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Stretchable and self-healing conductive fibers from hierarchical silver nanowires-assembled network

Nano Research 2024年第2期17卷 763-770页

作者： Ying-Ying Wu Hong Chen Fan Zhang Pan Guo Haili Qin Huai-Ping Cong anhui Province key laboratory of advanced catalytic materials and reaction engineering School of Chemistry and Chemical EngineeringHefei University of TechnologyHefei 230009China

Conductive fibers(CFs)with features of high conductivity,stretchability,self-healability,and electromechanical stability are key components of the increasingly popular wearable electronics.However,since the lack of structural design of conductive network and interfacial interaction between soft polymer and conductive additives,it is still hard to enable CFs to meet above requirements.Here,we describe a facial drawing method from a hydrogel reservoir which is remolded into ultrathin and stretchable CFs with excellent multi-responsive self-healability.The hydrogel reservoir was fabricated in synergy of an ice-templating method and in situ polymerization using the assembled framework as a crosslinker.Relying on the effective fabrication mechanism,the diameter of CFs could be well-tuned from 90 to 400μm by adjusting the dipping depth of the glass rod,accompanied with conductivity increased from 0.75 to 2.5 S/m.Since the hierarchical network structure was well maintained in the CFs,professional performances have been proved on the stretchability and electromechanical stability.The presence of massive hydrogen bonding and Ag–S bond enabled the CFs with excellent self-healability under the conditions of contact,electric field,and near infrared light,respectively.Excitingly,the CFs with high sensing property could be integrated into an advanced textile sensor through an effective healing-induced integration strategy,demonstrating its great potentials as superior two-dimensional(2D)electronic skins.

关键词： conductive fibers self-assembled silver nanowires Ag–S coordination self-healing flexible sensors

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Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in Li–S Batteries

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Nano-Micro Letters 2024年第5期16卷 370-383页

作者： Yu Du Weijie Chen Yu Wang Yue Yu Kai Guo Gan Qu Jianan Zhang key laboratory of advanced Energy catalytic and Functional materials Preparation of Zhengzhou City College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001People’s Republic of China

Spin-engineering with electrocatalysts have been exploited to suppress the“shuttle effect”in Li–S batteries.Spin selec-tion,spin-dependent electron mobility and spin potentials in activation barriers can be optimized as quantum spin exchange interactions lead-ing to a significant reduction of the electronic repulsions in the orbitals of catalysts.Herein,we anchor the MgPc molecules on fluorinated carbon nanotubes(MgPc@FCNT),which exhibits the single active Mg sites with axial displacement.According to the density functional theory calculations,the electronic spin polarization in MgPc@FCNT not only increases the adsorption energy toward LiPSs intermediates but also facilitates the tunneling process of electron in Li–S batter-ies.As a result,the MgPc@FCNT provides an initial capacity of 6.1 mAh cm^(-2) even when the high sulfur loading is 4.5 mg cm^(-2),and still maintains 5.1 mAh cm^(-2) after 100 cycles.This work provides a new perspective to extend the main group single-atom catalysts enabling high-performance Li–S batteries.

关键词： Metal phthalocyanines Spin polarization Electrocatalysis Li–S batteries

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Rationally construction of atomic-precise interfacial charge transfer channel and strong build-in electric field in nanocluster-based Zscheme heterojunctions with enhanced photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 5002-5010页

作者： Qingtao Zhu Honglei Shen Chao Han Liu Huang Yanting Zhou Yuanxin Du Xi Kang Manzhou Zhu Department of materials Science and engineering Centre for Atomic Engineering of Advanced MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui UniversityHefei 230601China

The lack of effective charge transfer driving force and channel limits the electron directional migration in nanoclusters(NC)-based heterostructures,resulting in poor photocatalytic performance.Herein,a Z-scheme NC-based heterojunction(Pt1Ag28-BTT/CoP,BTT=1,3,5-benzenetrithiol)with strong internal electric field is constructed via interfacial Co-S bond,which exhibits an absolutely superiority in photocatalytic performance with 24.89 mmol·h^(−1)·g−1 H_(2)production rate,25.77%apparent quantum yield at 420 nm,and~100%activity retention in stability,compared with Pt1Ag28-BDT/CoP(BDT=1,3-benzenedithiol),Ag29-BDT/CoP,and CoP.The enhanced catalytic performance is contributed by the dual modulation strategy of inner core and outer shell of NC,wherein,the center Pt single atom doping regulates the band structure of NC to match well with CoP,builds internal electric field,and then drives photogenerated electrons steering;the accurate surface S modification promotes the formation of Co-S atomic-precise interface channel for further high-efficient Z-scheme charge directional migration.This work opens a new avenue for designing NC-based heterojunction with matchable band structure and valid interfacial charge transfer.

关键词： atomically precise metal nanocluster Z-scheme heterojunction interfacial charge transfer build-in electric field photocatalytic hydrogen production

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Artificial stepwise light harvesting system in water constructed by quadruple hydrogen bonding supramolecular polymeric nanoparticles

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Chinese Chemical Letters 2024年第2期35卷 370-373页

作者： Tangxin Xiao Xiuxiu Li Liangliang Zhang Kai Diao Zheng-Yi Li Xiao-Qiang Sun Leyong Wang Jiangsu key laboratory of advanced catalytic materials and Technology School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Jiangsu key laboratory of advanced Organic materials School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Stepwise energy transfer is ubiquitous in natural photosynthesis,which greatly promotes the widespread use of solar energy.Herein,we constructed a supramolecular light harvesting system based on sequential energy transfer through the hierarchical self-assembly of M,which contains a cyanostilbene core flanked by two ureidopyrimidinone motifs,endowing itself with both aggregation-induced emission behavior and quadruple hydrogen bonding ability.The monomer M can self-assemble into hydrogen bonded polymers and then form supramolecular polymeric nanoparticles in water through a mini-emulsion process.The nanoparticles were further utilized to encapsulate the relay acceptor ESY and the final acceptor NDI to form a two-step FRET system.Tunable fluorescence including a white-light emission was successfully achieved.Our work not only shows a desirable way for the fabrication of efficient two-step light harvesting systems,but also shows great potential in tunable photoluminescent nanomaterials.

关键词： Light harvesting system Supramolecular polymer Quadruple hydrogen bonding AIE Self-assembly

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Boosting electrocatalytic nitrate reduction to ammonia via Cu_(2)O/Cu(OH)_(2)heterostructures promoting electron transfer

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Nano Research 2024年第6期17卷 4898-4907页

作者： Jing Geng Sihan Ji anhui Province International Research Center on advanced Building materials School of Materials Science and Chemical EngineeringAnhui Jianzhu UniversityHefei 230601China anhui Province key laboratory of advanced Building materials Anhui Jianzhu UniversityHefei 230601China School of Energy materials and Chemical engineering Hefei UniversityHefei 230601China

Electrocatalytic nitrate(NO_(3)^(−))reduction to ammonia(NH_(3))offers a viable approach for sustainable NH_(3)production and environmental denitrification.Copper(Cu)possesses a distinctive electronic structure,which can augment the reaction kinetics of NO_(3)^(−)and impede hydrogen evolution reaction(HER),rendering it a promising contender for the electrosynthesis of NH_(3)from NO_(3)^(−).Nevertheless,the role of Cu_(2)O in copper-based catalysts still requires further investigation for a more comprehensive understanding.Herein,the Cu_(2)O/Cu(OH)_(2)heterostructures are successfully fabricated through liquid laser irradiation using CuO nanoparticles as a precursor.Experimental and theoretical researches reveal that Cu_(2)O/Cu(OH)_(2)heterostructure exhibits enhanced electrocatalytic performance for NO_(3)^(−)to NH_(3)because Cu(OH)_(2)promotes electron transfer and reduces the valence state of Cu active site in Cu_(2)O.At−0.6 V(vs.reversible hydrogen electrode(RHE)),the NH_(3)yield reaches its maximum at 1630.66±29.72μg·h^(−1)·mgcat^(−1),while the maximum of Faraday efficiency(FE)is 76.95%±5.51%.This study expands the technical scope of copper-based catalyst preparation and enhances the understanding of the electrocatalytic mechanism of NO_(3)^(−)to NH_(3).

关键词： Cu_(2)O/Cu(OH)_(2)heterostructures electron transfer ammonia synthesis electrocatalysts nitrate

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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 batteries.The performance of SIB is determined by the behavior of its electrode surface and the electrode–electrolyte interface during charging and discharging.Thus,the characteristics of these surfaces and interfaces should be analyzed to realize large-scale energy storage systems with high energy density and long-cycle stability.Although 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 developed.Moreover,the results obtained thus far are insufficient to draw systematic conclusions.The present study reviews the literature on the mechanism of interfacial effects in Na+storage devices.The interfaces in a sodium-ion storage device include a heterogeneous interface between electrode materials,a solid electrolyte interphase,and a cathode electrolyte interphase.The interfacial effects during the intercalation,transformation,and alloy reactions and the resulting overall battery performance were theoretically analyzed.In 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 SIBs.In 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

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NO_(x) reduction against alkali poisoning over Ce(SO_(4))_(2)-V_(2)O_(5)/TiO_(2) catalysts by constructing the Ce^(4+)-SO_(4)^(2−)pair sites

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Chinese Chemical Letters 2024年第5期35卷 355-360页

作者： Shuangxi Li Huijun Yu Tianwei Lan Liyi Shi Danhong Cheng Lupeng Han Dengsong Zhang State key laboratory of advanced Special Steel School of Materials Science and EngineeringInternational Joint Laboratory of Catalytic ChemistryCollege of SciencesShanghai UniversityShanghai 200444China

Commercial V_(2)O_(5)-based catalysts have been successfully applied in NH_(3) selective catalytic reduction(NH_(3)-SCR)of NO_(x) from power stations,but their poor alkali-resistance restrains the wider application in nonelectrical industries.In this study,NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) is greatly improved via Ce(SO_(4))_(2) modification.It has been originally demonstrated that Ce^(4+)-SO_(4)^(2−)pair sites play crucial roles in improving NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) catalysts.The strong interaction between V species and Ce sites of Ce^(4+)-SO_(4)^(2−)pairs triggers the reaction between NH_(4)^(+) species and gaseous NO via Eley-Rideal(E-R)reaction pathway.After K-poisoning,the SO_(4)^(2−)sites of Ce^(4+)-SO_(4)^(2−)pairs as protective sites strongly bond with K and thus maintain the high reaction efficiency via the E-R reaction pathway.This work demonstrates an effective strategy to enhance NO_(x) reduction against alkali poisoning over catalysts via constructing Ce^(4+)-SO_(4)^(2−)pair sites,contributing to developing alkali-resistant SCR catalysts for practical application in nonelectrical industries.

关键词： Air pollution control Selective catalytic reduction NOx reduction Alkali poisoning Ce(SO_(4))_(2)

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Highly sensitive fluorescent sensing and photocatalytic degradation performance of two-dimensional Tb-organic network

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Journal of Rare Earths 2024年第2期42卷 303-313,I0003页

作者： Ting Gao Zhihu Ma Yixia Ren Zhixiang Wang Meili Zhang Xiaoli Chen Jijiang Wang laboratory of New Energy and New Function materials Shaanxi Key Laboratory of Chemical Reaction EngineeringCollege of Chemistry and Chemical EngineeringYan'an UniversityYan'an716000China

A novel tetra-nuclear Tb-organic network,named as [Tb_(4)(2-pyia)_(6)(HAc)_(0.5)(2,2'-bipy)(H_(2)O)_(4.5)]·2,2'-bipy·H_(2)O(1),was synthesized hydrothermally based on 5-(pyridin-2-ylmethoxy) isophthalic acid(H_(2)pyia) and 2,2'-bipyridine(2,2'-bipy) ligands,and characterized by single crystal X-ray diffraction,thermogravimetric(TG) analyses,powder X-ray diffraction(PXRD) and infrared(IR) technology.1 possesses a two-dimensional network based on the tetra-nuclear inorganic building units,and the π-πstacking interactions between the pyia^(2-) ligands and the guest 2,2'-bipy molecules play an important role in the forming of 3D supramolecular structure.1 exhibits excellent fluorescent sensing performance for Fe^(3+)(1.26×10^(-8) mol/L),Cr_(2)O_(7)^(2-)(8.1×10^(-7) mol/L),2,4,6-trinitrophenol(TNP)(2.71×10^(-8) mol/L)and tetracycline(TCT)(2.76×10^(-7) mol/L) in aqueous solution with lower detection concentrations.The sensing mechanisms of 1 were investigated by density functional theory(DFT) calculations,ultraviolet-visible(UV-Vis) diffuse reflectance spectroscopy,PXRD and fluorescent lifetime analyses.The activated product of 1 was prepared by heating at 255℃ under constant pressure and used to photo-catalytically degrade TCT.Both 1 and the activated one have good photocatalytic degradation performance for TCT with degradation rates of 84.29% and 96.07%,respectively.The photocatalytic mechanisms were discovered by UV-Vis diffuse reflectance spectroscopy and radical trap experiments.The Tb-organic framework might be an excellent multifunctional fluorescent sensor and a good photocatalytic agent for TCT degradation in the future.

关键词： Tb-organic network Fluorescent sensing Photocatalytic degradation Rare earths

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Bright dual-color electrochemiluminescence of a structurally determined Pt1Ag18 nanocluster

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Aggregate 2024年第1期5卷 345-352页

作者： Bing Yin Lirong Jiang Xiaojian Wang Ying Liu Kaiyang Kuang Mengmeng Jing Chunmin Fang Chuanjun Zhou Shuang Chen Manzhou Zhu Institutes of Physical Science and Information Technology and Centre for Atomic engineering of advanced materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationDepartment of Chemistry and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsAnhui UniversityHefeiChina

Metal nanoclusters possess excellent electrochemical,optical,and catalytic properties,but correlating these properties remains challenging,which is the foundation to generate electrochemiluminescence(ECL).Herein,we report for the first time that a structurally determined Pt1Ag18 nanocluster generates intense ECL and simultaneously enhances the ECL of carbon dots(CDs)via an electrocatalytic effect.Pt^(1)Ag_(18)nanocluster show aggregation-induced emission enhancement and aggregation-induced ECL enhancement under light and electrochemical stimulation,respectively.In the presence of tripropylamine(TPrA)as a coreactant,solid Pt1Ag18 shows unprecedented ECL efficiency,which is more than nine times higher than that of 1 mM Ru(bpy)32+with the same TPrA concentration.Potential-resolved ECL spectra reveal two ECL emission bands in the presence of TPrA.The ECL emission centered at 650 nm is assigned to the solid Pt_(1)Ag_(18)nanocluster,consistent with the peak wavelength in self-annihilation ECL and photoluminescence of the solid state.The ECL emission centered at 820 nm is assigned to the CDs on the glassy carbon electrode.The electrocatalytic effect of the nanoclusters enhanced the ECL of the CDs by a factor of more than 180 in comparison to that without nanoclusters.Based on the combined optical and electrochemical results,the ECL generation pathways and mechanisms of Pt1Ag18 and CDs are proposed.These findings are extremely promising for designing multifunctional nanocluster luminophores with strong emissions and developing ratiometric sensing devices.

关键词： AIECLE AIEE electrochemiluminescence nanocluster photoluminescence structure

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Crystalline-amorphous M@MNx（M=Co,Fe,Ni）encapsulated in nitrogen-doped carbon for enhanced efficient and durable hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1547-1556页

作者： Yang Yang Xiao-Chuan Duan Shao-Hui Guo Xian-Ming Zhang College of materials Science and engineering College of ChemistryKey Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of Technology

Developing earth-abundant electrocatalysts for hydrogen evolution reaction（HER） is important for the sustainable energy economy.Herein,efficient and stable heterocatalysts consisting of crystalline-amorphous M@MNx（M=Co,Fe,Ni） encapsulated in N-doped carbon layers supported with N-doped graphene sheets（denoted as M@MNx@NC-NG） are synthesized by facile hydrothermal reaction and nitridation process.During the nitriding process,metal ions in M（tzbc）2（H2O）4(tzbc=4-（1H-1,2,4-triazol-1-yl） benzoic acid) complexes are reduced to crystalline M cores,accompanied by the formation of amorphous MNxshells;the tzbc ligands are insitu carbonized to form outermost N-doped carbon（NC）layers that connect with inner MNxvia M-N-C motifs inherited from the complex precursors and inhibit the transition of MNxfrom amorphous to crystalline phase.The Co@CoNx@NC-NG catalyst exhibits excellent HER activity with small overpotentials of 45 and 64 mV at a cathode current density of 10 mA·cm-2and low Tafel slopes of 40 and 85 mV·dec-1in 0.5 mol·L-1H2SO4and1.0 mol·L-1KOH electrolytes,respectively.The Co@CoNx@NC-NG retains 97% of the initial overpotential after 100,000 s in both acidic and alkaline media.Such outstanding HER performance originates from the crystalline-amorphous Co@CoNxthat redistributes electrons around the heterointerfaces,facilitating the conversion process of H+/H2O to hydrogen and thereby promoting HER kinetics.The outermost NC layers serve as the armor of Co@CoNx,and graphene nanosheets act as carriers of egg-like Co@CoNx@NC and conduction paths for electron shuttles,ensuring stable and continuous electrocatalytic hydrogen production.

关键词： Hydrogen evolution reaction Electrocatalysts Iron group metals Heterojunction Crystalline-amorphous structure

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