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Polar solvent induced in-situ self-assembly and oxygen vacancies on Bi_(2)MoO_(6)for enhanced photocatalytic degradation of tetracycline

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Nano Research 2024年第6期17卷 4951-4960页

作者： fangyan liu Dongyue Su Weizhen liu Baiquan liu Chuan liu Hong Wang Mengye Wang State Key Laboratory of Optoelectronic Materials and Technologies Guangdong Province Key Laboratory of Display Material and TechnologySchool of Electronics and Information TechnologySun Yat-Sen UniversityGuangzhou 510275China School of Materials Sun Yat-Sen UniversityShenzhen 518107China School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and RecyclingSouth China University of TechnologyGuangzhou 510006China

It has been proved to be an effective route to efficiently ameliorate photocatalytic performance of catalysts via designing three-dimensional(3D)hierarchical nanostructures and constructing oxygen vacancies(VOs).However,controlling the self-assembly of organization into 3D hierarchical nanostructures while introducing VOs in photocatalysts remains a challenge.Herein,we reported an ethylene glycol(EG)mediated approach to craft 3D hydrangea-structure Bi_(2)MoO_(6)with VOs for efficient photocatalytic degradation of tetracycline.Through manipulating the EG concentration during the fabrication process,the influence of EG concentration on the Bi_(2)MoO_(6)structure was systematically investigated.EG could promote the self-assembly of Bi_(2)MoO_(6)nanosheets to form a 3D hierarchical structure.Compared with 2D nanoplates,3D hierarchical architecture enhanced the surface area and the amount of active sites of Bi_(2)MoO_(6).In addition,the reduction effect of EG on metallic oxide enabled the generation of VOs in Bi_(2)MoO_(6).The VOs adjusted the electronic structure of Bi_(2)MoO_(6),which not only enhanced the light harvesting,but also facilitated the simultaneous utilization of photo-induced electrons and holes to form reactive oxygen species(·O2−and·OH)for the efficient tetracycline decomposition.3D Bi_(2)MoO_(6)hydrangea with VOs achieved a 79.4%removal efficiency of tetracycline after 75 min.This work provides a simple yet robust EG-mediated strategy,which not only promotes the self-assembly of nano-catalysts into 3D hierarchical architectures,but also crafts tunable VOs for highly efficient photocatalysis.

关键词： three-dimensional(3D)hierarchical nanostructures tunable oxygen vacancies ethylene glycol(EG)-mediated strategy bismuth molybdate photocatalytic degradation tetracycline

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The key challenges and future opportunities of electrochemical capacitors

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Journal of Energy Chemistry 2023年第1期76卷 459-461,I0012页

作者： fangyan liu Xinliang Feng Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Center for Advancing Electronics Dresden(Cfaed)and Faculty of Chemistry and Food Chemistry Technische Universitat Dresden01062 DresdenGermany Department of Synthetic Materials and Functional Devices Max Planck Institute of Microstructure PhysicsD-06120 Halle(Saale)Germany

Electrochemical capacitors(ECs)with unique merits of fast charge/discharge rate and long cyclability are one of the representative electrochemical energy storage systems,possessing wide applications in power electroni... 详细信息

关键词： Electrochemical capacitors Electrical double layer capacitors Pseudocapacitors Li-ion capacitors Microscale electrochemical capacitors

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Robust route to H_(2)O_(2)and H_(2)via intermediate water splitting enabled by capitalizing on minimum vanadium-doped piezocatalysts

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Nano Research 2022年第9期15卷 7986-7993页

作者： Yuekun Li Li Li fangyan liu Biao Wang Feng Gao Chuan liu Jingyun Fang Feng Huang Zhang Lin Mengye Wang School of Materials Sun Yat-Sen UniversityShenzhen 518107.State Key Laboratory of Optoelectronic Materials and TechnologiesSun Yat-Sen UniversityGuangzhou 510275China School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and RecyclingSouth China University of TechnologyGuangzhou 510006China School of Metallurgy and Environment Central South UniversityChangsha 410083China Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology School of Environmental Science and EngineeringSun Yat-Sen UniversityGuangzhou 510275China The Guangdong Province Key Laboratory of Display Material and Technology School of Electronics and Information TechnologySun Yat-Sen UniversityGuangzhou 510275China

H_(2)O_(2)is an environmentally friendly chemical for a wide range of water treatments.The industrial production of H_(2)O_(2)is an anthraquinone oxidation process,which,however,consumes extensive energy and produces pollution.Here we report a green and sustainable piezocatalytic intermediate water splitting process to simultaneously obtain H_(2)O_(2)and H_(2)using single crystal vanadium(V)-doped NaNbO_(3)(V-NaNbO_(3))nanocubes as catalysts.The introduction of V improves the specific surface area and active sites of NaNbO_(3).Notably,V-NaNbO_(3)piezocatalysts of 10 mg exhibit 3.1-fold higher piezocatalytic efficiency than the same catalysts of 50 mg,as more piezocatalysts lead to higher probability of aggregation.The aggregation causes reducing active sites and decreased built-in electric field due to the neutralization between different nano-catalysts.Remarkably,piezocatalytic H_(2)O_(2)and H_(2)production rates of V-NaNbO_(3)(10 mol%)nanocubes(102.6 and 346.2μmol·g^(−1)·h^(−1),respectively)are increased by 2.2 and 4.6 times compared to the as-prepared pristine NaNbO_(3)counterparts,respectively.This improved catalytic efficiency is attributed to the promoted piezo-response and more active sites of NaNbO_(3)catalysts after V doping,as uncovered by piezoresponse force microscopy(PFM)and density functional theory(DFT)simulation.More importantly,our DFT results illustrate that inducing V could reduce the dynamic barrier of water dissociation over NaNbO_(3),thus enhancing the yield of H_(2)O_(2)and H_(2).This facile yet robust piezocatalytic route using minimal amounts of catalysts to obtain H_(2)O_(2)and H_(2)may stand out as a promising candidate for environmental applications and water splitting.

关键词： water splitting H_(2)evolution H_(2)O_(2)production piezocatalysis vanadium-doped NaNbO_(3)

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A safe,low-cost and high-efficiency presodiation strategy for pouch-type sodium-ion capacitors with high energy density

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Journal of Energy Chemistry 2022年第1期31卷 442-450,I0012页

作者： Congkai Sun Xiong Zhang Chen Li Kai Wang Xianzhong Sun fangyan liu Zhong-Shuai Wu Yanwei Ma Institute of Electrical Engineering Chinese Academy of SciencesBeijing 100190China School of Engineering Sciences University of Chinese Academy of SciencesBeijing 100049China Stare Key Laboratory of Catalysis.Dalian Institute of Chemical Physics Chinese Academy of SciencesDalianLiaoning 116023China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalianLiaoning 116023China

Sodium-ion capacitors(SICs)have attracted appreciable attention in virtue of the higher energy and power densities compared with their rivals,supercapacitors and sodium-ion batteries.Due to the lack of sodium resources in cathode,presodiation is critical for SICs to further augment performances.However,current presodiation strategy utilizes metallic sodium as the presodiation material.In this strategy,assembling/disassembling of half-cells is required,which is dangerous and in creases the time and cost of SIC leading to the restriction of their industrialization and commercialization.Herein we present a safe,low-cost and high-efficiency presodiation strategy by first employing Na_(2)C_(2)O_(4) as the sacrificial salt applied in SICs.Na_(2)C_(2)O_(4) is environmentally friendly and possesses considerably low expenditure.No additional residues remain after sodium extraction ascribed to its"zero dead mass"property.When paired with commercial activated carb on as the cathode and commercial hard carbon as the ano de,the constructed pouch-type SICs exhibit high energy and power densities of 91.7 Wh/kg and 13.1 kW/kg,respectively.This work shows a prospect of realizing the safe and low-cost manufacturing for high-performance SICs commercially.

关键词： Presodiation material Sacrificial salt High efficiency Zero dead mass Sodium-ion capacitors Lithium-ion capacitors

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Sustainable Lignin-Derived Carbon as Capacity-Kinetics Matched Cathode and Anode towards 4.5 V High-Performance Lithium-Ion Capacitors

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Energy & Environmental Materials 2023年第4期6卷 98-105页

作者： fangyan liu Pengfei Lu Ying Zhang Feng Su Liangzhu Zhang Shuanghao Zheng Xiong Zhang Fangyuan Su Yanwei Ma Zhongshuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China Anhui Key Laboratory of Spin Electron and Nanomaterials School of Chemistry and Chemical EngineeringSuzhou UniversitySuzhou 234000China University of Chinese Academy of Sciences Beijing 100049China CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Institute of Electrical Engineering Chinese Academy of SciencesBeijing 100190China School of Engineering Sciences University of Chinese Academy of SciencesBeijing 100049China Institute of Electrical Engineering and Advanced Electromagnetic Drive Technology Qilu ZhongkeJinan 250013China

The Li-ion capacitors(LICs)develop rapidly due to their double-high features of high-energy density and high-power density.However,the relative low capacity of cathode and sluggish kinetics of anode seriously impede the development of LICs.Herein,the precisely pore-engineered and heteroatomtailored defective hierarchical porous carbons(DHPCs)as large-capacity cathode and high-rate anode to construct high-performance dual-carbon LICs have been developed.The DHPCs are prepared based on triple-activation mechanisms by direct pyrolysis of sustainable lignin with urea to generate the interconnected hierarchical porous structure and plentiful heteroatominduced defects.Benefiting from these advanced merits,DHPCs show the well-matched high capacity and fast kinetics of both cathode and anode,exhibiting large capacities,superior rate capability and long-term lifespan.Both experimental and computational results demonstrate the strong synergistic effect of pore and dopants for Li storage.Consequently,the assembled dual-carbon LIC exhibits high voltage of 4.5 V,high-energy density of 208 Wh kg^(−1),ultrahigh power density of 53.4 kW kg^(−1)and almost zerodecrement cycling lifetime.Impressively,the full device with high mass loading of 9.4 mg cm^(−2)on cathode still outputs high-energy density of 187 Wh kg^(−1),demonstrative of their potential as electrode materials for high-performance electrochemical devices.

关键词： capacity-kinetics matching defective hierarchical porous carbons high mass loading high power density Li-ion capacitors

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Structural regulation chemistry of lithium-ion solvation in nonflammable phosphate-based electrolytes for high interfacial compatibility with graphite anode

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Journal of Energy Chemistry 2023年第12期87卷 501-508,I0013页

作者： Chenyang Shi Xinjing Huang Jiahao Gu Zeyu Huang fangyan liu Mengran Wang Qiyu Wang Bo Hong Zhian Zhang Jie Li Yanqing Lai School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina Engineering Research Centre of Advanced Battery Materials The Ministry of EducationChangsha 410083HunanChina Hunan Province Key Laboratory of Nonferrous Value-Added Metallurgy Central South UniversityChangsha 410083HunanChina Powder Metallurgy Research Institute State Key Laboratory of Powder MetallurgyCentral South UniversityChangsha 410083HunanChina

With the booming development of lithium-ion batteries,safety has become one of the most primary focuses of current researches.Although there are various approaches to enhance the safety of lithiumion batteries,phosphate-based electrolyte holds the greatest potential for practical application due to their non-flammability.Nonetheless,its compatibility issue with the graphite anode remains a significant obstacle to its widespread use.Herein,an effective method is proposed to improve the compatibility of electrolyte with graphite(Gr)anode by rationally adjusting the proportion of lithium salt and solvent components to optimize the Li^(+)solvation structure.By slightly increasing the Li^(+)/triethyl phosphate(TEP)ratio,TEP alone cannot fully occupy the inner solvation sheath and therefore less polar ethylene carbonate(EC)has to be recruited,and the solvation structure gradually changes from Li^(+)–[TEP]_(4)to Li^(+)–[TEP]_(3)[EC]with the coexistence of EC and TEP.Simultaneously,EC molecules in the Li^(+)–[TEP]_(3)[EC]could be preferentially reduced on graphite compared to the TEP molecules,resulting in the formation of a uniform and durable solid-electrolyte interphase(SEI)layer.Benefiting from the optimized phosphate-based electrolyte,the Gr|Li battery exhibits a capacity retention rate of 96.8%after stable cycling at 0.5 C for 470 cycles which shows a longer cycle life than the battery with carbonate electrolyte(cycling at 0.5 C for 450 cycles).Therefore,this work provides the guidance for designing a non-flammable phosphate-based electrolyte for high-safety and long cycling-life lithium-ion batteries.

关键词： Ethylene carbonate Triethyl phosphate Solvation structure Non-flammable electrolyte

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Lignin derived hierarchical porous carbon with extremely suppressed polyselenide shuttling for high-capacity and long-cycle-life lithium-selenium batteries

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Journal of Energy Chemistry 2021年第4期30卷 476-483页

作者： Pengfei Lu fangyan liu Feng Zhou Jieqiong Qin Haodong Shi Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Shijingshan DistrictBeijing 100049China

Lithium-selenium(Li-Se)batteries have attracted considerable attentions for next-generation energy storage systems owing to high volumetric capacity of 3265 m Ah cm^(-3) and excellent electronic conductivity(~10^(-5)S cm^(-1))of selenium.However,the shuttling effect and capacity fading prevent their wide applications.Herein we report a low-cost strategy for scalable fabrication of lignin derived hierarchical porous carbon(LHPC)as a new high-loading Se host for high-capacity and long-term cycling Li-Se batteries in carbonate electrolyte.The resulting LHPC exhibits three-dimensional(3D)hierarchically porous structure,high specific surface area of 1696 m^(2) g^(-1),and hetero-atom doping(O,S),which can effectively confine the Se particles into the micropores,and meanwhile,offer effective chemical binding sites for selenides from hetero-atoms(O,S).As a result,our Li-Se batteries based on Se@LHPC demonstrate high capacity of 450 m Ah g^(-1) at 0.5 C after 500 cycles,with a low capacity fading rate of only 0.027%.The theoretical simulation confirmed the strong affinity of selenides on the O and S sites of LHPC effectively mitigating the Se losing.Therefore,our strategy of using lignin as the low-cost precursor of hierarchically porous carbon for high-loading Se host offers new opportunities for high-capacity and long-life Li-Se batteries.

关键词： Lignin Hierarchical porous carbon Lithium selenium battery Long cycling stability Energy storage

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Synthesis of Size-Controllable NiCo2S4 Hollow Nanospheres Toward Enhanced Electrochemical Performance

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Energy & Environmental Materials 2020年第3期3卷 421-428页

作者： Lei Zhang Haitao Zhang Xiang Chu fangyan liu Chunsheng Guo Weiqing Yang Key Laboratory of Advanced Technologies of Materials(Ministry of Education) School of Materials Science and EngineeringSouthwest Jiaotong UniversityChengdu 610031China School of Physic Science&Technology Superconductivity and New Energy R&D CenterSouthwest Jiaotong UniversityChengdu Sichuan 610031China State Key Laboratory of Traction Power Southwest Jiaotong UniversityChengdu 610031China

Although the synthesis of novel nanostructured metal sulfides has been well established,further size-controllable optimization is still valuable to enhance their performance for various applications.Herein,a self-template method to size-controllably synthesize the hollow NiCo2S4 nanospheres is reported.Uniformly monodisperse Ni Co precursors with diameter widely ranging from 97 to 550 nm are controllably synthesized and subsequently transformed into hollow NiCo2S4 nanospheres through in situ sulfidation.Smaller nanoparticles’diameter results in the hollow NiCo2S4 nanospheres larger surface area and thinner shell thickness and hence provides much more electrochemical active sites as well as facilitate the ion and electron transfer.Consequently,the hollow NiCo2S4 nanospheres—used as the electrode materials in supercapacitors—achieve 19%enhancement of specific capacity from 484.8 to 575.1 C g-1 through lowering the 42.5%diameter of hollow NiCo2S4 nanospheres from 407 to 234 nm.Moreover,the hollow NiCo2S4 nanospheres with 234 nm diameter exhibit superior rate capacity indicated by 49%capacity retention from 1 to 50 A g-1 and excellent cycling stability(77%after 2000 cycles).Furthermore,this method is a potentially general strategy in the size-controllable synthesis of the metal sulfides hollow nanostructures and results in the remarkable electrochemical applications.

关键词： nickel-cobalt sulfides self-template method size-controllable supercapacitor

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Recent advances in carbon nanostructures prepared from carbon dioxide for high-performance supercapacitors

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Journal of Energy Chemistry 2021年第3期30卷 352-367页

作者： Chen Li Xiong Zhang Kai Wang Fangyuan Su Cheng-Meng Chen fangyan liu Zhong-Shuai Wu Yanwei Ma Institute of Electrical Engineering Chinese Academy of SciencesBeijing 100190China School of Engineering Sciences University of Chinese Academy of SciencesBeijing 100049China CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001ShanxiChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

The burgeoning global economy during the past decades gives rise to the continuous increase in fossil fuels consumption and rapid growth of CO_(2) emission,which demands an urgent exploration into green and sustainable devices for energy storage and power management.Supercapacitors based on activated carbon electrodes are promising systems for highly efficient energy harvesting and power supply,but their promotion is hindered by the moderate energy density compared with batteries.Therefore,scalable conversion of CO_(2) into novel carbon nanostructures offers a powerful alternative to tackle both issues:mitigating the greenhouse effect caused by redundant atmospheric CO_(2) and providing carbon materials with enhanced electrochemical performances.In this tutorial review,the techniques,opportunities and barriers in the design and fabrication of advanced carbon materials using CO_(2) as feedstock as well as their impact on the energy-storage performances of supercapacitors are critically examined.In particular,the chemical aspects of various Cv2 conversion reactions are highlighted to establish a detailed understanding for the science and technology involved in the microstructural evolution,surface engineering and porosity control of CO_(2)-converted carbon nanostructures.Finally,the prospects and challenges associated with the industrialization of CO_(2) conversion and their practical application in supercapacitors are also discussed.

关键词： Carbon materials Supercapacitors CO_(2)conversion Nanostructures

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Nitrogen-doped holey graphene nanoscrolls for high-energy and high-power supercapacitors

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Chinese Chemical Letters 2021年第2期32卷 914-917页

作者： Feng Su Shuanghao Zheng fangyan liu Xiong Zhang Fangyuan Su Zhong-Shuai Wu Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing J00049China Institute of Electrical Engineering Chinese Academy of SciencesBeijing 100190China CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Dalian National Laboratory for Clean Energy Chinese Academy of SciencesDalian 116023China

Porous structure and heteroatom doping are two key parameters for significantly boosting the capacitive performance of graphene-based materials.Herein,we report a facile approach to prepare onedimensional(ID) nitrogen-doped holey graphene nanoscrolls(NHGNSs) through cold quenching treatment of two-dimensional graphene oxide sheets,followed by thermal annealing in the successive atmosphere of NH3 and air.Benefiting from the synergy of the unique 1D tubular morphology,abundant nanoholes and nitrogen doping,the NHGNSs exhibit a high specific capacitance of 126 F/g at 1 A/g in ionic liquid electrolyte and excellent rate capability with 81% of the capacitance retained at 20 A/g.Furthermore,the fabricated symmetric supercapacitors based on NHGNSs achieve both high energy density of 53.5 Wh/kg at 875 W/kg and high power density of 17.5 kW/kg at 43.4 Wh/kg.The simple synthetic process and superior electrochemical performance suggest the great potential of NHGNSs for supercapacitor application.

关键词： Graphene nanoscrolls Nitrogen doping Holey grapheme Supercapacitors Ionic liquid

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