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Interlayer and doping engineering in partially graphitic hollow carbon nanospheres for fast sodium and potassium storage

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Chinese Chemical Letters 2023年第2期34卷 582-587页

作者： Dongfei Sun Sen Lin Dandan Yu Zijuan Wang Fangfang Deng Xiaozhong Zhou Guofu Ma Ziqiang Lei Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education Key Laboratory of Eco-environmental Polymer Materials of Gansu ProvinceCollege of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou 730070China

Constructing anodes with fast ions/electrons transfer paths is an effective strategy to achieve high-performance sodium ion batteries(SIBs)/potassium ion batteries(PIBs). Amorphous carbon is a promising candidate anode for SIBs/PIBs owing to its disordered carbon layers, abundant defects/pores, and lowcost resources. However, the larger radius of Na^(+)/K^(+) leading to depressed kinetics and poor cycling performance, impeding their further applications. Herein, we propose an efficient strategy to construct of nitrogen, sulfur co-doped hollow carbon nanospheres(NS-HCS) involving an in situ growth of polydopamine on nano-Ni(OH)2template with subsequent sulfur doping process. During the formation process, the produced Ni nanospheres play as the hard template and catalyst for the formation of hollow carbon nanosphere with partially graphite microcrystalline structure, while the sulfur doping process can enlarge the interlayer space and create more defects on the surface of carbon nanospheres, thus synchronous improve the Na^(+)/K^(+) insertion and adsorption ability in NS-HCS. With the synergistic control of the enlarged interlayer spacing, high content of pyridinic N/pyrrolic N and graphitization, a hybrid storage mechanism facilitates the transport kinetics and endows the NS-HCS electrode with high capacities and good cycling stability in SIBs and PIB. Benefit from the multiple effects, NS-HCS exhibits the improved capacity of 274.8 m Ah/g at 0.1 A/g and excellent cycling stability of 149.5 m Ah/g after 5000 cycles at2.5A/g in SIBs, as well as good potassium ion storage behavior with a high capacity retention of 76.5%after 700 cycles at 1.0 A/g, demonstrating the potential applications of NS-HCS for high-performance SIBs and PIBs.

关键词： Heteroatom doping Hollow carbon nanosphere Long cycle life Hybrid storage mechanism Sodium ion batteries Potassium ion batteries

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Hexagonal boron nitride based slippery liquid infused porous surface with anti-corrosion, anti-contaminant and anti-icing properties for protecting magnesium alloy

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Chinese Chemical Letters 2024年第4期35卷 532-538页

作者： Wenhao Yan Shuaiya Xue Xuerui Zhao Wei Zhang Jian Li Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education College of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou 730070China

In an era where the concept of green development is deeply rooted, magnesium(Mg) alloy as a light metal has a long-term development prospect in the process of energy saving, emission reduction and environmental improvement. However, anti-corrosion performance of Mg alloy is poor due to the high chemical activity and low equilibrium potential, which limits the development of Mg alloy products.Herein, three-dimensional mesopore hollow polypyrrole spheres(MHPS) were prepared, and the MHPS was inserted into the middle of the stacked hexagon boron nitride(h-BN) lamellae, which allowed the hBN to be separated forming a further composite with abundant pore structure. Subsequently, the MHPS/hBN-OH composite was uniformly sprayed on the Mg alloy surface via simple spraying method to form the superhydrophobic surface(SHS). Finally, the slippery liquid infused porous surface(SLIPS) was successfully fabricated by applying drops of silicone lubricant on the superhydrophobic coating surface. After a series of characterization and testing, the results showed that the stacking of h-BN lamellae was significantly reduced after h-BN was successfully embedded by MHPS. In addition, the fabricated SLIPS have excellent self-cleaning, mechanical stability, anti-icing and anti-corrosion properties. Therefore, the method of embedding polymer microspheres not only offers a new strategy for h-BN exfoliation, but also the successful prepared SLIPS largely retards the corrosion of Mg alloy while providing new ideas for the development of SLIPS.

关键词： Anti-corrosion Mg alloy Hexagon boron nitride Polypyrrole SLIPS

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A Pd_(2)L_(4) Metallacage-Cored Supramolecular Amphiphile and Its Application in Dual-Responsive Controllable Release

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Chinese Journal of Chemistry 2022年第20期40卷 2421-2427页

作者： Yongping Chai Peng Qin Xupeng Li Tai-Bao Wei Qi Lin You-Ming Zhang Hong Yao Wen-Juan Qu Bingbing Shi Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education Key Laboratory of Eco-environmental Polymer Materials of Gansu ProvinceCollege of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhouGansu730070 China Gansu Natural Energy Research Institute LanzhouGansu730046 China

The construction of multi-responsive supramolecular systems for drug delivery is a challenging task.In this work,a Pd_(2)L_(4) metallacage 1·([BF_(4)]^(−))_(4) with four pyrene units was first designed and synthesized through coordination-driven self-assembly.After the introduction ofγ-CD,a supramolecular amphiphile 1–γ-CD was successfully constructed based on the host–guest molecular recognition betweenγ-CD and the pyrene unit of 1·([BF_(4)]^(−))_(4),which further self-assembled into dual-responsive supramolecular vesicles in aqueous solution.DOX·HCl was used as a model molecule to study the drug encapsulation and release behavior of the supramolecular vesicles.By adjusting the pH of the solution to acidic condition or adding a certain amount ofα-amylase,the vesicle structure was destroyed to achieve rapid and effective release of the drug molecules.This study provides an example for the rational design of efficient dual-responsive supramolecular nanocarriers,which have potential application value in the field of controlled drug delivery.

关键词： Self-assembly Molecular recognition Metallacages Host-Guest systems Controllable release

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Synthesis of Stimuli-Responsive Block Copolymers and Block Copolymer Nano-assemblies

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Chinese Journal of Chemistry 2022年第8期40卷 965-972页

作者： Yuan Liu Yu Sun Wangqing Zhang key laboratory of functional polymer materials of the ministry of education Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China

Block copolymers have aroused much interest,and their application has been rapidly expanded.In recent years,our group has committed to exploring synthesis and self-assembly of block copolymers.We have designed and synthesized several new thermo-responsive polymers and photo-responsive polymers by living/controlled radical polymerization(LCRP)and investigated their stimuli-responsive properties.Aiming at convenient and efficient synthesis of block copolymer nano-assemblies,we have developed several methods based on polymerization-induced self-assembly(PISA).Herein,we give a short summary of our research in these years.The aim of this account is to stimulate innovative synthesis strategies of block copolymer nano-assemblies,and promote more scientific research cooperation to face the exciting opportunities and challenges encountered in block copolymers.

关键词： Block copolymers Living/controlled radical polymerization(LCRP) Stimuli-responsive Self-assembly Nanostructures

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Constructing oxygen deficiency-rich V_(2)O_(3)@PEDOT cathode for high-performance aqueous zinc-ion batteries

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Rare Metals 2024年第2期43卷 635-646页

作者： Dong-Fei Sun Zi-Juan Wang Tian Tian Xin Yu Dan-Dan Yu Xiao-Zhong Zhou Guo-Fu Ma Zi-Qiang Lei Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education Key Laboratory of Eco-environmental Polymer Materials of Gansu ProvinceSchool of College of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou730070China

Aqueous zinc-ion batteries(AZIBs)have attracted widespread attention due to the advantages of high safety and environmental friendliness.Although V_(2)O_(3) is a promising cathode,the strong electrostatic interaction between Zn^(2+) and V_(2)O_(3) crystal,and the sluggish reaction kinetics still limit their application in AZIBs.Herein,the oxygen defects rich V_(2)O_(3) with conducive poly(3,4-ethylenedioxythiophene)(PEDOT)shell(V_(2)O_(3)-Od@PEDOT)was fabricated for AZIBs by combining the sulfur-assisted thermal reduction and in-situ polymerization method.The introduced oxygen vacancies of V_(2)O_(3)–Od@PEDOT weaken the electrostatic interaction between Zn^(2+) and the host material,improving the interfacial electron transport,while the PEDOT coating enhances the structural stability and conductivity of V_(2)O_(3),thus accelerating the reaction kinetics.Based on the advantages,V_(2)O_(3)–Od@PEDOT electrode delivers a reversible capacity of 495 mAh·g^(−1) at 0.1 A·g^(−1),good rate capability(189 mAh·g^(−1)at 8.0 A·g^(−1)),and an impressive cycling stability with 90.1%capacity retention over 1000 cycles at 8.0 A·g^(−1).The strategy may provide a path for exploiting the other materials for high performance AZIBs.

关键词： Oxygen defects V_(2)O_(3) PEDOT Electrochemical self-optimization Aqueous zinc-ion batteries

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Chirality and chiral functional composites of bicontinuous cubic nanostructured cubosomes

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Chinese Chemical Letters 2022年第3期33卷 1488-1492页

作者： Deyin Wang Hongkai Liu Wei Wang Center for Synthetic Soft materials Key Laboratory of Functional Polymer Materials of Ministry of Education and Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China

Molecular self-assembly is the most important strategy for the development of chiral aggregates and chiral functional materials. In this study, we rationally designed and synthesized chiral fluorescent heteroclusters that were self-assembled into microscale cubosomes with a three-dimensional(3D) bicontinuous cubic phase nanostructure. The cubosomes exhibited chirality, indicating that chirality is transferred from the molecules to the 3D nanostructure. Therefore, we confirmed the formation of a chiral bicontinuous cubic phase nanostructure for the first time. We also showed that this chirality originates from the continuous change in the saddle-splay distortion of the molecules within the curved bilayer. At the same time, transparent films of chiral composites were prepared by mixing the chiral cubosomes with an epoxy resin and then curing the mixture. Therefore, we demonstrated an effective method for preparing chiral composites.

关键词： Chirality Self-assembly Nanostructure Composite

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CeO_(2)C_(2)Nanoparticles with Oxygen-Enriched Vacancies In-site Self-embedded in Fe,N Co-doped Carbon Nanofibers as Efficient Oxygen Reduction Catalyst for Zn-Air Battery

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Chinese Journal of Chemistry 2022年第23期40卷 2763-2772页

作者： Mingxin Zhang Hui Peng Kanjun Sun Xuan Xie Xiaofei Lei Sitong Liu Guofu Ma Ziqiang Lei Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education Key Laboratory of Polymer Materials of Gansu ProvinceCollege of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhouGansu 730070China College of Chemistry and Chemical Engineering Lanzhou City UniversityLanzhouGansu 730070China

Rational design of robust non-noble electrocatalysts with numerous oxygen vacancies and highly reactive activity for oxygen reduction reaction(ORR)towards Zn-air batteries is extremely paramount yet challenging.Herein,a novel CeO_(2)C_(2)nanoparticles self-embedded in Fe,N co-doped carbon nanofibers(CeO_(2)C_(2)@Fe-N-C)heterostructure catalyst has been prepared by the in-site dual template assisted electrospinning technique and subsequent high temperature pyrolysis strategy.Thanks to the CeO_(2)C_(2)with oxygen-enriched vacancies and versatile Fe-N-C with rich reactive species and high conductivity,CeO_(2)C_(2)@Fe-N-C catalyst exhibits outstanding catalytic performance in the ORR process,and shows excellent methanol tolerance and cycle stability.In addition,CeO_(2)C_(2)@Fe-N-C delivers a nearly four-electron transfer process in the process of oxygen reduction catalysis,providing a fast-electrochemical kinetic rate,which makes it an efficient air cathode for the Zn-air battery.Importantly,the Zn-air battery fabricated with CeO_(2)C_(2)@Fe-N-C cathode achieves superior performance including large open-circuit voltage(1.5 V)and high specific capacity(780 mAh·g–1 at 10 mA·cm–2)together with superior reversibility and cycling stability,outperforming commercial Pt/C catalyst.The present work introduces a new strategy to design and develop highly active non-noble catalysts and highlights the synergy from heterostructure in oxygen electrocatalysis for advanced Zn-air batteries.

关键词： Energy conversion Doping Nanoparticles Carbon nanofibers Zn-air battery

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Scattering Function and Spinodal Transition of Linear and Nonlinear Block Copolymers Based on a Unified Molecular Model

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Chinese Journal of polymer Science 2021年第6期39卷 779-788,I0009页

作者： Weichao Shi key laboratory of functional polymer materials of ministry of education Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China

This work uses a block copolymer architecture[(A′B)nA2]m to unify the scattering function and spinodal transition of typical AB-type block copolymers.The key roles of block number,junction points and asymmetry ratios of block length are(1)to determine the form factor of each block copolymer at the molecular scale;(2)to affect the entropy loss across the spinodal transition and may result in deflection of spinodal curves.The common features are validated in typical linear and nonlinear block copolymers,including AB diblock,asymmetric A′BA triblock,miktoarm stars of ABn,AnBn,(AB)n,(A′B)nA,A′BAm,and multi-graft combs of(BnA2)m and[(A′B)nA2]m.The explicit scattering functions and form factors of various block copolymers can be directly applied in radiation experiments(i.***.neutron or X-ray scattering)to unravel the effect of molecular architecture in solution and microphase separation in disordered melt.The molecular model used in this study is also helpful to guide the chemical synthesis to explore more potentially interesting block copolymers.

关键词： Scattering function Form factor Spinodal transition Molecular structure Block copolymer

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Dopamine-triggered one-step functionalization of hollow silica nanospheres for simultaneous lubrication and drug release

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Friction 2023年第3期11卷 410-424页

作者： Qiangbing WEI Tian FU Lele LEI Huan LIU Yixin ZHANG Shuanhong MA Feng ZHOU Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education Key Laboratory of Polymer Materials of Gansu ProvinceCollege of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou 730070China State key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Shandong laboratory of Yantai Advanced materials and Green Manufacture Yantai 264006China

Osteoarthritis(OA)has been regarded as a lubrication deficiency related joint disease.Combination of both joint lubrication and drug intervention may provide a promising nonsurgical strategy for treatment of OA.Developing novel and simple approaches to fabricate superlubricating nanoparticles with drug release property is highly required.Herein,dopamine triggered one-step polymerization method was employed to fabricate polydopamine/poly(3-sulfopropyl methacrylate potassium salt)(PDA-PSPMA)conjugate coating on hollow silica(h-SiO_(2))nanosphere surfaces to engineer functional nanoparticles(h-SiO_(2)/PDA-PSPMA).The as-prepared h-SiO_(2)/PDA-PSPMA exhibits excellent aqueous lubrication performance on biomaterial substrates as well as natural bovine articular cartilage based on hydration effect of negatively charged PDA-PSPMA coating and"rolling"effect of h-SiO_(2)nanospheres.In vitro drug loading-release experiments demonstrate that PDA-PSPMA coating functionalized h-SiO_(2)nanospheres show high drug-loading and sustained-release capability of an anti-inflammatory drug,diclofenac sodium(DS).Such h-SiO_(2)/PDA-PSPMA nanospheres can be potentially used as a synergistic therapy agent for OA treatment combining by simultaneous joint lubrication anddrugrelease.

关键词： osteoarthritis treatment functionalized nanoparticles injectable biolubricant friction reduction drug release

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Perylene Diimide-Based Oligomers and polymers for Organic Optoelectronics

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Accounts of materials Research 2022年第3期3卷 309-318页

作者： Pei Cheng Xingang Zhao Xiaowei Zhan key laboratory of polymer Chemistry and Physics of ministry of education School of Materials Science and EngineeringPeking UniversityBeijing 100871China College of polymer Science and Engineering State Key Laboratory of Polymer Material and EngineeringSichuan UniversityChengdu 610065China key laboratory of eco-functional polymer materials of ministry of education College of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou 730070China

CONSPECTUS:Perylene diimide(PDI)as a classical dye has some advantages,such as structural diversity,tunable optical and electronic properties,strong light absorption,high electron affinity,and good electron-transporting properties and stability.The PDI-based oligomers and polymers are good candidates for n-type semiconductors in organic electronics and photonic devices.A polymer solar cell(PSC)that converts sunlight into electricity is a promising renewable and clean energy technology and has some superiorities,such as simple preparation and being lightweight,low cost,semitransparent,and flexible.For a long time,fullerene derivatives(e.g.,PCBM)have been the most important electron acceptors used in the active layer of PSCs.However,PCBM suffers from some disadvantages,for example,weak absorption,a large amount of energy loss,and unstable morphology.Compared to PCBM,PDI-based materials present some advantages:intense visible-light absorption;lowest unoccupied molecular orbital(LUMO)energy levels can be modulated to achieve a suitable charge separation driving force and high open-circuit voltage(V_(OC));and the molecular configuration can be adjusted to achieve morphology stability.Thus,PDI-based oligomers and polymers are widely used as electron acceptors in the active layer of PSCs.In addition,PDI-based oligomers and polymers are widely used as n-type semiconductors in other electronic and photonic devices,such as organic field-effect transistors(OFETs),light-emitting diodes,lasers,optical switches,and photodetectors.

关键词： stability absorption separation

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