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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

Binding SnO2 Nanoparticles with MoS2 Nanosheets Toward Highly Reversible and Cycle-Stable Lithium/Sodium Storage

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Energy & Environmental Materials 2024年第4期7卷 135-142页

作者： Deliang Cheng Wenbiao Zhang Yi Tang Qingsheng Gao Renzong Hu Lichun Yang Min Zhu Institute of advanced Materials Jiangxi Normal University School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials South China University of Technology College of Chemistry and Materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and Applications Jinan University Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Laboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials Fudan University

SnO2,with its high theoretical capacity,abundant resources,and environmental friendliness,is widely regarded as a potential anode material for lithium-ion batteries （LIBs）.Nevertheless,the coarsening of the Sn nanop... 详细信息

关键词： 1 T-MoS2 heterostructure lithium-ion batteries Sn coarsening SnO2

Simultaneously enhanced electrochemical performance and air stability of Ni-rich cathode with a modified washing process

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Rare Metals 2024年第1期43卷 87-97页

作者： Ben-Rui Hu Ying-Yi Yuan Yu-Cheng Wang Xun-Hui Xiong School of Environment and Energy Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510640China

Water washing has been regarded as one of the most effective strategies to remove surface residual lithium of nickel-rich layered oxides for lithium-ion batteries(LIBs).However,the loss of lattice lithium during the water washing process deteriorates the electrochemical performances and air ***,washing the LiNi_(0.90)Co_(0.05)Al_(0.02)O_(2)(NCA) with ammonium dihydrogen phosphate(NH_(4)H_(2)PO_(4)) solution has been proposed to simultaneously enhance electrochemical performances and air stability,in which in-situ generated Li_(3)PO_(4) coating layer on surface of NCA can suppress the loss of lattice ***,as a fast ionic conductor,Li_(3)PO_(4) coating layer on NCA can prevent the direct contact with electrolyte/*** a result,the NH_(4)H_(2)PO_(4) solution washed NCA cathode can deliver a high capacity of131.9 mAh·g^(-1) at 10.0C rate as well as impressive cycle stability with a capacity retention of 83.1% after 100 cycles at 1.0C,much higher than those of water washed NCA(WS-NCA) *** exposed in air for 7 days,the NH_(4)H_(2)PO_(4) solution washed NCA electrode can more effectively maintain the structural integrity as well as the electrochemical performances than water-washed *** work provides a simple and effective approach to enhance the cycle stability and air stability of Nickel-rich cathode materials.

关键词： Layered Ni-rich cathode Residual lithium Li_(3)PO_(4)coating Rate performance Air stability

Chain Dynamics Heterogeneity in Plasticized Poly(vinyl butyral)(PVB) as Elucidated by Solid-State NMR

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Chinese Journal of Polymer Science 2024年第1期42卷 113-124,I0010页

作者： Jing Lv Xu Chen Zi-Shuo Wu Ya-Hui Li Wei Chen National Synchrotron Radiation laboratory Anhui Provincial Engineering Laboratory of Advanced Functional Polymer FilmCAS Key Laboratory of Soft Matter ChemistryUniversity of Scienceand Technology of ChinaHefei 230026China

The chain dynamics heterogeneity of the poly(vinyl butyral)(PVB) plasticized by triethylene glycol bis(2-ethylhexa noate)(TEG-EH) was investigated by various solid-state NMR *** plasticized PVB shows two domains in distinct molecular dynamics differences,namely,rigid and soft domains,where the latter is the plasticizer-rich *** time domain low field NMR was first used to investigate the dynamics heterogeneity of the plasticized PVB,and the results show the decreasing activated energy of components in the soft domain of plasticized PVB(E_a=20.2 kJ/mol) as compared with that of the pristine one(E_a=24.3 kJ/mol).Detailed dynamics heterogeneity was obtained by high-field NMR with site-specific *** quadrupole-echo ~2H-NMR was adopted to elucidate the dynamics heterogeneity of the vinyl alcohol(VA) units,where only the hydroxyl group of VA is *** ~1H-^(13)C WISE NMR spectra show that there is not much difference in the mobility of the VB unit in PVB with and without plasticizer,whereas the glass transition temperature differed by approximately 53℃.This is further supported by Torchia's T_1 relaxation *** origin of such an unusual phenomenon is attributed to the critical role of the remaining VA(~22%) in the soft domain,where the VA units locally aggregate through hydrogen ***,the existence of a mobility gradient in the VB unit has been ***,the mobility difference for VB with different stereo-geometry(meso or racemic conformation) is observed for the first *** indicates the importance of modulating the ratio of meso over racemic VB for controlling the macroscopic perfo rmance of PVB.

关键词： Poly(vinyl butyral) Dynamics heterogeneity Plasticizer Solid state NMR

Unraveling role of double-exchange interaction in electrochemical water oxidation by external magnetic field

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Rare Metals 2024年第1期43卷 289-297页

作者： Jun Li Jun-Ming Li Hong Hong Dong-Xue Liu Qing-Qi Cao Dun-Hui Wang National laboratory of Solid State Microstructures and jiangsu provincial key laboratory for Nanotechnology Nanjing UniversityNanjing 210093China School of Electronics and Information Hangzhou Dianzi UniversityHangzhou 310018China

Double-exchange(DE) interaction plays an important role in electrocatalytic oxygen evolution reaction(OER).However,precise achievement of DE interaction often requires foreign dopants or vacancy engineering,leading to destabilization of the catalysts and deterioration of *** contrast,the utilization of environmentally friendly,contactless,and continuously adjustable magnetic fields to study the OER process is profitable to avoid aforementioned interference factors and further elucidate the direct relationship_(0.5)between DE interaction and OER ***,by using cobalt hydroxide carbonate(Co(OH)(CO_(3))·xH_(2)O,CoHC) nanostructures as a proof-of-concept study,external magnetic fields are carefully implemented to verify the role of DE interaction during water oxidation *** studies reveal that external magnetic fields effectively enhance the reaction rate of the catalyst,the overpotential decreases from 386 to 355 mV(100 mA·cm^(-2)),while Tafel slopes drastically decline from 93 to 67 mV·dec^(-1)(1.0 T).Moreover,magnetic field increment exhibits robust *** in situ Raman and impedance measurements under external field,it can be found that magnetic field promotes the electron migration between Co^(2+) and Co^(3+) in the CoHC catalysts with the assistance of DE interactions,thus boosting the OER efficiency.

关键词： Magnetic field Double-exchange(DE)interaction Electrocatalysis Oxygen evolution reaction(OER) Cobalt hydroxide carbonate

Membrane-less MoO_(3-x)@TiO_(2)-bromine battery with excellent rate capability and cyclic stability

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Journal of Energy Chemistry 2024年第6期93卷 316-321,I0008页

作者： Wenjie Huang Hui Wang Bin Yuan Liuzhang Ouyang Lichun Yang Min Zhu School of Materials Science and Engineering Guangdong Provincial Key Laboratory of Advanced Energy Storage MaterialsSouth China University of TechnologyGuangzhou 510640GuangdongChina

Bromine has attracted significant attention as a cathode material for aqueous batteries due to its high reduction potential of 1.05 V(Br_(3)^(-)+2e~-■3Br~-),impressive theoretical specific capacity of 223 mA h g^(-1),and rapid reaction kinetics in the ***,searching for compatible anode materials to match with bromine has posed a challenge due to its highly corrosive *** this study,we developed oxygen-deficient MoO_(3) with TiO_(2) coating(referred to as MoO_(3-x)@TiO_(2))as an anode material to pair with a bromine cathode in static full *** oxygen deficiency contributes to enhanced electronic and protonic diffusion within the MoO_(3-x)lattice,while the TiO_(2) coating mitigates structural dissolution and proton trapping during *** MoO_(3-x)@TiO_(2) demonstrates fast charge storage kinetics and excellent resistance to bromine *** impressive compatibility between MoO_(3-x)@TiO_(2) and bromine enables the construction of membrane-less full batteries with exceptional rate capability and cyclic *** MoO_(3-x)@TiO_(2)-bromine battery achieves an energy density of70.8 W h kg^(-1)at a power density of 328.1 W kg^(-1),showcasing an impressive long-term cyclic life of 20,000 *** study provides valuable insights for the development of high-performance aqueous secondary batteries.

关键词： Molybdenum trioxide Oxygen deficiency TiO_(2)coating Compatibility Bromine-based battery

Enhanced hydrogen evolution reaction in FePt film with remanence due to decrease in domain walls

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Rare Metals 2024年第3期43卷 1108-1115页

作者： Hong Hong Dong-Xue Liu Jun Li Jun-Ming Li Li-Qian Wu Bo Yang Qing-Qi Cao Dun-Hui Wang National laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced MicrostructuresJiangsu Provincial Key Laboratory for NanotechnologySchool of PhysicsNanjing UniversityNanjing210093China Hangzhou Dianzi University Hangzhou310018China key laboratory for Anisotropy and Texture of Materials(Ministry of Education) School of Material Science and EngineeringNortheastern UniversityShenyang110819China

As an effective strategy to improve the properties of electrocatalysts,magnetic field-assisted electrocatalytic water splitting has attracted increasing attention ***,the corresponding enhancements mostly depend on the exertion of an external magnetic field during electrochemical reactions,which results in a high cost of industrial production,and makes the magnetic field manipulation of electrocatalysis become a challenging *** this work,instead of the external magnetic field,a bias magnetic field is self-supplied by the remanence state of a ferromagnetic electrocatalyst of *** to the assistance of this bias magnetic field,the FePt film in the remanence state shows the overpotential of 229 mV during hydrogen evolution reaction,which is much lower than that in its demagnetization state(283 mV).Our findings demonstrate that the remanence in ferromagnetic electrocatalysts can improve the catalytic performance,which is attributed to the decrease in domain walls.

关键词： Remanence Magnetic domains Electrocatalysis Hydrogen evolution reaction(HER)

Synthesis and characterization of iron clusters with an icosahedral [Fe@Fe12]16+ Core

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National Science Review 2024年第4期11卷 123-129页

作者： Gan Xu Yun-Shu Cui Xue-Lian Jiang Cong-Qiao Xu Jun Li Xu-Dong Chen jiangsu Collaborative Innovation Center of Biomedical Functional Materials and jiangsu key laboratory of New Power Batteries School of Chemistry and Materials Science Nanjing Normal University Department of Chemistry and Guangdong provincial key laboratory of Catalytic Chemistry Southern University of Science and Technology Department of Chemistry and Engineering Research Center of advanced Rare-Earth Materials of Ministry of Education Tsinghua University State key laboratory of Coordination Chemistry Nanjing University

Iron-metal clusters are crucial in a variety of critical biological and material systems,including metalloenzymes,catalysts,and magnetic storage ***,a synthetic high-nuclear iron cluster has been absent due to the extreme difficulty in stabilizing species with direct iron-iron *** this work,we have synthesized,crystallized,and characterized a（Tp*）4W4S12(Fe@Fe12) cluster(Tp*=tris（3,5-dimethyl-1-pyrazolyl）borate（1-）),which features a rare trideca-nuclear,icosahedral[Fe@Fe12] cluster core with direct multicenter iron-iron bonding between the interstitial iron（Fei） and peripheral irons（Fep）,as well as Fep…Fepferromagnetic *** chemistry studies reveal that the stability of the cluster arises from the 18-electron shell-closing of the [Fe@Fe12]16+core,assisted by its bonding interactions with the peripheral tridentate [（Tp*）WS3]4-ligands which possess both S→Fe donation and spin-polarized Fe-Wσ *** ground-state electron spin is theoretically predicted to be S=32/2 for the *** existence of low oxidation-state（OS～+1.23） iron in this compound may find interesting applications in magnetic storage,spintronics,redox chemistry,and cluster catalysis.

关键词： Fe13 cluster iron-sulfur cluster low-valence iron iron−iron bond high spin complex

Subnanometric bimetallic Pt-Pd clusters in zeolites for efficient hydrogen production and selective tandem hydrogenation of nitroarenes

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Science China Chemistry 2024年第9期67卷 2911-2917页

作者： Jiafu Li Tao Cai Yanran Feng Xia Liu Ning Wang Qiming Sun Institute of Sustainable Energy and Resources College of Chemistry and Chemical EngineeringKey Laboratory of Shandong Provincial Universities for Functional Molecules and MaterialsQingdao UniversityQingdao 266071China Innovation Center for Chemical Sciences College of ChemistryChemical Engineering and Materials ScienceJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China

The solvolysis of ammonia borane(AB)and the hydrogenation of nitroarenes represent significant reactions for hydrogen generation and value-added chemical *** strategic engineering of the catalysts is imperative for surmounting obstacles associated with their stability and catalytic *** this work,subnanometric bimetallic Pt–Pd clusters were encapsulated within silicalite-1(S-1)zeolites through a ligand-protected in-situ hydrothermal synthesis *** synergetic effect of bimetallic composition and zeolite confinement markedly enhances the catalytic performance of representative Pt_(0.5)Pd_(0.5)@S-1-H catalyst,affording exceptional turnover frequency(TOF)values of 1,043 and 573 mol_(H_(2))mol_(metal)^(-1)min^(-1)for AB hydrolysis and methanolysis at ambient conditions,respectively,surpassing most of the state-of-the-art Pt-based *** and isotopic experiments reveal that the bimetallic catalytic system remarkably boosts the O-H cleavage of water,thereby facilitating the H_(2) production from AB ***,a conspicuous synergistic effect is demonstrated in the shape-selective tandem hydrogenation of nitroarenes,with the bimetallic catalyst facilitating both AB hydrolysis and nitroarene hydrogenation,giving a high TOF value of 1,260 h^(-1)under atmospheric *** study not only demonstrates the effectiveness of bimetallic nanocatalysts encapsulated in zeolites for hydrogen production from chemical hydrogen storage materials,but also paves the way for the design of catalysts with multifunctional active sites capable of synergistically promoting tandem catalytic processes.

关键词： subnanometer bimetallic cluster zeolite synergistic effect ammonia borane solvolysis selective tandem hydrogenation