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Realizing the highly reversible Zn^(2+)and Na^(+) dual ions storage in high-crystallinity nickel hexacyanoferrate microcubes for aqueous zinc-ion batteries

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Journal of Materials Science & Technology 2023年第33期164卷 102-110页

作者： Kexuan Wang Zhu Xu Heng Li Huibo Wang Mingzheng Ge Jilei Liu Shengwen Li Zekun Hu Mengyu Zhu Yanyan Zhang Yuxin Tang Shi Chen Institute of Applied Physics and Materials Engineering University of MacaoMacao SAR 999078China State Key Laboratory of high-Performance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China College of Materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology of Clean EnergyHunan Province Key Laboratory for Advanced Carbon Materials and Applied TechnologyHunan UniversityChangsha 410082China College of Chemical Engineering Fuzhou UniversityFuzhou 350116China

Prussian blue analogues(PBAs)with the 3D open framework are regarded as promising cathode candidates for aqueous Zinc ion batteries(ZIBs).Among various PBAs,nickel hexacyanoferrate(NiHCF)has attracted considerable attention because of its high operating voltage and economic merit.However,the cyclability of NiHCF is unsatisfactory due to poor structural stability during Zn^(2+) ions insertion/deinsertion.Moreover,the ion storage mechanism of NiHCF in aqueous electrolytes has not been fully revealed yet.Herein,high-crystallinity NiHCF(HC-NiHCF)microcubes with improved structural stability and larger crystal plane spacing are synthesized.For the first time,highly reversible Zn2+ions and Na+ions co-insertion/extraction are achieved for the HC-NiHCF microcubes in mixed aqueous electrolyte,as evidenced by various observations including two separated discharge plateaus and sequential changes of Na 1s and Zn 2p signals in ex-situ X-ray photoelectron spectroscopy(XPS).As a result,a high specific capacity of 73.9 mAh g^(−1) is obtained for the HC-NiHCF microcubes at 0.1 A g−1,combined with enhanced cycle stability(75%vs.16.4%)over 1000 cycles at 2 A g^(−1).The reversible Zn^(2+) ions and Na+ions co-insertion in HC-NiHCF microcubes reveals a new ion storage mechanism of Ni-based PBAs in aqueous electrolytes.

关键词： Aqueous zinc-ion batteries Prussian blue analogues Ion storage mechanism Dual ions storage high crystallinity

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Synthesis of crystalline g-C_(3)N_(4) with rock/molten salts for efficient photocatalysis and piezocatalysis

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Green Energy & Environment 2024年第5期9卷 890-898页

作者： Tingting Xu Jung Hur Ping Niu Shulan Wang Sangwook Lee Sang-Eun Chun Li Li Department of Chemistry College of ScienceNortheastern UniversityShenyang110819China State Key Laboratory of Rolling and Automation Northeastern UniversityShenyang110819China School of Metallurgy Northeastern UniversityShenyang110819China School of Materials Science and Engineering Kyungpook National UniversityDaegu41566Republic of Korea School of Industrial Technology Advances Kyungpook National UniversityDaegu41566Republic of Korea

Graphitic carbon nitride(g-C_(3)N_(4))is emerging as a promising visible-light photocatalyst while the low crystallinity with sluggish charge separation/migration dynamics signiﬁcantly restricts its practical applications.Currently,synthesizing highly crystalline g-C_(3)N_(4) with sufﬁcient surface activities still remains challenging.Herein,different from using alkali molten salts which is commonly reported,we propose an approach for synthesis of highly crystalline g-C_(3)N_(4) with FeCl3/KCl rock/molten mixed salts.The rock salt can serve as the structure-directing template while molten salt provides the required liquid medium for re-condensation.Intriguingly,the synthesized photocatalyst showed further enhanced crystallinity and improved surface area along with high p/p*excitation compared with crystalline C_(3)N_(4) prepared from conventional molten-salt methods.These catalytically advantageous features lead to its superior photocatalytic and piezocatalytic activities with a high reactivity for overall water splitting that is not commonly reported for C_(3)N_(4).This work provides an effective strategy for structural optimization of organic semiconductor based materials and may inspire new ideas for the design of advanced photocatalysts.

关键词： high crystallinity Carbon nitride Photocatalysis Piezocatalysis Overall water splitting

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Hydrothermal Formation of Lath-Shaped Trioctahedral Smectite with high crystallinity

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Acta Geologica Sinica(English Edition) 2006年第2期80卷 290-295页

作者： Hirohisa YAMADA Kenji TAMURA Shingo YOKOYAMA Yujiro WATANABE Ecomaterials Center Nuclear Fuel Cycle Back-end Research Center College of Environmental Engineering and Architecture

Lath-shaped and highly crystalline trioctahedral smectites were synthesized under hydrothermal conditions. The quenched glasses with stoichiometrically dehydrated Na-smectite compositions were treated at （a） 500℃ and 100 MPa for 1 and 11 days; and （b） 300℃ and 100 MPa for 7 days. The crystallinity and particle size of products were dependent on the chemical composition of the starting glass, synthetic temperature and duration of hydrothermal treatment. The high structural ordering and large dimensions of the products were confirmed from the sharpness of XRD peaks; and hydration behavior under controlled relative humidity. Transmission electron microscopy was also performed for the characterization of the particle size of product. Particle sizes vary from ca. 10 nm to a few pm by changing the chemical compositions of the starting materials. The product with the highest structural ordering and largest dimension was obtained from Nao.33（Mg1.83Al0.67）Si4O11 glass treated at 500℃ and 100 MPa for 1 day. The obtained results also confirmed the metastability and compositional dependency in the formation of highly crystalline trioctahedral smectite at hydrothermal conditions.

关键词： high crystallinity hydration behavior hydrothermal formation lath-shaped trioctahedral smectite

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Regulating crystallinity in linear conjugated polymer to boost the internal electric field for remarkable visible-light-driven disinfection

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Journal of Materials Science & Technology 2023年第6期137卷 26-35页

作者： Dawei Zhang Chengling Yang Hanwen Wang Yukun Yan Zhanyong Wang Xiangrong Li Yan Liang Jinsong Zhang Jun Xiao Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016China College of Bioscience and Biotechnology Shenyang Agricultural UniversityShenyang 110866China College of Light Industry Liaoning UniversityShenyang 110036China

Conjugated linear polymers are promising metal-free photocatalysts for visible-light-driven photocatalytic water disinfection,but it was still bottlenecked by the insufficient photogenerated charge separation and transport(CST)process.Herein,we obtained the highly crystalline imine-linked conjugated linear poly-mer(ODA-BPAH)with a greatly enhanced CST process.The highly crystalline ODA-BPAH exhibited excel-lent broad-spectrum water disinfection efficiency up to 99.99999%in 1 h,which is among the reported highest of state-of-the-art photocatalysts.The crystallinity of ODA-BPAH was regulated by simply turn-ing the solvent and the experiment results revealed that the ODA-BPAH with high crystallinity exhibited higher internal electric field strength and photocatalytic performance than that with low crystallinity,which indicates that higher crystallinity in linear conjugated polymers contributes to superior CST ef-ficiency as well as the generation of reactive oxygen species.This work highlights the impact of poly-mer crystallinity on the internal electric field and proves that linear poly-imine could be a new type of promising metal-free photocatalyst for water treatment.

关键词： Polymeric photocatalysts Water disinfection Imine-linked conjugated polymer high crystallinity Internal electric field

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A two-step solvothermal procedure to improve crystallinity of covalent organic frameworks and achieve scale-up preparation

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Chinese Chemical Letters 2022年第5期33卷 2464-2468页

作者： Xiang-Hao Han Jia-Qi Chu Wen-Zhuang Wang Qiao-Yan Qi Xin Zhao Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China Shanghai Normal University Shanghai 200234China

Covalent organic frameworks(COFs),as a novel class of functional polymers,exhibit versatile applica-tions due to their crystalline porous structures and conjugated skeletons.However,synthesis of COFs with high crystallinity still faces great challenges,especially for scale-up preparation.Herein we report a two-step solvothermal process to improve crystallinity of COFs.The first step focuses on polycondensa-tion of monomers with no need for optimizing crystallization conditions.In the second step,appropriate solvothermal conditions are used to facilitate crystallization of the COFs through defects correction and structural repairing.Furthermore,this strategy could also be applicable to scale-up synthesis of high qual-ity COFs,which lays a foundation for their practical applications.

关键词： Covalent organic frameworks Synthesis Solvothermal condensation high crystallinity Scale-up preparation

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Hierarchical loading of CuO on SiO_(2) aerogel@high crystalline TiO_(2) nanofibers for efficiently photocatalytic reduction of CO_(2) without sacrificial agent

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Nano Research 2022年第5期15卷 3872-3879页

作者： Man Wen Beibei Ren Xiangzhi Ye Jianxiong He Hong Jiang Chunrong Xiong State Key Laboratory of Marine Resource Utilization in South China Sea Special Glass Key Lab of Hainan ProvinceHainan Provincial Fine Chemical Engineering Research CenterHainan UniversityHaikou 570228China Hainan haikong Special Glass Techology Co. Ltd.Chengmai 571900China

Silica aerogel was prepared by a sol-gel method with combination of freeze drying.The aerogel was filled with TiCl4 in autoclave and used to fabricate a hierarchical structure of TiO_(2) nanofiber shell and SiO_(2) aerogel core(SiO_(2)@TiO_(2)).The TiO_(2) nanofibers with a diameter of 10-15 nm were highly crystalline and mainly grew along the(101)or(001)planes,favoring charge migration along the growth axis of the fibers.The photoluminescence(PL)emission spectra show that the TiO_(2) nanofibers exhibited much lower PL intensity than P25.The free standing TiO2 nanofibers loaded with CuO had a band gap of 3.04 eV.When CuO was hierarchically loaded on the nanofiber surface and into the aerogel core(SiO_(2)/CuO@TiO_(2)/CuO),the absorption edge significantly red shifted,and the band gap was further narrowed to 2.66 eV.Meanwhile,Fe^(3+)implanted TiO_(2) nanofibers on the aerogel surface(SiO_(2)@Fe-TiO_(2))were also fabricated in the same strategy.The CuO loaded nanofibers(SiO_(2)/CuO@Fe-TiO_(2)/CuO)had a band gap of 2.62 eV.The photocatalytic reduction of CO_(2) was performed under light irradiation by a 300 W Xe-lamp for 4 h.The methanol yield over the SiO_(2)/CuO@Fe-TiO_(2)/CuO reached~2,400 μmol·gcat^(-1) in the absence of sacrificial agent.

关键词： hierarchical structure fibrous morphology high crystallinity lattice doping without sacrificial agent

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快速微波还原电化学衍生氧化石墨烯制备高结晶石墨烯膜

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Science China Materials 2023年第12期66卷 4733-4741页

作者：熊志远于沛梁庆华李丹 School of Light Industry and Engineering South China University of TechnologyGuangzhou 510614China Department of Chemical Engineering The University of MelbourneParkvilleVictoria 3010Australia Department of Materials Science and Engineering Monash UniversityClaytonVictoria 3800Australia Key Laboratory of Rare Earth Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou 341000China

电化学氧化石墨,可用于大规模合成氧化石墨烯,是一种可持续且直接的方法.然而,关于电化学衍生氧化石墨烯(EGO)进一步还原的研究却很缺少.本文中,我们报道了EGO膜的快速微波还原过程.化学法合成的氧化石墨烯膜需要数分钟微波辐射才能被还... 详细信息

电化学氧化石墨,可用于大规模合成氧化石墨烯,是一种可持续且直接的方法.然而,关于电化学衍生氧化石墨烯(EGO)进一步还原的研究却很缺少.本文中,我们报道了EGO膜的快速微波还原过程.化学法合成的氧化石墨烯膜需要数分钟微波辐射才能被还原,但是我们制备的EGO膜经3秒微波辐射即可转化为高结晶石墨烯膜(HCGM),并且该过程无需对膜进行预处理或添加微波增敏剂.与以前报道的微波法制备的石墨烯相比,本文制备的HCGM具有大尺寸芳香区(约100 nm)、高碳/氧原子比(约33)和高电导率(约5×10^(4)S m^(−1)).EGO的高微波还原效率可以归因于其独特分子结构,EGO中丰富的芳香区可高效吸收微波,引发EGO膜实现瞬时体相加热.该研究加深了对氧化石墨烯微波还原机理的理解,并为HCGM的生产提供了一条便捷途径.

关键词： graphene oxide graphene membrane electrochemical oxidation high crystallinity microwave reduction

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Constructing Crystalline g-C_(3)N_(4)/g-C_(3)N_(4-x)S_(x)Isotype Heterostructure for Efficient Photocatalytic and Piezocatalytic Performances

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Energy & Environmental Materials 2023年第2期6卷 8-16页

作者： Tingting Xu Zhonghui Xia Hongguan Li Ping Niu Shulan Wang Li Li Department of Chemistry School of ScienceNortheastern UniversityShenyang 110819China State Key Laboratory of Rolling and Automation Northeastern UniversityShenyang 110819China School of Metallurgy Northeastern UniversityShenyang 110819China

Graphitic carbon nitride(g-C_(3)N_(4))is viewed as a promising visible-light photocatalyst for industrialization due to its low processing temperature and high chemical stability.However,serious charge recombination caused by incomplete polymerization during direct calcination of nitrogen-rich precursors significantly limits its photocatalytic performances.To boost charge separation,herein,we propose a rational strategy by constructing a crystalline g-C_(3)N_(4)/g-C_(3)N_(4-x)S_(x) isotype heterostructure through the molten salt method.Theoretical calculation reveals that apparent charge-transfer channels are formed between g-C_(3)N_(4) and S-doped g-C_(3)N_(4) layers in the heterostructure.Owing to high crystallinity for decreasing charge recombination and isotype heterostructure for efficient charge transfer,the as-prepared g-C_(3)N_(4)/g-C_(3)N_(4-x)S_(x) showed remarkable photocatalytic performances with the hydrogen production rate elevated by up to 12.3 times of its singular components.Another novelty of this work is we investigated for the first time the piezocatalytic activity of crystalline g-C_(3)N_(4) by characterizing its performance for H2O2 generation and KMnO4 reduction.Strikingly,its superior piezocatalytic performance over components can be further improved by NaBH4 treatment,which is uncovered to enhance the asymmetric structure of crystalline g-C_(3)N_(4) by introducing extra cyano groups and removing partial NHx species in its tri-s-triazine layer structure.This work opens up new strategies for the design of highly efficient polymeric photocatalysts and highlights the piezocatalytic studies of g-C_(3)N_(4).

关键词： carbon nitride high crystallinity isotype heterostructure photocatalysis piezoelectric catalysis

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Promoting condensation kinetics of polymeric carbon nitride for enhanced photocatalytic activities

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Chinese Chemical Letters 2020年第1期31卷 115-118页

作者： Dongya Ni Yuye Zhang Yanfei Shen Songqin Liu Yuanjian Zhang Jiangsu Engineering Laboratory of Smart Carbon-Rich Materials and Device Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical ResearchSchool of Chemistry and Chemical EngineeringMedical SchoolSoutheast University

Polymeric carbon nitride(CN)semiconductor by thermal condensation of N-rich precursors has attracted much attention for its capability ranging from photocatalytic and photoelectrochemical energy conversion to biosensing.However,the influence of condensation process on the final structure of CN was rarely studied,making the condensation kinetic far from be fully optimized.Herein,we report the preparation of CN by a simple condensation kinetics modulation using a faster ramping rate during the polymerization process.The modified condensation recipe was even simpler than the conventional one,but led to an improved photocatalytic H2 evolution up to 3 times without any additional chemicals or other complements.Detailed mechanism studies revealed the increase of crystallinity and surface area due to the rapid condensation played the key roles.This work would offer a more facile and effective way to prepare bulk CN for large-scale industrial applications of bulk CN with higher photocatalytic actives for sustainable energy,environmental and biosensing.

关键词： Polymeric carbon nitride Condensation kinetics Fast ramping rate high crystallinity Photocatalytic hydrogen evolution

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