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Construction of phosphorus-doping with spontaneously developed Selenium vacancies: Inducing superior ion-diffusion kinetics in hollow Cu_(2)Se@C nanospheres for efficient sodium storage

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Journal of Energy Chemistry 2023年第2期77卷 227-238,I0007页

作者： Xiaoqing Ma Yadong Li Xiaojiang Long Hong-chuan Luo Chunping Xu Guangzhao Wang Wenxi Zhao School of Chemistry and Chemical Engineering Yangtze Normal UniversityChongqing 408100China Sports Medicine Center Department of Orthopedic SurgerySouthwest Hospitalthe 3rd Military Medical UniversityChongqing 400038China School of Electronic Information Engineering Key Laboratory of Extraordinary Bond Engineering and Advanced Materials Technology of ChongqingYangtze Normal UniversityChongqing 408100China Postgraduate Admission Office of Graduate School Southwest UniversityChongqing 400715China Vanadium and Titanium Resource Comprehensive Utilization Key Laboratory of Sichuan Province Panzhihua 617000SichuanChina

Achieving high-efficiency sodium storage in metal selenides is still severely constrained in consideration of their inferior electronic conductivity and inadequate Na^(+)insertion pathways and active sites.Heteroatom doping accompanied by spontaneously developed lattice defects can effectively tune electronic structure of metal selenides,which give a strong effect to motivate fast charge transfer and Na^(+)accessibility.Herein,we finely designed and successfully constructed a fascinating phosphorus-doped Cu_(2)Se@C hollow nanosphere with abundant vacancy defects(Cu_(2)P_(x)Se_(1-x)@C)through a combination strategy of selenization of Cu_(2)O nanosphere template,self-polymerization of dopamine,and subsequent phosphorization treatment.Such exquisite composite possesses enriched active sites,superior conductivity,and sufficient Na^(+)insertion channel,which enable much faster Na^(+)diffusion rates and more remarkable pseudocapacitive features,Satisfyingly,the Cu_(2)P_(x)Se_(1-x)@C composites manifest the supernormal sodium-storage capabilities,that is,a reversible capacity of 403.7 mA h g^(-1) at 1.0 A g^(-1) over 100 cycles,and an ultrastable cyclic lifespan over 1000 cycles at 20.0 A g^(-1) with a high capacity-retention of about249.7 mA h g^(-1).The phase transformation of the Cu_(2)P_(x)Se_(1-x)@C involving the intercalation of Na^(+)into Cu_(2)Se and the following conversion of NaCuSe to Cu and Na2Se were further demonstrated through a series of ex-situ characterization methods.DFT results demonstrate that the coexistence of phosphorusdoping and vacancy defects within Cu_(2)Se results in the reduction of Na^(+)adsorption energy from-1.47to-1.56 eV improving the conductivity of Cu_(2)Se to further accelerate fast Na^(+)mobility.

关键词： Phosphorus-doping Selenium vacancies Hollow Cu_(2)Se@C nanospheres Anode Sodium storage

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Selenium vacancies enable efficient immobilization and bidirectional conversion acceleration of lithium polysulfides for advanced Li-S batteries

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Nano Research 2022年第8期15卷 7234-7246页

作者： Yuanchang Li Zhenfang Zhou Yong Li Zhonghua Zhang Xiaosong Guo Jing Liu Changming Mao Zhenjiang Li Guicun Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China

Heterostructures composed of oxides and sulfides(nitrides or carbides)show great potential as sulfur host additives because of the strong adoptability of oxides and catalytic capability of sulfides towards the notorious lithium polysulfides(LiPSs).However,the migration and conversion pathway of LiPSs is seriously confined at a localized interface with inadequate active sites.In this work,the introduction of Selenium vacancies into VSe_(2−x)has been demonstrated to successfully synergize the adsorbability and catalytic reactions of LiPSs at an integrated functional surface.The N-doped carbon nanosheets-assembled flower architectures embedded with selenium vacancy-rich VSe_(2−x)and partial vanadium oxides have been controllably synthesized and employed as the cathode additives for lithium-sulfur(Li-S)batteries.Both the experiments and first-principle calculations reveal their strong adsorption to LiPSs and their bidirectional catalytic functionality towards the conversion between S8 and Li_(2)S.As expected,the charge and discharge kinetics of VSe_(2−x)containing sulfur cathodes is fundamentally improved(an outstanding rate capabilitiy with 693.7 mAh·g^(−1)at 2 C,a remarkable long-term cyclability within 1,000 cycles at 2 C with S loading 2.27 mg·cm^(−2),and an excellent areal capacity with 3.44 mAh·cm^(−2)within 100 cycles at 0.5 C).This work presents an effective resolution to couple the adsorbability and catalytic reactions of LiPSs at the material design perspective,and the insights on bidirectional catalytic functionality are of vital to develop functional materials for advanced Li-S batteries.

关键词： lithium-sulfur batteries Selenium vacancies vanadium selenide bidirectional catalysis conversion kinetics

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Lithiation-induced controllable vacancy engineering for developing highly active Ni_(3)Se_(2) as a high-rate and large-capacity battery-type cathode in hybrid supercapacitors

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Journal of Energy Chemistry 2023年第3期78卷 37-46,I0002页

作者： Yinna He Ting Liu Jiangnan Song Yiwei Wang Yuxiao Zhang Jie Feng Alan Meng Guicun Li Lei Wang Jian Zhao Zhenjiang Li College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Materials Science and Engineering College of Electromechanical EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

The poor rate capability and low capacity are huge barriers to realize the commercial applications of battery-type transition metal compounds(TMCs) cathode.Herein,numerous Se vacancy defects are introduced into the Ni_(3)Se_(2)lamellas by pre-lithiation technique,which can be acted as a novel class of battery-type cathode for hybrid supercapacitors.Appropriately modulating the contents of the preembedded lithium(Li) ions can induce a controllable vacancy content in the series of as-prepared products,effectively endowing a fast reaction kinetic and high activity for the cathode.Benefiting from the distinct design,the optimized cathode(Li2-Ni_(3)Se_(2)) presents a high specific capacity of 236 mA h g^(-1)at1 A g^(-1),importantly,it can still possess 117 mA h g^(-1)when the current density is increased up to 100A g^(-1),exhibiting relatively high rate capability.It is much superior to other battery-type TMC cathodes reported in previous studies.Moreover,the cathode also shows the excellent cycling stability with 92%capacity retention after 3,000 cycles.In addition,a hybrid supercapacitor(HSC) is assembled with the obtained Li2-Ni_(3)Se_(2)as the cathode and active carbon(AC) as the anode,which delivers a high energy density of 77 W h kg^(-1)at 4 kW kg^(-1)and long-term durability(90% capacitance retention after 10,000 cycles).Therefore,the strategy not only provides an effective way to realize the controllable vacancy content in TMCs for achieving high-perfo rmance cathodes for HSC,but also further promotes their large-scale applications in the energy storage fields.

关键词： Pre-lithiation Selenium vacancies High-rate Battery-type cathode Hybrid supercapacitor

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