructures with well-defined mesopore structure(12 nm)and adjustable thickness(7.5–14.1 nm)for planar high-energy pseudocapacitive *** to medium thickness,exposed mesopore of 12 nm and large SSA of 108 m^(2)/g,the m PDG with 10.8 nm thickness reveals prominent mass capacitance of 419 F/g and impressive cycling stability with~96%capacitance retention after 5000 ***,the symmetric mPDG-based MSCs with“water-in-salt”gel electrolyte present wide voltage window of 1.6 V,superior volumetric energy density of 11.5 mWh/cm^(3),outstanding flexibility and self-integration ***,this work offers a new platform of controllably synthesizing 2D mesoporous heterostructures for high-performance MSCs.

关键词： 2D materials Mesopores Heterostructures Polydopamine High energy density Micro-supercapacitors

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Modeling and analysis of air combustion and steam regeneration in methanol to olefins processes

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Chinese Journal of Chemical Engineering 2024年第2期66卷 94-103页

作者： Jinqiang Liang Danzhu Liu Shuliang Xu Mao Ye Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China National Engineering Research Center of Lower-Carbon catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116021China University of Chinese Academy of Sciences Beijing 100049China

Light olefins is the incredibly important materials in chemical *** to olefins(MTO),which provides a non-oil route for light olefins production,received considerable attention in the past ***,the catalyst deactivation is an inevitable feature in MTO processes,and regeneration,therefore,is one of the key steps in industrial MTO *** the MTO catalyst is regenerated by removing the deposited coke via air combustion,which unavoidably transforms coke into carbon dioxide and reduces the carbon utilization *** study shows that the coke species over MTO catalyst can be regenerated via steam,which can promote the light olefins yield as the deactivated coke species can be essentially transferred to industrially useful synthesis gas,is a promising pathway for further MTO processes *** this work,we modelled and analyzed these two MTO regeneration methods in terms of carbon utilization efficiency and technology *** shown,the steam regeneration could achieve a carbon utilization efficiency of 84.31%,compared to 74.74%for air combustion *** MTO processes using steam regeneration can essentially achieve the near-zero carbon *** addition,light olefins production of the MTO processes using steam regeneration is 12.81%higher than that using air combustion *** this regard,steam regeneration could be considered as a potential yet promising regeneration method for further MTO processes,showing not only great environmental benefits but also competitive economic performance.

关键词： Model Methanol to olefins Regeneration Greenhouse gas Processes simulation

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Design and synthesis of polyoxovanadate-based framework for efficient dye degradation

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Tungsten 2024年第2期6卷 447-453页

作者： Qing Lan Su-Juan Jin Zheng Wang Xu-Yang Li Yan Xiong Zhuo-Cheng Wang Shan-Shan Liu Zhi-Ming Zhang Qiang Zhao Engineering Technology Research Center of Henan Province for Solar catalysis School of Chemical and Pharmaceutical EngineeringNanyang Normal UniversityNanyang 473061China institute of New Energy Materials&Low Carbon Technology Tianjin University of TechnologyTianjin 300384China

A new polyoxovanadate-based framework material[Cu(en)_(2)]_(4)V_(18)O_(42)(H_(2)O)·6H_(2)O(1)was designed and synthesized by hydrothermal reaction of NaVO_(3),Cu(NO_(3))_(2)·6H_(2)O and 1,2-diaminoethane(en)via carefully adjusting the pH value of the reaction *** structure of the title compound has been determined by single-crystal X-ray diff raction analysis,thermogravimetric analysis,infrared spectra and elemental *** structural analysis demonstrate the three-dimensional(3D)framework structure of compound 1,which was composed of the[V_(18)O_(42)(H_(2)O)]_(8)−({V_(18)O_(42)(H_(2)O)})anions linked by the Cu^(2+)*** 1 represents the fi rst 3D framework based on{V_(18)O_(42)(H_(2)O)}polyoxoanions and copper ***-driven degradation of residual organic pollutants in industrial wastewater is still a major problem for human *** experiments reveal that compound 1 possesses of excellent photocatalytic activity for the degradation of methylene blue and rhodamine B.

关键词： Polyoxovanadate Framework Polyoxovanadate-based framework Photocatalytic Organic pollutants

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Catalytic enantioselective N-silylation of sulfoximine

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Chinese Chemical Letters 2024年第4期35卷 352-356页

作者： Xingfen Huang Jiefeng Zhu Chuan He Shenzhen Grubbs institute and Department of Chemistry Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhen 518055China Key Laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education Hangzhou Normal UniversityHangzhou 311121China

A rhodium/diphosphine-catalyzed asymmetric cross-dehydrogenative coupling between sulfoximines and dihydrosilanes has been achieved. This is the first report on the enantioselective N-silylation of sulfoximines. The protocol gives access to a variety of Si-stereogenic N-silylated sulfoximines in decent yield(up to 99%) with excellent stereoselectivity(up to 99%), featuring high atom economy, and a cleaner manner with H2as the sole byproduct. The obtained bis-Si-stereogenic monohydrosilane product can be further converted into the corresponding chiral polymer with pendant sulfoximine groups.

关键词： N-Silylation of sulfoximine Chiral silylamine Si-stereogenic silanes Si-CADC Asymmetric catalysis

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The nature of active sites in Pt–ReO_X/TiO_2 catalysts for selective hydrogenation of carboxylic acids to alcohols

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Journal of Energy Chemistry 2015年第5期24卷 646-654页

作者： Alexey Suknev Vladimir Zaikovskii Vasily Kaichev Eugenii Paukshtis Ekaterina Sadovskaya Bair Bal'zhinimaev boreskov institute of catalysis sb ras Novosibirsk State University

The highly dispersed Pt-ReOx （x _〈 1 ） sites ca. 0.5 nm in size were formed via a successive and strong inter- action of the Re precursor with titania and then of the Pt complex with deposited low-valent rhenium oxide clusters. The size, charge and chemical composition were characterized by means of HRTEM/STEM with EDX mapping, XPS, and FTIRS. These sites with Re/Pt = 2 were shown to be highly active and selective in the hydrogenation of carboxylic acid to alcohol under very mild conditions （T = 130 ℃, P = 50 bar）. The reaction rate constant for the hydrogenation of hexanoic acid increased linearly with the Pt content. As for the homogeneous pincer-type Ru-organic complexes, the active Pt-ReOx sites can dissociate heterolytically the molecular hydrogen with the formation of hydroxyl groups and Pt hydride for hydrogenation of the carboxylic group. Indeed, TOF of 20 h 1 and selectivity of 98%-99% are approaching the values typical of homogeneous catalysts. The first order kinetics described well the experimental data obtained in a wide range of reaction conditions.

关键词： Selective hydrogenation Hexanoic acid Hexanol PlatinumRhenium Nanoparticles

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Deciphering dynamic surface of PtRu alloy nanocatalysts to revisit their synergistic effects during the electrooxidation

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Science China Chemistry 2024年第7期67卷 2224-2233页

作者： Xiao-Chong Li Bo Wang Zhou Yu Qiang Wan Ju-Fang Zheng Emmanuel Maisonhaute Xiao-Shun Zhou Ya-Hao Wang Key Laboratory of the Ministry of Education for Advanced catalysis Materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China Laboratoire Interface et Systèmes Electrochimiques CNRS UMR 8235Sorbonne UniversitéF-75252 Paris cedex 5France

Correlating dynamic structural transformation of catalysts with the surface intermediate species under operating conditions is critical for updating the understanding of structure–performance ***,we probe the electrochemical potentialdependent surface structures and adsorbed intermediates on PtRu binary alloy nanocatalysts to revisit its synergistic mechanisms for CO electrooxidation enhanced ***-situ spectral characteristics by using modified shell-isolated nanoparticle-enhanced Raman spectroscopy,show that in acidic solution,when the potential is positively scanned from 0.1 V to 1.5 V relative to reversible hydrogen electrode(RHE),the surface of the alloy catalyst evolves from metallic PtRu to adsorbed oxygen gradually covering and accumulating on Ru sites(denoted as PtRuO_(x),x≤2),forming segregated RuO_(2),and finally forming a threedimensional oxide layer(denoted as 3D PtRuO_(4)).Moreover,molecular evidence associated with periodic density functional theory calculations reveals that electronic effects promote ruthenium to become more oxidizable and *** particular,we found here that ^(*)O and ^(*)OH at surface RuO_(x) sites are highly efficient CO oxidation active species in comparison to the same entities adsorbed on metallic Ru *** work sheds light on the complex surface dynamic process of practical Pt-based binary nanocatalysts and improves the understanding of synergistic mechanism for the development of fuel cell devices.

关键词： in-situ Raman spectroscopy surface evolution bifunctional mechanism PtRu electrooxidation

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高能量密度的微型储能器件的展望

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Science Bulletin 2024年第6期69卷 714-717页

作者：王森 Pratteek Das 吴忠帅 State Key Laboratory of catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

The pursuit for Internet of Things(IoT)-enabled microelectronic devices has taken the scientific community by storm,and to power them,microscale electrochemical energy storage devices(MESDs),including microsupercapacitors(MSCs)and microbatteries(MBs)are considered ideal on-chip power sources[1].This is not surprising,given the inherent advantages of MESDs like facile microfabrication with an ultra-compact footprint,easy achievement of high areal capacity,and compatible integration with various functional microelectronic devices while providing smaller current drains.

关键词：高能量密度 pursuit drain

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