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Reversible solid-liquid conversion enabled by self-capture effect for stable non-flow zinc-bromine batteries

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Green Energy & Environment 2024年第6期9卷 1035-1044页

作者： Xixi Zhang Xiaoke Wang guangmeng qu Tairan Wang Xiliang Zhao Jun Fan Cuiping Han Xijin Xu Chunyi Zhi Hongfei Li School of Physics and Technology University of JinanShandong250022China Songshan Lake Materials Laboratory DongguanGuangdong523808China Department of Materials Science and Engineering City University of Hong Kong83 Tat Chee AvenueHong KongChina Faculty of Materials Science and Engineering and Low Dimensional Energy Materials Research Center Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhenGuangdong518055China School of System Design and Intelligent Manufacturing Southern University of Science and TechnologyShenzhenGuangdong518055China

Non-flow aqueous zinc-bromine batteries without auxiliary components(e.g.,pumps,pipes,storage tanks)and ion-selective membranes represent a cost-effective and promising technology for large-scale energy ***,they generally suffer from serious diffusion and shuttle of polybromide(Br^(-),Br^(3-))due to the weak physical adsorption between soluble polybromide and host carbon materials,which results in low energy efficiency and poor cycling ***,we develop a novel self-capture organic bromine material(1,10-bis[3-(trimethylammonio)propyl]-4,4'-bipyridinium bromine,NVBr4)to successfully realize reversible solid complexation of bromide components for stable non-flow zinc-bromine battery *** quaternary ammonium groups(NV^(4+)ions)can effectively capture the soluble polybromide species based on strong chemical interaction and realize reversible solid complexation confined within the porous electrodes,which transforms the conventional“liquid-liquid”conversion of soluble bromide components into“liquid-solid”model and effectively suppresses the shuttle ***,the developed non-flow zinc-bromide battery provides an outstanding voltage platform at 1.7 V with a notable specific capacity of 325 mAh g^(-1)NVBr4(1 A g^(-1)),excellent rate capability(200 mAh g^(-1)NVBr4 at 20 A g^(-1)),outstanding energy density of 469.6 Wh kg^(-1)and super-stable cycle life(20,000 cycles with 100%Coulombic efficiency),which outperforms most of reported zinc-halogen *** mechanism analysis and DFT calculations demonstrate that the chemical interaction of quaternary ammonium groups and bromide species is the main reason for suppressing the shuttle *** developed strategy can be extended to other halogen batteries to obtain stable charge storage.

关键词： Solid-liquid conversion Self-capture Non-ﬂow zinc-bromine batteries quaternary ammonium

Highly robust zinc metal anode directed by organic–inorganic synergistic interfaces for wearable aqueous zinc battery

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SmartMat 2024年第1期5卷 135-146页

作者： Xixi Zhang Chuanlin Li guangmeng qu Chenggang Wang Shunshun Zhao Tongkai Wang Na Li Xiaojuan Li Xijin Xu School of Physics and Technology University of JinanJinanChina School of Chemistry and Chemical Engineering Shandong UniversityJinanChina State Key Laboratory of Chemical Resource Engineering Beijing Key Laboratory of Electrochemical Process and Technology of MaterialsBeijing University of Chemical TechnologyBeijingChina

Flexible aqueous zinc batteries(FAZBs)with high safety and environmental friendliness are promising smart power sources for smart wearable ***,the bare zinc anode usually suffers from damnable dendrite growth and rampant side reaction on the surface,greatly impeding practical applications in ***,a composite polymer interface layer is artificially self‐assembled on the surface of the zinc anode by graft‐modified fluorinated monomer(polyacrylic acid‐2‐(Trifluoromethyl)propenoic acid,PAA‐TFPA),on which an organic–inorganic hybrid(PAA‐Zn/ZnF2)solid electrolyte interface(SEI)with excellent ionic conductivity is formed by interacting with Zn2+.Both the pouch cell and fiber zinc anode exhibit excellent plating/stripping reversibility after protecting by this organic–inorganic SEI,which can be stably cycled more than 3000 h in symmetric Zn||Zn cells or 550 h in fiber Zn||Zn ***,this interface layer preserves zinc anode with excellent mechanical durability under various mechanical deformation(stably working for another 1200 h after bending 100 h).The corresponding PAA‐Zn/ZnF2@Zn||MnO2 full cell displays an ultra‐long life span(79%capacity retention after 3000 cycles)and mechanical robustness(85%of the initial capacity for another 3000 cycles after bending 100 times).More importantly,the as‐assembled cells can easily power smart wearable devices to monitor the user's health condition.

关键词： hybrid SEI mechanical durability wearable zinc battery zinc anode

Nickel/cobalt based materials for supercapacitors

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Chinese Chemical Letters 2018年第12期29卷 1731-1740页

作者： Chenggang Wang Pengxiao Sun guangmeng qu Jiangmei Yin Xijin Xu School of Physics and Technology University of Jinan

The electrode materials as the key component of supercapacitors have attracted considerable research interests, especially for nickel/cobalt based materials by virtue of their superior electrochemical performance with multiple oxidation states for richer redox reactions, abundant natural resources, lower prices and toxicity. There are many advanced electrodes based on the nickel/cobalt materials exploited for the application of supercapacitors, however, some controversial statements have induced some confusion. Herein, we refine the mechanism of energy storage for the nickel/cobalt based materials for supercapacitors and reclassify them into battery-type materials with the corresponding devices named as hybrid supercapacitors.

关键词： Nickel/cobalt based materials Battery-type materials Pseudocapacitors EDLCs Hybrid supercapacitors

Defect engineering in Co-doped Ni_(3)S_(2) nanosheets as cathode for high-performance aqueous zinc ion battery

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Journal of Materials Science & Technology 2022年第23期118卷 199-207页

作者： Xiaojuan Li Shunshun Zhao guangmeng qu Xiao Wang Peiyu Hou Gang Zhao Xijin Xu School of Physics and Technology University of JinanJinan 250022China School of Electronic and Information Engineering(Department of Physics) Qilu University of Technology(Shandong Academy of Sciences)Jinan 250353China

With the merits of low cost,environmental benignity,and high safety,aqueous zinc ion batteries(AZIBs)have great potential in the field of energy *** this paper,we craft a Co-doped Ni3 S2 with abundant sulfur vacancies as effective cathode materials(Co-Ni_(3) S_(2-x)) for AZIBs by hydrothermal and chemical reduction ***,cobalt doping and abundant sulfur vacancies can effectively increase the conductivity and the number of active sites for electrochemical reactions,which gives the Co-Ni_(3) S_(2-x) electrode the outstanding capability to energy *** coupling Co-Ni_(3) S_(2-x) cathode with Zn anodes to assemble alkaline AZIBs,the Co-Ni_(3) S_(2-x)//Zn full battery exhibits excellent specific capacity(183.9 mAh g^(-1) at 1 A g^(-1),based on cathode mass) and extraordinary cycling durability(72.9% capacity retention after 6000 cycles).First-principles calculations based on density functional theory(DFT) confirm that the Co-Ni_(3) S_(2-x) electrode has strong energy storage capacity and electrochemical *** results provide an extremely significant reference in designs of self-supported bimetallic sulfide nanosheets,which have promising applications in high-performance energy storage devices.

关键词： Zinc ion battery Metal doping Sulfur vacancy Ni_(3)S_(2)

An integrated approach to configure rGO/VS_(4)/S composites with improved catalysis of polysulfides for advanced lithium-sulfur batteries

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Chinese Chemical Letters 2022年第8期33卷 3909-3915页

作者： Feng Li Lu Wang guangmeng qu Peiyu Hou Linglong Kong Jinzhao Huang Xijin Xu School of Physics and Technology University of JinanJi'nan 250022China College of Chemistry and Material Science Shandong Agricultural UniversityTaian 271018China State Forestry and Grassland Administration Key Laboratory of Silviculture in Downstream Areas of the Yellow River School of ForestryShandong Agricultural UniversityTaian 271018China

Lithium-sulfur(Li-S)battery is labeled as a promising high-energy-density battery system,but some inherent drawbacks of sulfur cathode materials using relatively complicated techniques impair the practical ***,an integrated approach is proposed to fabricate the high-performance rGO/VS_(4)/S cathode composites through a simple one-step solvothermal method,where nano sulfur and VS_(4) particles are uniformly distributed on the conductive rGO *** and sulfiphilic VS_(4)provide electron transfer skeleton and physical/chemical anchor for soluble lithium polysulfides(LiPS).Meanwhile,VS_(4) could also act as an electrochemical mediator to efficiently enhance the utilization and reversible conversion of ***,the rGO/VS_(4)/S composites maintain a high reversible capacity of 969 mAh/g at 0.2 C after 100 cycles,with a capacity retention rate of 82.3%.The capacity fade rate could lower to 0.0374%per cycle at 1 ***,capacity still sustains 795 m Ah/g after 100 cycles in the relatively high-sulfurloading battery(6.5 mg/cm^(2)).Thus,the suggested method in configuring the sulfur-based composites is demonstrated a simple and efficient strategy to construct the high-performance Li-S batteries.

关键词： Lithium-sulfur batteries rGO/VS_(4)/S composites In-situ synthesis Adsorbing Catalysis

ZIF-67 derived hollow Ni-Co-Se nano-polyhedrons for flexible hybrid supercapacitors with remarkable electrochemical performances

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Chinese Chemical Letters 2020年第7期31卷 2007-2012页

作者： guangmeng qu Xixi Zhang Guotao Xiang Yunrui Wei Jiangmei Yin Zonghua Wang Xiaoli Zhang Xijin Xu School of Physics and Technology University of JinanJi'Nan 250022China State Centre for Inrernational Cooperation on Designer Low-Carbon&Environmental Materials School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001China

Nano-polyhedral NiSe2/CoSe2(Ni-Co-Se) with hollow architectures are synthesized by selenizing the precursors of Ni-Co bimetallic hydroxides that are directly derived from *** as-fabricated Ni-Co-Se electrodes exhibit high specific capacitance of 1668 F/g at 1 A/g accompanying with outstanding rate capability(about 82.8% retention of the initial capacity at 20 A/g).The corresponding Ni-Co-Se//AC all-solid-state hybrid supercapacitors are assembled by directly using the Ni-Co-Se on carbon fabric as the positive electrode,which deliver high energy density and power density(38.5 Wh/kg at 802.1 W/kg,32.0 Wh/kg at 8008.8 W/kg),excellent cyclic stability(82.3% retention after 5000 cycle) and robust mechanical flexibility(no obvious attenuation at bending to different angles).This work will provide a new and smart route for constructing transition metal selenides for supercapacitor devices.

关键词： Ni-Co-Se Nano-polyhedrons Hybrid supercapacitors

Hollow polyhedron structure of amorphous Ni-Co-S/Co(OH)_(2) for high performance supercapacitors

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Chinese Chemical Letters 2021年第8期32卷 2453-2458页

作者： Xixi Zhang guangmeng qu Zonghua Wang Guotao Xiang Shuhua Hao Xiaoke Wang Xijin Xu Wenxuan Ma Gang Zhao School of Physics and Technology University of JinanJi’nan 250022China

In power storage technology,ion exchange is widely used to modify the electronic structures of electrode materials to stimulate their electrochemical ***,we proposed a multistep ion exchange(cation exchange and anion exchange) strategy to synthesize amorphous Ni-Co-S and β-Co(OH)_(2) hybrid nanomaterials with a hollow polyhedron *** synergistic effects of different components and the remarkable superiorities of hollow structure endow Ni-Co-S/Co(OH)_(2) electrode with outstanding electrochemical performance,including ultra-high specific capacity(1440.0 C/g at 1 A/g),superior capacitance retention rate(79.1% retention at 20 A/g) and long operating lifespan(81.4% retention after5000 cycles).Moreover,the corresponding hybrid supercapacitor enjoys a high energy density of 58.4 Wh/kg at the power density of 0.8 kW/kg,and a decent cyclability that the capacitances are maintained at80.8% compared with the initial *** research presents a high-performance electrode material and provides a promising route for the construction of electrode materials for supercapacitors with both structural and component advantages.

关键词： Ion exchange Amorphous β-Co(OH)2 Hollow polyhedron Supercapacitor

Amorphous Ni-Co-S nanocages assembled with nanosheet arrays as cathode for high-performance zinc ion battery

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Chinese Chemical Letters 2022年第6期33卷 3272-3276页

作者： Na Li guangmeng qu Xixi Zhang Shunshun Zhao Chenggang Wang Gang Zhao Peiyu Hou Xijin Xu School of Physics and Technology University of JinanJi’nan 250022China Key Laboratory of Colloid and Interface Chemistry Ministry of Education School of Chemistry and Chemical Engineering Shandong UniversityJi’nan 250100China School of Electronic and Information Engineering(Department of Physics) Qilu University of Technology(Shandong Academy of Sciences)Ji’nan 250353China

The selection and development of cathode of alkaline zinc batteries(AZBs)is still hindered and often leads to poor rate capability and short cycle ***,amorphous hollow nickel-cobalt-based sulfides nanocages with nanosheet arrays(AM-NCS)are designed and constructed with ZIF-67 as the selftemplate to exchange with Ni^(2+) and S^(2-) by using a two-step ion exchange *** synthesized AM-NCS possess the high specific capacity(160 m Ah/g at 2 A/g),and the assembled battery has excellent rate performance(146 m Ah/g reversible capacity at 5 A/g).The assembled device has excellent rate performance(155 m Ah/g at 2 A/g)and long cycling stability(7000 cycles,62.5%of initial capacity).The excellent electrochemical properties of the electrode materials are mainly attributed to the unique structure,in particular,polyhedron structure with hollow structure can improve the cyclic stability,and the amorphous structure can expose more reactive sites on the surfaces of nickel,cobalt and *** work provides a new strategy for the design and fabrication of high performance cathode materials for AZBs.

关键词： Alkaline zinc batteries Metal sulfide Hierarchical structures Amorphous structure Hollow structure

Dual-functional Ni Co2S4 polyhedral architecture with superior electrochemical performance for supercapacitors and lithium-ion batteries

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Science Bulletin 2020年第6期65卷 443-451,M0003页

作者： Guotao Xiang Yao Meng guangmeng qu Jiangmei Yin Bing Teng Qin Wei Xijin Xua School of Physics and Technology.University of Jinan Jinan 250022China College of Physics Qingdao UniversityQingdao 266071China Shandong University of Traditional Chinese Medicine Jinan 250355China Collaborative Innovation Center of Light Manipulations and Applications Shandong Normal UniversityJinan 250358China

Dual-functional NiCo2S4 polyhedral architectures with outstanding electrochemical performance for supercapacitors and lithium-ion batteries(LIBs) have been rationally designed and successfully synthesized by a hydrothermal method. The as-synthesized NiCo2S4 electrode for supercapacitor exhibits an outstanding specific capacitance of 1298 Fg-1 at 1 A g-1 and an excellent rate capability of ~80.4% at20 A g-1. Besides, capacitance retention of 90.44% is realized after 8000 cycles. In addition, the NiCo2S4 as anode in LIBs delivers high initial charge/discharge capacities of 807.6 and 972.8 m Ah g-1 at 0.5 C as well as good rate capability. In view of these points, this work provides a feasible pathway for assembling electrodes and devices with excellent electrochemical properties in the next generation energy storage applications.

关键词： NiCo2S4 Polyhedron Supercapacitor Lithium-ion batteries