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Insight into the Role of Isolated Gold Atoms-Ceria Conjunction in Catalyzing the Water-Gas Shift Reaction

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Chinese Journal of Chemistry 2024年第6期42卷 636-644页

作者： Xin-Pu Fu Hui-Zhao Wei-Wei Wang Chun-Jiang Jia Key laboratory for colloid and interface Chemistry Key Laboratory of Special Aggregated MaterialsSchool of Chemistry and Chemical EngineeringShandong UniversityJinanShandong250100 China

As the promising catalysts for the water-gas shift(WGS)reaction,the activity of Au-CeO_(2) composites is susceptible to the aggregation size and electronic state of Au *** reports were extensively focused on the discrepancy between nonmetallic Au and metallic Au nanoparticles,whereas the understanding of the authentic role of the isolated Au atoms was ***,we investigated the catalytic behavior and structural information over two types of Au/CeO_(2) catalysts,in which the predominant conjunctions were isolated Au1-CeO_(2) and Aun-CeO_(2),*** on comprehensive characterizations,particularly by in-situ Raman and in-situ DRIFTS,we found that the isolated Au atoms were responsible for enhancing the reducibility of the CeO_(2) *** CO adsorption ability on the isolated Au sites was significantly inferior to clustered Au atoms,especially at relatively high temperatures(>200°C).As a result,the boosted O vacancy on the isolated Au1-CeO_(2) conjunctions could improve the H2O activation ability for the Au-CeO_(2) catalysts and demonstrate a comparable activity to the clustered Aun-CeO_(2) *** work might deepen understanding of the catalytic function for the isolated Au1 site within Au/CeO_(2) systems while catalyzing the WGS reaction.

关键词： Isolated Au atoms Ceria-based catalysts Water-gas shift reaction Defect Adsorption

Molecular template derived ultrathin N-doped carbon layer on cobalt selenide nanobelts for durable and rapid sodium storage

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Nano Research 2024年第9期17卷 8145-8154页

作者： Chuanliang Wei Baojuan Xi Kangdong Tian Xinlu Zhang Quanyan Man Keyan Bao Wutao Mao Jinkui Feng Shenglin Xiong Key laboratory of the colloid and interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringSchool of Materials Science and EngineeringShandong UniversityJinan 250100China Resource Environment and Clean Energy laboratory School of Chemical and Environmental EngineeringJiangsu University of TechnologyChangzhou 213001China

Sodium-ion batteries(SIBs)are an attractive battery system because of similar characteristics to lithium-ion batteries(LIBs)and large Na element ***,exploring stable,high-capacity and high-rate anode materials for SIBs is still challenging ***,diethylenetriamine(DETA)molecular template derived ultrathin N-doped carbon(NC)layer decorated CoSe_(2)nanobelts(CoSe_(2)/NC)are prepared by solvothermal reaction followed by calcination *** CoSe_(2)/NC exhibits large potential as an anode for *** and theoretical calculations reveal that the in situ formed conductive ultrathin NC layer can not only relieve the volume change of CoSe_(2)but also accelerate electron and ion *** addition,the nanobelt structure of CoSe_(2)/NC with abundant exposed active sites can obviously accelerate the electrochemical *** the synergistic effect of special nanobelt structure and NC layer,the rate as well as cycling performances of CoSe_(2)/NC are obviously improved.A superior capacity retention of 94.8%is achieved at 2 A·g^(-1)after 2000 *** using Na3V2(PO4)3 cathodes,the pouch full batteries can work steadily at 0.5 C,verifying the application ***_(2)/NC anodes also exhibit impressive performances in LIBs and potassium-ion batteries(PIBs).

关键词： CoSe2 nanobelts ultrathin N-doped carbon layer sodium-ion batteries anode high rate

Evolution of template-assisted two-dimensional porphyrin chiral grating structure by directed self-assembly using chiral second harmonic generation microscopy

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Chinese Chemical Letters 2024年第10期35卷 196-200页

作者： Changhui Yu Peng Shang Huihui Hu Yuening Zhang Xujin Qin Linyu Han Caihe Liu Xiaohan Liu Minghua Liu Yuan Guo Zhen Zhang Beijing National laboratory for Molecular Sciences State Key Laboratory of Molecular Reaction Dynamics Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences Beijing National laboratory for Molecular Science CAS Key Laboratory of Colloid Interface and Chemical Thermodynamics Institute of Chemistry Chinese Academy of Sciences

Directed self-assembly has been used to create micro-nano scale patterns, including chiral periodic structures of organic molecules, for potential applications in optics, photonics, metamaterials, and medical and sensing technologies. This study presents a straightforward approach for fabricating large-scale chiral grating porphyrin assemblies through template-assisted techniques. The solution of tetrakis(4-sulfonatophenyl)porphyrin(TPPS) was induced by chiral amino acids(L/D-arginine and L/D-serine) to selfassemble into highly ordered chiral grating structures with the assistance of sodium dodecyl sulfate(SDS).The structures show precise line widths(5.5 μm) and gaps(18 μm). Using in situ optical microscopy and second harmonic generation(SHG) microscopy, the chiral characteristics and dynamic evolution of the template-assisted self-assembly are investigated. It is found that the chirality of amino acids induced TPPS self-assembled into chiral structures and the liquid contraction interface significantly enhanced the chirality of the assemblies. This study is significant for understanding the mechanism of chiral evolution and designing novel micro-nano materials with predetermined chiral properties.

关键词： Chiral assembly Chiral evolution Micro-nano structure Porphyrin Second harmonic generation microscopy Template-assisted self-assembly

Rational cathode configuration with bilayer membranes to engineer current-collector-free high-areal-sulfur lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5224-5232页

作者： Jianmei Han Hua Zhang Peng Wang Ning Song Xuguang An Baojuan Xi Shenglin Xiong College of Chemistry and Chemical Engineering Taishan UniversityTai’an 271021China Key laboratory of the colloid and interface Chemistry Ministry of Educationand School of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China School of Mechanical Engineering Chengdu UniversityChengdu 610106China

The application of light-weight current collectors is preferred because of the increased energy density of the *** it in mind,the cathode is designed with self-made paperlike memberane as current collector coupled with another interlayer to enable the high-energy-density lithium-sulfur *** a facile and green step-by-step methodology,the hybrid membrane is finalized successfully,consisting of reduced graphene oxide sheets covering paper-derived carbon(GPC)bearing Fe@Fe2O3 and Fe1−xS@Fe2O3 core-shell nanoparticles(FeFeO/FeSFeO@GPC).The film works as the current collector and interlayer simultaneously considering the porous and conductive *** demonstrated by the electrochemical testing,the FeFeO/FeSFeO@GPC hybrid cell exhibits attractive cycling stability and superior rate *** cell configuration and structural/composition merits of FeFeO/FeSFeO@GPC film facilitate the faster reaction kinetics,conducive to the improvement of capacity *** view of the effective cathode design,the areal sulfur loading is increased to 10.46 mg·cm^(−2)and a reversible capacity of 6.67 mAh·cm^(−2)can be retained after 60 cycles at 0.1 C.

关键词： light-weight self-made current collector core-shell high-areal-sulfur lithium-sulfur batteries

pH- and near-infrared light-responsive,biomimetic hydrogels from aqueous dispersions of carbon nanotubes

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Nano Research 2024年第4期17卷 3120-3129页

作者： Lulin Hu Xinxin Yu Jingcheng Hao Lu Xu Shandong laboratory of Yantai Advanced Materials and Green Manufacturing Yantai 264000China State Key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Yantai Center for Food and Drug Control Yantai 264000China Key laboratory of colloid and interface Chemistry&Key laboratory of Special Aggregated Materials Shandong UniversityJinan 250100China

Owing to their low flexibility,poor processability and a lack of responsiveness,inorganic materials are usually non-ideal for constructing a living ***,to date,lifelike materials with structural hierarchies and adaptive properties usually rely on light and soft organic molecules,although few exceptions have been acquired using two-dimensional(2D)inorganic ***,with a systematic study on the gelation behavior of carbon-based 0D quantum dots,1D nanotubes,and 3D fullerenes,we find that acidified 1D carbon nanotubes(CNTs)can serve as an alternative building block for fabricating purely inorganic biomimetic soft *** as-prepared CNT gels exhibit not only a pH-or photothermal-triggered mechanical and tribological adaptivity,which allows them to simulate the behavior of sea cucumbers,peacock mantis shrimps,and mammalian muscles or cortical bones,but also a unique damping property that is similar to spider’s cuticular *** high elasticity,effective lubrication,excellent biocompatibility,and controllable friction and wear also allow them to function as a new type of smart lubricants,whose tribological properties can be regulated either by its internal pH changes or spatiotemporally by near-infrared(NIR)light irradiations,free of any toxic and flammable base oils or additives.

关键词： biomimetic hydrogels carbon nanotubes(CNTs) mechanical and tribological adaptivity pH-and near-infrared(NIR)light responsiveness switchable lubrication

Versatile MXene Gels Assisted by Brief and Low‑Strength Centrifugation

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Nano-Micro Letters 2024年第5期16卷 231-247页

作者： Weiyan Yu Yi Yang Yunjing Wang Lulin Hu Jingcheng Hao Lu Xu Weimin Liu State Key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000People’s Republic of China Shandong laboratory of Advanced Materials and Green Manufacturing at Yantai Yantai 264006People’s Republic of China Key laboratory of colloid and interface Chemistry and Key laboratory of Special Aggregated Materials Shandong UniversityJinan 250100People’s Republic of China

Due to the mutual repulsion between their hydrophilic surface terminations and the high surface energy facilitating their ran-dom restacking,2D MXene nanosheets usually cannot self-assemble into 3D macroscopic gels with various applications in the absence of proper linking *** this work,a rapid spontaneous gelation of Ti3C2Tx MXene with a very low dispersion concentration of 0.5 mg mL^(-1) into multifunctional architectures under moderate centrifugation is *** as-prepared MXene gels exhibit reconfigurable internal structures and tunable rheological,tribological,electrochemical,infrared-emissive and photothermal-conversion properties based on the pH-induced changes in the surface chemistry of Ti_(3)C_(2)T_(x) *** adopting a gel with optimized pH value,high lubrication,exceptional specific capacitances(~635 and~408 F g^(-1) at 5 and 100 mV s^(-1),respectively),long-term capacitance retention(~96.7%after 10,000 cycles)and high-precision screen-or extrusion-printing into different high-resolution anticounterfeiting patterns can be achieved,thus displaying extensive potential applications in the fields of semi-solid lubrication,control-lable devices,supercapacitors,information encryption and infrared camouflaging.

关键词： MXene Centrifugation-assisted rapid gelation Lubrication Supercapacitor Anti-counterfeiting applications

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Transient self-assembly driven by chemical fuels

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ChemPhysMater 2024年第1期3卷 1-23页

作者： Ling Wang Jin Yuan Jingcheng Hao Key laboratory of colloid and interface Chemistry Shandong UniversityMinistry of EducationJinan 250100China School of Chemistry and Chemical Engineering Qilu Normal UniversityJinan 250200China

Self-assembly has been extensively studied in chemistry,physics,biology,and materials engineering and has become an important“bottom-up”approach in creating intriguing structures for different *** dissipative self-assembly to construct fuel-dependent,energy-consuming,and dynamic nonequilibrium systems is important for developing intelligent life-like ***,dissipative self-assembly has become a research hotspot in materials chemistry,biomedical science,environmental chemistry,and physical *** in-depth understanding of the process and mechanism provides useful insights to the researchers for devel-oping materials using dissipative self-assembly and also helps guide future innovation in material *** critical review comprehensively analyzes various chemical fuel input and energy consumption mechanisms,supported by numerous illustrative *** transient assemblies,including gels,vesicles,micelles,and nanoparticle aggregates,have been systematically studied in our and other *** relationship between the molecular structure of precursors and temporal assemblies in dissipative self-assemblies is discussed from the perspective of physical *** dissipative self-assembly methods to construct functional assemblies provides important implications for constructing high-energy,nonequilibrium,and intelligent functional materials.

关键词： Self-Assembly Chemical Fuel Consumption mechanisms Functional assemblies

Nitrogen-doping boosts *CO utilization and H2O activation on copper for improving CO2 reduction to C2+ products

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Green Energy & Environment 2024年第9期9卷 1459-1465页

作者： Yisen Yang Zhonghao Tan Jianling Zhang Jie Yang Renjie Zhang Sha Wang Yi Song Zhuizhui Su Beijing National laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences School of Chemical Sciences University of Chinese Academy of Sciences Key laboratory of Photochemistry CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences

To improve the electrocatalytic transformation of carbon dioxide （CO2） to multi-carbon (C2+) products is of great *** we developed a nitrogen-doped Cu catalyst,by which the maximum C2+Faradaic efficiency can reach 72.7%in flow-cell system,with the partial current density reaching 0.62 A *** in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst,thus promoting the*CO utilization in the subsequent C–C coupling ***,the water activation can be well enhanced by N doping on Cu *** to the synergistic effects,the selectivity and activity for C2+products over the N-deoped Cu catalyst are much improved.

关键词： Electrocatalytic CO 2 reduction reaction Copper catalyst Doping Multi-carbon products In situ Raman measurement

Performance optimization of chalcogenide catalytic materials in lithium-sulfur batteries:Structural and electronic engineering

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Chinese Chemical Letters 2024年第7期35卷 147-166页

作者： Jianmei Han Peng Wang Hua Zhang Ning Song Xuguang An Baojuan Xi Shenglin Xiong College of Chemistry and Chemical Engineering Taishan UniversityTai'an 271021China Key laboratory of colloid and interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJi'nan 250100China School of Mechanical Engineering Chengdu UniversityChengdu 610106China

Lithium-sulfur batteries(LSBs)boasting remarkable energy density have garnered significant attention within academic and industrial ***,the progression of LSBs remains constrained by the languid redox kinetics intrinsic to sulfur and the pronounced shuttle effect induced by lithium polysulfides(Li PSs),which seriously affecting the energy density,cycling life and rate *** conceptualization and implementation of catalytic materials stand acknowledged as a propitious stratagem for orchestrating kinetic modulation,particularly in excavating the conversion of LiPSs and has evolved into a focal point for *** them,chalcogenide catalytic materials(CCMs)have shown satisfactory catalytic effects ascribe to the unique physicochemical properties,and have been extensively developed in recent *** the lack of systematic summary regarding the development of CCMs and corresponding performance optimization strategies,herein,we initiate a comprehensive review regarding the recent progress of CCMs for effective collaborative immobilization and accelerated transformation kinetics of Li *** that,the modulation strategies to improve the catalytic activity of CCMs are summarized,including structural engineering(morphology engineering,surface/interface engineering,crystal engineering)and electronic engineering(doping and vacancy,etc.).Finally,the application prospect of CCMs in LSBs is clarified,and some enlightenment is provided for the reasonable design of CCMs serving practical LSBs.

关键词： Lithium-sulfur batteries Chalcogenide Catalytic materials Lithium polysulfides Structural engineering Electronic engineering

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