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Confinement of ionomer for electrocatalytic CO2 reduction reaction via efficient mass transfer pathways

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national Science Review 2024年第2期11卷 168-176页

作者： Xiaowei Du Peng Zhang Gong Zhang Hui Gao Lili Zhang Mengmeng Zhang Tuo Wang Jinlong Gong school of Chemical Engineering and Technology Key Laboratory for Green Chemical Technology of the Ministry of Education Tianjin University Collaborative Innovation Center of Chemical Science and Engineering(tianjin) national Industry-Education Platform of Energy Storage Tianjin University joint school of the national university of singapore and tianjin university International Campus of Tianjin University Haihe Laboratory of Sustainable Chemical Transformations

Gas diffusion electrodes（GDEs） mediate the transport of reactants, products and electrons for the electrocatalytic CO2reduction reaction（CO2RR） in membrane electrode assemblies. The random distribution of ionomer, added by the traditional physical mixing method, in the catalyst layer of GDEs affects the transport of ions and CO2. Such a phenomenon results in elevated cell voltage and decaying selectivity at high current densities. This paper describes a pre-confinement method to construct GDEs with homogeneously distributed ionomer, which enhances mass transfer locally at the active centers. The optimized GDE exhibited comparatively low cell voltages and high CO Faradaic efficiencies（FE > 90%） at a wide range of current densities. It can also operate stably for over 220 h with the cell voltage staying almost unchanged. This good performance can be preserved even with diluted CO2feeds, which is essential for pursuing a high single-pass conversion rate. This study provides a new approach to building efficient mass transfer pathways for ions and reactants in GDEs to promote the electrocatalytic CO2RR for practical applications.

关键词： CO2 electroreduction gas diffusion electrode mass transfer ionomer Ag catalyst

Mg-doped,carbon-coated,and prelithiated SiO_(x) as anode materials with improved initial Coulombic efficiency for lithium-ion batteries

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Carbon Energy 2024年第3期6卷 204-214页

作者： Bin Liu Jie Liu Cheng Zhong Wenbin Hu Key Laboratory of Advanced Ceramics and Machining Technology(Ministry of Education) School of Materials Science and EngineeringTianjin UniversityTianjinChina tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and EngineeringTianjin UniversityTianjinChina joint school of national university of singapore and tianjin university TianjinChina International Campus of tianjin university Binhai New CityFuzhouChina

Silicon suboxide(SiO_(x),x≈1)is promising in serving as an anode material for lithium-ion batteries with high capacity,but it has a low initial Coulombic efficiency(ICE)due to the irreversible formation of lithium silicates during the first cycle.In this work,we modify SiO_(x) by solid-phase Mg doping reaction using low-cost Mg powder as a reducing agent.We show that Mg reduces SiO_(2) in SiO_(x) to Si and forms MgSiO_(3) or Mg_(2)SiO_(4).The MgSiO_(3) or Mg_(2)SiO_(4) are mainly distributed on the surface of SiO_(x),which suppresses the irreversible lithium-ion loss and enhances the ICE of SiO_(x).However,the formation of MgSiO_(3) or Mg_(2)SiO_(4) also sacrifices the capacity of SiO_(x).Therefore,by controlling the reaction process between Mg and SiO_(x),we can tune the phase composition,proportion,and morphology of the Mg-doped SiO_(x) and manipulate the performance.We obtain samples with a capacity of 1226 mAh g^(–1) and an ICE of 84.12%,which show significant improvement over carbon-coated SiO_(x) without Mg doping.By the synergistical modification of both Mg doping and prelithiation,the capacity of SiO_(x) is further increased to 1477 mAh g^(–1) with a minimal compromise in the ICE(83.77%).

关键词： initial Coulombic efficiency lithium-ion batteries magnesium doping prelithiation silicon suboxide

Bilayer separator enabling dendrite-free zinc anode with ultralong lifespan >5000 h

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Green Energy & Environment 2024年第4期9卷 771-776页

作者： Lu Wang Feifei Wang Zhe Ding Yingxin Liu Ziyi Zhang Chunpeng Yang Kian Ping Loh Quan-Hong Yang joint school of national university of singapore and tianjin university International Campus of Tianjin UniversityFuzhou350207China Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192China Department of Chemistry National University of Singapore117543Singapore Institute of Process Engineering Chinese Academy of SciencesBeijing100190China

Aqueous zinc(Zn)batteries with Zn metal anodes are promising clean energy storage devices with intrinsic safety and low cost.However,Zn dendrite growth severely restricts the use of Zn anodes.To effectively suppress Zn dendrite growth,we propose a bilayer separator consisting of commercial butter paper and glassfiber membrane.The dense cellulose-based butter paper(BP)with low zincophilicity and high mechanical properties prevents the pore-filling behavior of deposited Zn and related separator piercing,effectively suppressing the Zn dendrite growth.As a result,the bilayer separators endow the ZnjjZn symmetrical batteries with a superlong cycling life of Zn anodes(over 5000 h)at 0.5 mA cm^(-2) and the full batteries enhanced capacity retention,demonstrating the advancement of the bilayer separator to afford excellent cyclability of aqueous metal batteries.

关键词： Zn battery Bilayer separator Butter paper Zn metal anode Zn dendrite

Enabling an Inorganic-Rich Interface via Cationic Surfactant for High-Performance Lithium Metal Batteries

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Nano-Micro Letters 2024年第8期16卷 1-17页

作者： Zejun Sun Jinlin Yang Hongfei Xu Chonglai Jiang Yuxiang Niu Xu Lian Yuan Liu Ruiqi Su Dayu Liu Yu Long Meng Wang Jingyu Mao Haotian Yang Baihua Cui Yukun Xiao Ganwen Chen Qi Zhang Zhenxiang Xing Jisheng Pan Gang Wu Wei Chen Department of Chemistry National University of Singapore3 Science Drive 3Singapore 117543Singapore Agency for Science Technology and Research(A*STAR)Institute of High-Performance Computing1 Fusionopolis Way#16‑16 ConnexisSingapore 138632Singapore Department of Physics National University of Singapore2 Science Drive 3Singapore 117542Singapore joint school of national university of singapore and tianjin university International Campus of Tianjin UniversityBinhai New CityFuzhou 350207People’s Republic of China Agency for Science Technologyand Research(A*STAR)Institute of Materials Research and EngineeringInnovis2 Fusionopolis Way#08‑03Singapore 138634Singapore

An anion-rich electric double layer(EDL)region is favorable for fabricating an inorganic-rich solid-electrolyte interphase(SEI)towards stable lithium metal anode in ester electrolyte.Herein,cetyltrimethylammonium bromide(CTAB),a cationic surfactant,is adopted to draw more anions into EDL by ionic interactions that shield the repelling force on anions during lithium plating.In situ electrochemical surface-enhanced Raman spectroscopy results combined with molecular dynamics simulations validate the enrichment of NO_(3)^(−)/FSI−anions in the EDL region due to the positively charged CTA^(+).In-depth analysis of SEI structure by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results confirmed the formation of the inorganic-rich SEI,which helps improve the kinetics of Li^(+)transfer,lower the charge transfer activation energy,and homogenize Li deposition.As a result,the Li||Li symmetric cell in the designed electrolyte displays a prolongated cycling time from 500 to 1300 h compared to that in the blank electrolyte at 0.5 mA cm^(-2) with a capacity of 1 mAh cm^(-2).Moreover,Li||LiFePO_(4) and Li||LiCoO_(2) with a high cathode mass loading of>10 mg cm^(-2) can be stably cycled over 180 cycles.

关键词： Cationic surfactant Lithium nitrate additive Solid-electrolyte interphase Electric double layer Lithium metal batteries

High-entropy oxide-supported platinum nanoparticles for efficient hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1537-1546页

作者： Ming-Yu Fan Jia-Jun Wang Jun Zhao Hong Zhang Tian-Yi Ma Xiao-Peng Han Wen-Bin Hu school of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional Materials Key Laboratory of Advanced Ceramics and Machining Technology Tianjin University school of national university of singapore and tianjin university International Campus of Tianjin University school of Science RMIT University

High-entropy oxides（HEOs） are a new class of single-phase structures with unique electronic and catalytic properties;therefore,it is worthwhile to explore their applications in electrocatalysis.In this study,a Pt/（FeCoNiCrAl）3O4nanohybrid using HEO as a support was developed as an efficient catalyst for the hydrogen evolution reaction（HER）.Pt/（FeCoNiCrAl）3O4exhibited high HER activity with a low overpotential of 22 mV at10 mA·cm-2,outperforming other binary,ternary,and quaternary supports.The HER activity of Pt/（FeCoNiCrAl）3O4was higher than that of a commercial Pt/C with a significantly lower Pt loading.The catalyst exhibited good activity and long-term stability（60 h） in an electrolytic water-splitting device.This good activity can be attributed to the fact that the introduction of Pt effectively facilitates electronic interactions between Pt and the HEO.In addition,the HEO substrate was more favorable for dispersing Pt particles,optimizing the electrochemical specific surface area,and significantly reducing the charge resistance of the HER.This study extends the application of HEOs in electrocatalysis and demonstrates the promising prospects of HEOs as supports for electrocatalysts.

关键词： High-entropy oxides Hydrogen evolution reaction Nanohybrid Water electrolysis

The synthesis of fluorescent nanoclusters based on the etching reaction

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Nano Research 2024年第5期17卷 4631-4638页

作者： Hongbin Lin Yitao Cao Qiaofeng Yao Tiankai Chen Huiting Shan Jianping Xie joint school of national university of singapore and tianjin university International Campus of Tianjin UniversityFuzhou 350207China Department of Chemical and Biomolecular Engineering National University of SingaporeSingapore 117585Singapore national and Local joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)and Key Laboratory of ETESPG(GHEI)South China Normal UniversityGuangzhou 510006China tianjin Key Laboratory of Molecular Optoelectronic Sciences Key Laboratory of Integrated Organic CircuitsMinistry of EducationDepartment of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China

Thiolate-protected atomically precise nanoclusters(NCs)demonstrate a series of unique luminescent characteristics attributed to their various peculiar electronic structures.Therefore,fluorescent NCs present extraordinary practical values in biosensing and bioimaging research fields.Nevertheless,restricted by the types of fluorescent NCs,there are great difficulties in promoting the development of NCs in fluorescent research areas.As a result,it is of significant necessity for researchers to develop new synthetic pathways to produce high-quality fluorescent NCs.According to the analysis about the structural characteristics of fluorescent NCs,some general features like longer motif and higher ligand-to-metal ratio can be found,consistent to some presented regularities in etching reaction.Consequently,in this work,we used Au_(25)(MHA)_(18)(MHA=6-mercaptohexanoic acid)as a model nanocluster and utilized the etching reaction to systematically explore etching products and their corresponding luminescent properties.Moreover,we also identified three main reaction processes in the entire etching reaction process,which can generate new metal nanocluster species with various fluorescent properties.Hence,the etching reaction will provide a good platform to produce new luminescent metal NC species.

关键词： etching reaction metal nanoclusters fluorescent properties fluorescent conversion

Sparse Reconstructive Evidential Clustering for Multi-View Data

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IEEE/CAA Journal of Automatica Sinica 2024年第2期11卷 459-473页

作者： Chaoyu Gong Yang You school of Computing National University of SingaporeSingapore

Although many multi-view clustering(MVC) algorithms with acceptable performances have been presented, to the best of our knowledge, nearly all of them need to be fed with the correct number of clusters. In addition, these existing algorithms create only the hard and fuzzy partitions for multi-view objects,which are often located in highly-overlapping areas of multi-view feature space. The adoption of hard and fuzzy partition ignores the ambiguity and uncertainty in the assignment of objects, likely leading to performance degradation. To address these issues, we propose a novel sparse reconstructive multi-view evidential clustering algorithm(SRMVEC). Based on a sparse reconstructive procedure, SRMVEC learns a shared affinity matrix across views, and maps multi-view objects to a 2-dimensional humanreadable chart by calculating 2 newly defined mathematical metrics for each object. From this chart, users can detect the number of clusters and select several objects existing in the dataset as cluster centers. Then, SRMVEC derives a credal partition under the framework of evidence theory, improving the fault tolerance of clustering. Ablation studies show the benefits of adopting the sparse reconstructive procedure and evidence theory. Besides,SRMVEC delivers effectiveness on benchmark datasets by outperforming some state-of-the-art methods.

关键词： Evidence theory multi-view clustering(MVC) optimization sparse reconstruction

Recent advances in fabrication and functions of neuromorphic system based on organic field effect transistor

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International Journal of Extreme Manufacturing 2024年第2期6卷 273-295页

作者： Yaqian Liu Minrui Lian Wei Chen Huipeng Chen school of Physics and Electronic Engineering Zhengzhou University of Light IndustryHenan 450002People’s Republic of China Institute of Optoelectronic Display National&Local United Engineering Lab of Flat Panel Display TechnologyFuzhou UniversityFuzhou 350002People’s Republic of China joint school of national university of singapore and tianjin university International Campus of Tianjin UniversityFuzhou 350207People’s Republic of China Department of Chemistry National University of Singapore3 Science Drive 3Singapore 117543Singapore Department of Physics National University of Singapore3 Science Drive 3Singapore 117543Singapore

The development of various artificial electronics and machines would explosively increase the amount of information and data,which need to be processed via in-situ remediation.Bioinspired synapse devices can store and process signals in a parallel way,thus improving fault tolerance and decreasing the power consumption of artificial systems.The organic field effect transistor(OFET)is a promising component for bioinspired neuromorphic systems because it is suitable for large-scale integrated circuits and flexible devices.In this review,the organic semiconductor materials,structures and fabrication,and different artificial sensory perception systems functions based on neuromorphic OFET devices are summarized.Subsequently,a summary and challenges of neuromorphic OFET devices are provided.This review presents a detailed introduction to the recent progress of neuromorphic OFET devices from semiconductor materials to perception systems,which would serve as a reference for the development of neuromorphic systems in future bioinspired electronics.

关键词： organic field effect transistor neuromorphic systems synaptic transistor sensory perception systems device fabrication

Research Progress in the Fabrication of Covalent Organic Framework Membranes for Chemical Separations

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Chinese Journal of Polymer Science 2024年第2期42卷 141-158,I0005页

作者： Cui-Ting Ding Jin-Qiu Yuan Meng-Ying Xie Qing-Yuan Liu Zeng-Guang Yao Shi-Yu Zhang Run-Nan Zhang Hong Wu Zhong-Yi Jiang Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China Zhejiang Institute of tianjin university NingboZhejiang315201China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192China tianjin Key Laboratory of Membrane Science and Desalination Technology Tianjin UniversityTianjin300072China joint school of national university of singapore and tianjin university International Campus of Tianjin UniversityBinhai New CityFuzhou350207China

Membrane technology has become one of the most promising separation technologies for its energy saving, high separation efficiency, environmental friendliness, and economic feasibility. Covalent organic frameworks(COFs) with intrinsically high porosity, controllable pore size, uniform pore size distribution and long-range ordered channel structure, have emerged as next-generation materials to fabricate advanced separation membranes. This feature article summarizes some latest studies in the development of pure COF membranes in our lab, including their fabrication and applications in chemical separations. Finally, current challenges facing high-performance COF separation membranes are discussed.

关键词： Covalent organic frameworks Covalent organic framework membranes Water treatment Organic solvent nanofiltration Gas separation