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Chinese Journal of chemistry 2024年第11期42卷 1217-1222页

作者： Xianjing Xie Yirong Zhang Junrui Zhang Xingyuan Cui Wei Liu Xunshan Liu key laboratory of surface&interface Science of Polymer Materials of Zhejiang province School of Chemistry and Chemical EngineeringZhejiang Sci-Tech University928 Second StreetHangzhouZhejiang310018 China State key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchunJilin130022 China School of Materials Science and Engineering Nanjing University of Science and TechnologyNanjingJiangsu210094 China

Investigating the quantum interference effect in single molecules is essential to comprehensively understand the underlying mechanism of single-molecule charge *** this study,we employed the mother molecule m-OPE and introduced a series of side groups with various electronic effects at the 2-position of the central phenyl ring,creating four daughter m-OPE *** single molecular conductivities of these molecule wires were measured using the scanning tunneling microscope breaking junction *** findings demonstrate that the substitutions regularly modulate the destructive quantum interference occurring within the m-OPE *** combining optical and electrochemical investigations,along with density functional theory computations,we discover that the conductivity of the molecules corresponds to the electron-donating/withdrawing ability of the ***,by adjusting the electron structures of the molecular backbone,we can systematically tailor the destructive quantum interference in the m-OPE molecules.

关键词： Quantum interference Single-molecule junctions Electron effect substituents Charge transport Molecular devices

Molecule aging induced by electron attacking

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Journal of Energy chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu State key laboratory of Electroanalytical chemistry and jilin province key laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai key laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C *** density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water *** results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction

Organic interfacial engineering of gold nanowires for selective glycerol electrooxidation

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Chinese Chemical Letters 2024年第3期35卷 502-507页

作者： Zhe Wang Qingling Hong Boqiang Miao Tianjiao Wang Yu Ding Pujun Jin Pei Chen Yu Chen key laboratory of Macromolecular Science of Shaanxi province Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education)Shaanxi Key Laboratory for Advanced Energy DevicesSchool of Materials Science and EngineeringShaanxi Normal UniversityXi'an 710062China

The selective electrochemical conversion of glycerol into value-added products is a green and sustainable strategy for the biomass *** this work,Au nanowires(Au-NW)modified with polyethyleneimine(PEI)molecule(Au-NW@PEI)is obtained by an up-bottom post-modification *** characterization,molecular dynamics simulation and density functional theory demonstrate that the loose-packed PEI monolayer firmly and uniformly distribute on the Au-NW surface due to the strong Au-N *** experiments and product analysis display that PEI modification significantly enhance the electro-activity of Au-NW for the glycerol electro-oxidation reaction(GEOR)due to the electronic ***,the steric hindrance and electrostatic effect of PEI layer make the optimizing adsorption of intermediates ***,the selectivity of C3 product glyceric acid over Au-NW@PEI is increased by nearly 20%.The work thus indicates that the rational design of metal-organic interface can effectively elevate the electro-activity and selectivity of Au nanostructures,which may have wide application in biomass development.

关键词： Glycerol electrooxidation reaction Organic interface engineering Gold-based nanomaterials Electrocatalysis Selectivity

Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li Meiling Xiao Changpeng Liu Wei Xing State key laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor *** the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient ***,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)*** lattice disorder in HEOs is believed to increase migration energy barrier of lattice *** a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) *** work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction

surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan Institute of Physical chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of jilin University Changchun 130021China State key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow ***,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater *** 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 ***-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

Dimensional reduction enhances photocatalytic carbon dioxide reduction performance of metal-organic frameworks

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Nano Research 2024年第5期17卷 3653-3659页

作者： Kaiyue Ma Jixin Li Jinlu Liu Chunguang Li Zhan Shi Shouhua Feng State key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Metal-organic frameworks(MOFs)have shown significant potential as *** has been widely assumed that all catalytic active sites within MOFs are functional in photocatalytic reactions but for a three-dimensional MOF,whether the internal catalytic active sites can effectively absorb light and actively contribute to photocatalytic reactions remains to be *** this context,we synthesized a two-dimensional nanosheet MOF(2D-MOF)and a three-dimensional bulk MOF(3D-MOF)composed of Zr^(6) clusters and tetracarboxylic porphyrin(TCPP)by the approach described in the ***(bpy)(CO)^(3)Cl(bpy=2,2’-bipyridine),which has remarkable CO_(2) photoreduction ability,was introduced to the two MOFs to create two new photocatalysts 2D-MOF-Re and 3D-MOF-Re,*** CO_(2) reduction experiments show that based on the equal number of catalytic active sites,the CO turnover number(TON)of 2D-MOF-Re reaches 27.8 in 6 h,which is 50 times that of *** result shows that certain catalytic active sites inside the bulk MOF are inactive due to the inability to absorb *** study illuminates the potential of the dimensional reduction approach in the design of photocatalysts to exploit the capabilities fully.

关键词： photocatalysis CO_(2)reduction metal-organic frameworks(MOFs) nanosheets light absorption

Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Nano Research 2024年第3期17卷 1199-1208页

作者： Huafeng Fan Dongxu Jiao Jinchang Fan Dewen Wang Bilal Zaman Wei Zhang Lei Zhang Weitao Zheng Xiaoqiang Cui State key laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterJilin UniversityChangchun 130012China College of chemistry Jilin UniversityChangchun 130012China

Designing high-performance electrocatalysts toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to reduce the activation barrier and optimize free adsorption energy of reactive ***,we report that incorporating high-valence Cr into NiSe_(2)(Cr_(x)Ni_(1-x)Se_(2))kinetically and thermodynamically expedites elementary steps of both HER and *** as-prepared Cr_(0.05)Ni_(0.95)Se_(2) catalyst displays excellent HER and OER activities,with low overpotentials of 89 and 272 mV at the current density of 10 mA·cm^(-2)(j10),respectively,and remains stable during operation for 30 h.A low cell voltage of only 1.59 V is required to drive j10 in alkaline *** situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER ***,theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H*adsorption during HER process,lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate,thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe_(2) for over water *** strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

关键词： nickel selenide electrocatalytic water splitting high-valence Cr density functional theory(DFT)calculation

Ligand-controlled electrochemiluminescence generation from CdSe/CdS/ZnS core/shell/shell quantum dots

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Nano Research 2024年第8期17卷 7776-7785页

作者： Hui Sun Zhiyuan Cao Haiyan Qin Xiaogang Peng Bin Su key laboratory of Excited-State Materials of Zhejiang province Department of ChemistryZhejiang UniversityHangzhou 310058China

The CdSe/CdS/ZnS core/shell/shell quantum dots(QDs)with strong exciton confinement have manifested themselves as competitive light-emitting materials in electrochemiluminescence(ECL).However,cathodic ECL generation by these QDs requires the injection of electron and hole from solid electrode and electrogenerated radicals(for example SO_(4)•^(−)),which is inevitably influenced by not only the inorganic structure of QDs but also the organic ligands on the *** this work we aimed at studying the impact of surface organic ligands on ECL performance of CdSe/CdS/ZnS *** changing the surface ligand from oleate to acetate,we phenomenologically observed the positive shift of ECL onset potential by ca.200 mV and the increase of ECL intensity by~100 times,suggesting that a short ligand is more favorable for ECL *** further comprehend the ligand effect,we measured the charge injection kinetics using potential-modulated,time-resolved photoluminescence,and thinlayer spectroelectrochemistry *** electron and hole injection into QDs were found to be accelerated by 2–20 times if shortening the ligand from oleate to acetate,confirming the significant impact of surface ligands on ECL performance of *** study is expected to provide guidance on how to design surface functionalized QDs for specific applications such as ECL immunodiagnosis,photocatalysis,and photovoltaics.

关键词： electrochemiluminescence quantum dots spectroelectrochemistry surface ligands charge injection charge transfer

Stabilizing high-efficiency iridium single atoms via lattice confinement for acidic oxygen evolution

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Nano Research 2024年第4期17卷 2492-2498页

作者： Yibo Wang Jiadong Jiang Zhaoping Shi Hongxiang Wu Jiahao Yang Pengbo Wang Shuai Hou Meiling Xiao Junjie Ge Changpeng Liu Wei Xing laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026.China State key laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China jilin province key laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China key laboratory of Physics and Technology for Advanced Batteries Ministry of EducationCollege of PhysicsJilin UniversityChangchun 130012China

Stable and efficient single atom catalysts(SACs)are highly desirable yet challenging in catalyzing acidic oxygen evolution reaction(OER).Herein,we report a novel iridium single atom catalyst structure,with atomic Ir doped in tetragonal PdO matrix(IrSAs-PdO)via a lattice-confined *** optimized IrSAs-PdO-0.10 exhibited remarkable OER activity with an overpotential of 277 mV at 10 mA·cm^(-2) and long-term stability of 1000 h in 0.5 M H_(2)SO_(4).Furthermore,the turnover frequency attains 1.6 s^(-1) at an overpotential of 300 mV with a 24-fold increase in the intrinsic *** high activity originates from isolated iridium sites with low valence states and decreased Ir–O bonding covalency,and the excellent stability is a result of the effective confinement of iridium sites by Ir–O–Pd ***,we demonstrated for the first time that SACs have great potential in realizing ultralow loading of iridium(as low as microgram per square center meter level)in a practical water electrolyzer.

关键词： lattice confinement iridium single atoms ultralow iridium loading acidic oxygen evolution proton exchange membrane water electrolysis

Mechanism of interfacial effects in sodium-ion storage devices

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Nano Research 2024年第3期17卷 1313-1326页

作者： Yifan Wei Lingxing Zan Huicong Xia Wenfu Yan Jia-Nan Zhang College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China key laboratory of Advanced Energy Catalytic and Functional Material Preparation of Zhengzhou City Zhengzhou 450001China key laboratory of Chemical Reaction Engineering of Shaanxi province College of Chemistry&Chemical EngineeringYan’an UniversityYan’an 716000China State key laboratory of Inorganic Synthesis and Preparative chemistry and College of chemistry Jilin UniversityChangchun 130012China

Rechargeable sodium-ion batteries(SIBs)are considered as the next-generation secondary *** performance of SIB is determined by the behavior of its electrode surface and the electrode–electrolyte interface during charging and ***,the characteristics of these surfaces and interfaces should be analyzed to realize large-scale energy storage systems with high energy density and long-cycle *** various studies have investigated the properties of electrode materials,few studies have focused on the construction of stable and efficient SIB interfaces,and even fewer have explored the mechanisms of interfacial effects;however,the strategies of regulating interfacial effects are yet to be completely ***,the results obtained thus far are insufficient to draw systematic *** present study reviews the literature on the mechanism of interfacial effects in Na+storage *** interfaces in a sodium-ion storage device include a heterogeneous interface between electrode materials,a solid electrolyte interphase,and a cathode electrolyte *** interfacial effects during the intercalation,transformation,and alloy reactions and the resulting overall battery performance were theoretically *** this review,we aim to provide a theoretical basis for optimizing the structures of electrode surface and electrode–electrolyte interface to optimize the performance of *** addition,the challenges of investigating interfacial effects and several possible helpful methods and opportunities for studying the mechanisms of interfacial effects in SIBs will be presented.

关键词： sodium-ion storage interfacial effects solid electrolyte interphase cathode electrolyte interphase