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Single-atom catalysis enables long-life, high-energy lithium-sulfur batteries

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Nano Research 2020年第7期13卷 1856-1866页

作者： Zechao Zhuang Qi Kang Dingsheng Wang Yadong Li Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Polymer Science and Engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingShanghai Jiao Tong UniversityShanghai 200240China

With high energy density and low material cost,lithium sulfur batteries(LSBs)emerge quite expeditiously as a fascinating energy storage system over the past decade.Broad applications of LSBs ranging from electric vehicles to stationary grid storage seem rather bright in recent literatures.However,there still exist many pressing challenges to be addressed because we do not yet fully understand and control the electrode-electrolyte interface chemistries during battery operation,such as polysulide shuttling and poor utilization of active sulfur.Single-atom catalysts(SACs)pave new possibilities of tackling the tough issues due to their decent applicability in the atomic-level identification of structure-activity relationships and reaction mechanism,as well as their structural tunability with atomic precision.This review comprehensively summarizes the very recent advances in utilization of highly active SACs for LSBs by stating and discussing the related publications,which involves catalyst synthesis routes,battery pertormance,catalytic mechanisms,optimization strategies,and promises to achieve long-lite,high-energy LSBs.We see that endeavors to employ SACs to modify sulfur cathode have allowed efficient polysulfide conversion and confinement,leading to the minimization of shuttle effect.Parallel efforts are being devoted to extending the scope of SACs to cell separator and lithium metal anode in order to unlock the full potential of LSBs.We also obtain mechanistic insights into battery chemistries and nature of SACs in their strong interactions with polysulfides through advanced in situ characterizations documented.Overall,acceleration in the development of LSBs by introducing SACs is noticeable,and this cutting edge needs more attentions to further promoting the design of better LSBs.

关键词： single-atom catalysis lithium-sulfur battery polysulfide conversion shuttle effect atomic-level insight

Dielectric polymer based electrolytes for high-performance all-solid-state lithium metal batteries

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Journal of Energy Chemistry 2022年第6期31卷 194-204,I0006页

作者： Qi Kang Yong Li Zechao Zhuang Dingsheng Wang Chunyi Zhi Pingkai Jiang Xingyi Huang Department of Polymer Science and Engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingState Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200240China Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology University of BremenBremen 28359Germany Department of Chemistry Tsinghua UniversityBeijing 100084China Department of Materials Science and Engineering City University of Hong KongHong Kong 999077China

Solid polymer electrolytes (SPEs) are urgently required for achieving practical all-solid-state lithium metal batteries (ASSLMBs) but remain plagued by low ionic conductivity.Herein,we propose a strategy of salt polarization to fabricate a highly ion-conductive SPE by employing a high-dielectric polymer that can interact strongly with lithium salts.Such a polymer with large dipole moments can guide lithium cations (Li^(+)) to be arranged along the chain,forming a continuous pathway for Li^(+) hopping within the SPE.The as-fabricated SPE,poly(vinylidene difluoride)(PVDF)-LiN(SO_(2)F)_(2)(LiFSI),has an extraordinarily high dielectric constant (up to 10^(8)) and ultrahigh ionic conductivity (0.77×10^(-3)S cm^(-1)).Based on the PVDF–LiFSI SPE,the assembled Li metal symmetrical cell shows excellent Li plating/stripping reversibility at 0.1 m A cm^(-2),0.1 m Ah cm^(-2)over 1500 h^(-1) the ASS LiFePO_(4) batteries deliver long-term cycling stability at 1 C over 350 cycles (2.74 mg cm^(-2)) and an ultralong cycling lifespan of over 2600 h(100 cycles) with high loading (11.5 mg cm^(-2)) at 28°C.First-principles calculations further reveal the ion-dipole interactions-controlled conduction of Li^(+) in PVDF–LiFSI SPE along the PVDF chain.This work highlights the critical role of dielectric permittivity in SPE,and provides a promising path towards high-energy,long-cycling lifespan ASSLMBs.

关键词： Salt polarization High dielectric High-loading All-solid-state Lithium metal battery 2600 h lifespan

Dislocation-strained MoS_(2)nanosheets for high-efficiency hydrogen evolution reaction

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Nano Research 2022年第6期15卷 4996-5003页

作者： Shihao Wang Longlu Wang Lingbin Xie Weiwei Zhao Xia Liu Zechao Zhuang YanLing zhuang Jing Chen Shujuan Liu Qiang Zhao College of Electronic and Optical Engineering Nanjing University of Posts and TelecommunicationsNanjing 210023China Key Laboratory for Organic Electronics and Information Displays and Jiangsu Key Laboratory for Biosensors Institute of Advanced Materials(IAM)and Institute of Flexible Electronics(Future Technology)Nanjing University of Posts and TelecommunicationsNanjing 210023China College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071China Department of Chemistry Tsinghua UniversityBeijing 100084China

Defect engineering is one of the effective strategies to optimize the physical and chemical properties of molybdenum disulfide(MoS_(2))to improve catalytic hydrogen evolution reaction(HER)performance.Dislocations,as a typical defect structure,are worthy of further investigation due to the versatility and sophistication of structures and the influence of local strain effects on the catalytic performance.Herein,this study adopted a low-temperature hydrothermal synthesis strategy to introduce numerous dislocation-strained structures into the in-plane and out-of-plane of MoS_(2)nanosheets.Superior HER catalytic activity of 5.85 mmol·g^(−1)·h^(−1)under visible light was achieved based on the high-density dislocations and the corresponding strain field.This work paves a new pathway for improving the catalytic activity of MoS_(2)via a dislocation-strained synergistic modulation strategy.

关键词： molybdenum disulfide dislocation strain hydrogen evolution reaction

Designing multi-heterogeneous interfaces of Ni-MoS_(2)@NiS_(2)@Ni_(3)S_(2)hybrid for hydrogen evolution

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Nano Research 2024年第6期17卷 4782-4789页

作者： Haoxuan Yu Junan Pan Yuxin Zhang Longlu Wang Huachao Ji Keyu Xu Ting Zhi Zechao Zhuang College of Electronic and Optical Engineering&College of Flexible Electronics(Future Technology) Nanjing University of Posts&Telecommunications(NJUPT)Nanjing 210023China Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA

The transition metal chalcogenides represented by MoS_(2)are the ideal choice for non-precious metal-based hydrogen evolution catalysts.However,whether in acidic or alkaline environments,the catalytic activity of pure MoS_(2)is still difficult to compete with Pt.Recent studies have shown that the electronic structure of materials can be adjusted by constructing lattice-matched heterojunctions,thus optimizing the adsorption free energy of intermediates in the catalytic hydrogen production process of materials,so as to effectively improve the electrocatalytic hydrogen production activity of catalysts.However,it is still a great challenge to prepare heterojunctions with lattice-matched structures as efficient electrocatalytic hydrogen production catalysts.Herein,we developed a one-step hydrothermal method to construct Ni-MoS_(2)@NiS_(2)@Ni_(3)S_(2)(Ni-MoS_(2)on behalf of Ni doping MoS_(2))electrocatalyst with multiple heterogeneous interfaces which possesses rich catalytic reaction sites.The Ni-MoS_(2)@NiS_(2)@Ni_(3)S_(2)electrocatalyst produced an extremely low overpotential of 69.4 mV with 10 mA·cm^(−2)current density for hydrogen evolution reaction(HER)in 1.0 M KOH.This work provides valuable enlightenment for exploring the mechanism of HER enhancement to optimize the surface electronic structure of MoS_(2),and provides an effective idea for constructing rare metal catalysts in HER and other fields.

关键词： MoS_(2) heterojunctions multiple heterogeneous interfaces hydrogen evolution

Stabilizing effects of atomic Ti doping on high-voltage high-nickel layered oxide cathode for lithium-ion rechargeable batteries

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Nano Research 2022年第5期15卷 4091-4099页

作者： Yong Cheng Yan Sun Changting Chu Limin Chang Zhaomin Wang Dongyu Zhang Wanqiang Liu Zechao Zhuang Limin Wang Key Laboratory of Preparation and Applications of Environmental Friendly Materials(Ministry of Education) Jilin Normal UniversityChangchun 130103China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of materials science and engineering Changchun University of Science and TechnologyChangchun 130022China Department of Chemistry Tsinghua UniversityBeijing 100084China

High-voltage high-nickel lithium layered oxide cathodes show great application prospects to meet the ever-increasing demand for further improvement of the energy density of rechargeable lithium-ion batteries(LIBs)mainly due to their high output capacity.However,severe bulk structural degradation and undesired electrode-electrolyte interface reactions seriously endanger the cycle life and safety of the battery.Here,2 mol%Ti atom is used as modified material doping into LiNi_(0.8)Co_(0.2)Mn_(0.2O2)(NCM)to reform LiNi_(0.6)Co_(0.2)Mn_(0.18)Ti_(0.02)O_(2)(NCM-Ti)and address the long-standing inherent problem.At a high cut-off voltage of 4.5 V,NCM-Ti delivers a higher capacity retention ratio(91.8%vs.82.9%)after 150 cycles and a superior rate capacity(118 vs.105 mAh·g^(-1))at the high current density of 10 C than the pristine NCM.The designed high-voltage full battery with graphite as anode and NCM-Ti as cathode also exhibits high energy density(240 Wh·kg^(-1))and excellent electrochemical performance.The superior electrochemical behavior can be attributed to the improved stability of the bulk structure and the electrode-electrolyte interface owing to the strong Ti-O bond and no unpaired electrons.The in-situ X-ray diffraction analysis demonstrates that Ti-doping inhibits the undesired H2-H3 phase transition,minimizing the mechanical degradation.The ex-situ TEM and X-ray photoelectron spectroscopy reveal that Ti-doping suppresses the release of interfacial oxygen,reducing undesired interfacial reactions.This work provides a valuable strategic guideline for the application of high-voltage high-nickel cathodes in LIBs.

关键词： lithium-ion battery high-voltage high-nickel cathode Ti-doping structural stability interface stability

Moirésuperlattice engineering of two-dimensional materials for electrocatalytic hydrogen evolution reaction

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Nano Research 2023年第7期16卷 8712-8728页

作者： Yang Li Yuqi Hua Ning Sun Shijie Liu Hengxu Li Cheng Wang Xinyu Yang Zechao Zhuang Longlu Wang College of Electronic and Optical Engineering&College of Flexible Electronics(Future Technology) Nanjing University of Posts and Telecommunications(NJUPT)Nanjing 210023China Department of Chemistry Tsinghua UniversityBeijing 100084China

Vertically stacking two-dimensional(2D)materials with small azimuthal deviation or lattice mismatch generate distinctive global structural periodicity and symmetry,revealed as the moirésuperlattices(MSLs).Manipulating the interlayer twist angle enables the modification of the electronic structure of 2D materials to explore the advanced applications.Although extraordinary progress has been achieved in the unique structure and emergent properties of MSLs,the investigation of the catalytic applications of MSLs materials is still in its infancy.It is therefore very urgent to summarize the advanced development of MSLs in the field of catalysis.In this review,we firstly summarize the advanced fabrication and high-resolution characterization techniques of the MSLs materials,as well as their novel properties related to catalysis represented by electrocatalytic hydrogen evolution reaction(HER).Then,all the MSLs materials such as MoS_(2),WS_(2),and Ru serving as electrocatalysts for HER are further reviewed in detail.Finally,we outline the current challenges as well as the experimental and theoretical strategies to advance the development of function-oriented MSLs materials for catalysis.This review aims to provide profound insight into the wide applications of this novel material platform in catalytic field.

关键词： moirésuperlattices two-dimensional(2D)materials fabrication characterization properties hydrogen evolution reaction(HER)

Diverse atomic structure configurations of metal-doped transition metal dichalcogenides for enhancing hydrogen evolution

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Nano Research 2024年第5期17卷 3586-3602页

作者： Longlu Wang Yuxin Zhang Chen Gu Haoxuan Yu Yanling zhuang Zechao Zhuang College of Electronic and Optical Engineering and College of Flexible Electronics(Future Technology) Jiangsu Province Engineering Research Center for Fabrication and Application of Special Optical Fiber Materials and DevicesNanjing University of Posts and TelecommunicationsNanjing 210023China Department of Chemical Engineering Columbia UniversityNew YorkNY 10027USA

Doping foreign metal atoms into the substrate of transition metal dichalcogenides(TMDs)enables the formation of diverse atomic structure configurations,including isolated atoms,chains,and clusters.Therefore,it is very important to reasonably control the atomic structure and determine the structure-activity relationship between the atomic configurations and the hydrogen evolution reaction(HER)performance.Although numerous studies have indicated that doping can yield diverse atomic structure configurations,there remains an incomplete understanding of the relationship between atomic configurations within the lattice of TMDs and their performance.Here,diverse atomic structure configurations of adsorptive doping,substitutional doping,and TMDs alloys are summarized.The structure-activity relationship between different atomic configurations and HER performance can be determined by micro-nanostructure devices and density functional theory(DFT)calculations.These diverse atomic structure configurations are of great significance for activating the inert basal plane of TMDs and improving the catalytic activity of HER.Finally,we have summarized the current challenges and future opportunities,offering new perspectives for the design of highly active and stable metal-doped TMDs catalysts.

关键词： transition metal dichalcogenides(TMDs) dopant effect diverse atomic structure configurations hydrogen evolution reaction(HER)

Constructing stable Li-solid electrolyte interphase to achieve dendrites-free solid-state battery:A nano-interlayer/Li prereduction strategy

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Nano Research 2022年第8期15卷 7180-7189页

作者： Yajun Niu Zhaozhe Yu Yongjian Zhou Jiawen Tang Maoxin Li Zechao Zhuang Yan Yang Xiao Huang Bingbing Tian Guangxi Key Laboratory of Manufacturing Systems and Advanced Manufacturing Technology Guilin University of Electronic TechnologyGuilin 541004China International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China Department of Chemistry Tsinghua UniversityBeijing 100084China Collaborative Innovation Center for Vessel Pollution Monitoring and Control Dalian Maritime UniversityDalian 116026China

Solid-state batteries based on Li and nonflammable solid-state electrolytes(SSEs)have aroused the attention of numerous researchers because of their absolute safety and potentially high energy density.Most SSEs after coming into contact with Li are reduced,which leads to high interfacial charge-transfer impedance and dendrites formation.In this study,an“interlayer-Li pre-reduction strategy”was proposed to solve the above problem of reduction.An intermediate layer was introduced between solid electrolyte and Li,and it reacted with Li to produce a stable and ion-conductive interphase.Cubic garnet-type Nb-doped Li_(7)La_(3)Zr_(2)O_(12)(Nb-LLZO)was selected as an example solid electrolyte since it is characterized by high ionic conductivity,feasible preparation under ambient conditions,as well as low cost.The high impedance arising from the reduction at the Nb-LLZO|Li interface has limited its application.In this paper,a nano-scale Li phosphorus oxynitride(LiPON)layer was deposited on the Nb-LLZO pellets through radio frequency(RF)magnetron sputtering,which pre-reacted with Li in-situ to produce a lithiophilic,electronically insulating,and ionic conductive interphase.The produced interphase significantly inhibited the reduction of Nb5+against Li and the formation and propagation of Li dendrites.It is noteworthy that Li|LiPON|Nb-LLZO|LiPON|Li cells stably cycled for over 2,000 h without any short circuit.This study emphasizes and demonstrates the significance of the pre-conversion of modification layer between unstable SSE and Li metal to improve interfacial stability.

关键词： Nb-doped Li_(7)La_(3)Zr_(2)O_(12)(Nb-LLZO) conversion reaction Li phosphorus oxynitride(LiPON) interfacial reduction solid-state battery

Manipulating dielectric property of polymer coatings toward highretention-rate lithium metal full batteries under harsh critical conditions

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Nano Research 2023年第7期16卷 9240-9249页

作者： Qi Kang Zechao Zhuang Yong Li Yinze Zuo Jian Wang Yijie Liu Chaoqun Shi Jie Chen Hongfei Li Pingkai Jiang Xingyi Huang Department of Polymer Science and Engineering Shanghai Key Laboratory of Electrical Insulation and Thermal AgeingSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Tsinghua UniversityBeijing 100084China Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology University of BremenBremen 28359Germany Institute for Sustainable Energy/College of Sciences Shanghai UniversityShanghai 200444China Helmholtz Institute Ulm(HIU) Ulm D89081Germany School of Electrical Engineering Xi’an Jiaotong UniversityXi’an 710049China

Lithium(Li)metal batteries(LMBs)can potentially deliver much higher energy density but remain plagued by uncontrollable Li plating with dendrite growth,unstable interfaces,and highly abundant excess Li(>50 mAh·cm^(-2)).Herein,different from the artificial layer or three-dimensional(3D)matrix host constructions,various dielectric polymers are initially well-comprehensively investigated from experimental characterizations to theoretical simulation to evaluate their functions in modulating Li ion distribution.As a proof of concept,a 3D interwoven high dielectric functional polymer(HDFP)nanofiber network with polar C-F dipole moments electrospun on copper(Cu)foil is designed,realizing uniform and controllable Li deposition capacity up to 5.0 mAh·cm^(-2),thereby enabling stable Li plating/stripping cycling over 1400 h at 1.0 mA·cm^(-2).More importantly,under the highcathode loading(~3.1 mAh·cm^(-2))and only 0.6×excess Li(N/P ratio of 1.6),the full cells retain capacity retention of 97.4%after 200 cycles at 3.36 mA·cm^(-2)and achieve high energy density(297.7 Wh·kg^(-1)at cell-level)under lean electrolyte conditions(15μL),much better than ever-reported literatures.Our work provides a new direction for designing high dielectric polymer coating toward high-retention-rate practical Li full batteries.

关键词： high dielectric functional polymer nanofiber Li metal full cell low N/P ratio high-retention capacity