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Chinese Journal of Chemical Engineering 2024年第3期67卷 58-67页

作者： Deqing He Zihao Xie Qian Yang Wei Wang Chao Su School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212100China State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

The sluggish redox kinetics of polysulfides in lithium-sulfur(Li-S)batteries are a significant obstacle to their widespread adoption as energy storage devices.However,recent studies have shown that tungsten oxide(WO_(3))can facilitate the conversion kinetics of polysulfides in Li-S batteries.Herein,we fabricated host materials for sulfur using nitrogen-doped carbon nanotubes(N-CNTs)and WO_(3).We used low-cost components and simple procedures to overcome the poor electrical conductivity that is a disadvantage of metal oxides.The composites of WO_(3) and N-CNTs(WO_(3)/N-CNTs)create a stable framework structure,fast ion diffusion channels,and a 3D electron transport network during electrochemical reaction processes.As a result,the WO_(3)/N-CNT-Li2S6 cathode demonstrates high initial capacity(1162 mA·h·g^(-1) at 0.5℃),excellent rate performance(618 mA·h·g^(-1) at 5.5℃),and a low capacity decay rate(0.093%up to 600 cycles at 2℃).This work presents a novel approach for preparing tungsten oxide/carbon composite catalysts that facilitate the redox kinetics of polysulfide conversion.

关键词： Li-S batteries Composites Ion diffusion channels 3D electron transport network redox kinetics

Three-in-one LaNiO_(3) functionalized separator boosting electrochemical stability and redox kinetics for high-performance Li-S battery

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Journal of Energy Chemistry 2023年第7期82卷 581-591,I0013页

作者： Weiyu Wang Mingxiu Hou Fangqian Han Di Yu Jie Liu Qian Zhang Fengli Yu Lei Wang Maoshuai He State Key Laboratory Base of Eco-chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Weifang Key Laboratory of Green Processing of Separator for Chemical Power Sources School of Chemistry and EngineeringWeifang Vocational CollegeWeifang 261108ShandongChina Shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

The lithium-sulfur(Li-S)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy density.However,the poor redox kinetics and the"shuttle effect"of polysulfides severely restrict the use of Li-S batteries in practical applications.Herein,a novel bimetallic LaNiO_(3) functional material with high electrical conductivity and catalytic property is prepared to act as a high-efficiency polysulfide shuttling stopper.The three LaNiO_(3) samples with different physical/chemical characteristics are obtained by controlling the calcination temperature.In conjunction with the high electrical conductivity and excellent catalytic properties of the as-prepared materials,the appropriate chemisorption toward polysulfides offers great potential to enhance electrochemical stability for highperformance Li-S batteries.Particularly,the Li-S cell with the separator modified by such functional material gives a specific capacity of 658 mA h g^(-1) after 500 cycles at a high current density of 2 C.Even with high sulfur loading of 6.05 mg cm^(-2),the Li-S battery still exhibits an areal specific capacity of 2.81 m A h cm^(-2)after 150 cycles.This work paves a new avenue for the rational design of materials for separator modification in high-performance Li-S batteries.

关键词： Li-S battery Functional separator Catalytic property Electrochemical stability redox kinetics

Field-assisted electrocatalysts spark sulfur redox kinetics:From fundamentals to applications

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Interdisciplinary Materials 2023年第3期2卷 390-415页

作者： Hongtai Li Yanguang Li Liang Zhang Zhongwei Chen Xueliang Sun Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhouChina Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhouChina Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterlooOntarioCanada Department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada

The chief culprit impeding the commercialization of lithium–sulfur(Li–S)batteries is the parasitic shuttle effect and restricted redox kinetics of lithium polysulfides(LiPSs).To circumvent these key stumbling blocks,incorporating electrocatalysts with rational electronic structure modulation into sulfur cathode plays a decisive role in vitalizing the higher electrocatalytic activity to promote sulfur utilization efficiency.Breaking the stereotype of contemporary electrocatalyst design kept on pretreatment,field-assisted electrocatalysts offer strategic advantages in dynamically controllable electrochemical reactions that might be thorny to regulate in conventional electrochemical processes.However,the highly interdisciplinary fieldassisted electrochemistry puzzles researchers for a fundamental understanding of the ambiguous correlations among electronic structure,surface adsorption properties,and catalytic performance.In this review,the mechanisms,functionality explorations,and advantages of field-assisted electrocatalysts including electric,magnetic,light,thermal,and strain fields in Li–S batteries have been summarized.By demonstrating pioneering work for customized geometric configuration,energy band engineering,and optimal microenvironment arrangement in response to decreased activation energy and enriched reactant concentration for accelerated sulfur redox kinetics,cutting-edge insights into the holistic periscope of chargespin-orbital-lattice interplay between LiPSs and electrocatalysts are scrutinized,which aspires to advance the comprehensive understanding of the complex electrochemistry of Li–S batteries.Finally,future perspectives are provided to inspire innovations capable of defeating existing restrictions.

关键词： electrocatalysis electronic properties external fields Li-S batteries redox kinetics

2D spinel ZnCo_(2)O_(4) microsheet-coated functional separator for promoted redox kinetics and inhibited polysulfide dissolution

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Journal of Energy Chemistry 2021年第4期30卷 468-475页

作者： Jeong Seok Yeon Tae Ho Park Young Hun Ko Periyasamy Sivakumar Jun Su Kim Youngkywon Kim Ho Seok Park School of Chemical Engineering Sungkyunkwan UniversitySuwon 16419Gyeonggi-doRepublic of Korea Advanced Batteries Research Center Korea Electronics Technology InstituteSeongnam 13509Gyeonggi-doRepublic of Korea Department of Health Sciences and Technology Samsung Advanced Institute for Health Sciences and Technology(SAIHST)Sungkyunkwan UniversitySuwon 16419Gyeonggi-doRepublic of Korea Department of Chemistry Dongguk University-Seoul CampusJung-gu 04620 SeoulRepublic of Korea

Lithium-sulfur(Li-S)batteries are receiving increasing attention as one of the potential next-generation batteries,owing to their high energy densities and low cost.However,practical Li-S batteries with high energy densities are extremely hindered by the sulfur loss,low Coulombic efficiency,and short cycling life originating from the polysulfide(LiPS)shuttle.In this study,two-dimensional(2D)ZnCo_(2)O_(4) microsheets fabricated by a facile hydrothermal process are employed to modify the separator,for improving the electrochemical performances of Li-S cells.The resulting 2D Zn Co_(2)O_(4)-coated separator features a coating thickness of approximately 10 lm,high ionic conductivity of 1.8 m S/cm,and low mass loading of 0.2 mg/cm^(2).This 2D ZnCo_(2)O_(4)-coated separator effectively inhibits Li PS shuttle by a strong chemical interaction with Li PS as well as promotes the redox kinetics by Zn CO2O4-coated layers,as determined by X-ray photoelectron spectroscopy analysis,self-discharge,time-dependent permeation test,Li symmetric cell test,and Li2S nucleation analyses.Consequently,the Li-S batteries based on the 2D Zn Co_(2)O_(4)-coated separator exhibit a high initial discharge capacity of 1292.2 m Ah/g at 0.1 C.Moreover,they exhibit excellent long cycle stability at 1 and 2 C with capacity retention of 84%and 86%even after800 cycles,corresponding to a capacity fading rate of 0.020%and 0.016%per cycle,respectively.Effectively,these Li-S cells with a high sulfur loading at 5.3 mg/cm^(2) and low electrolyte concentration of 9 l L/mg deliver a high discharge capacity of 4.99 m Ah/cm^(2) after 200 cycles at 0.1 C.

关键词： Lithium sulfur batteries Functional separator 2D microsheet Polysulfide redox kinetics

The　redox　kinetics　of　the　Oxidation　for　CO　on　EuFeO_3　Catalyst

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Journal of Rare Earths 1995年第4期13卷 267-270页

作者：张瑞芹俞启全金韵 Peking Univ Beijing China

EuFeO_3 was prepared by the complexation method of citric acid. The Perovskite phase of EuFeO_3 was determined by XRD. The redox mechanism for oxidation of CO on EuFeO_3 was proven by the pulse method of reduction with CO and reoxidation with O_2. The redox kinetics of oxidation for CO on EuFeO_3 has been investigated with the external circulation flow reactor. The experimental data obeyed the redox equation. The parameters of the kinetic equation were estimated by the method of orthogonal design.

关键词： EuFeO_3 Oxidation for CO redox kinetics

Modulating eg orbitals through ligand engineering to boost the electrocatalytic activity of NiSe for advanced lithium-sulfur batteries

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Journal of Energy Chemistry 2022年第11期31卷 317-323,I0009页

作者： Tianran Yan Jie Feng Pan Zeng Gang Zhao Lei Wang Cheng Yuan Chen Cheng Youyong Li Liang Zhang Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123JiangsuChina Jiangsu Key Laboratory for Carbon-Based Functional Materials&Devices Soochow UniversitySuzhou 215123JiangsuChina Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123JiangsuChina

Accelerating the sluggish redox kinetics of lithium polysulfides(LiPSs)by electrocatalysis is essential to achieve high performance lithium-sulfur(Li-S)batteries.However,the issue of insufficient catalytic activity remains to be addressed.Herein,a strategy of modulating e_(g) orbitals through ligand engineering has been proposed to boost the catalytic activity of NiSe for rapid LiPSs redox conversion.The X-ray spectroscopic measurements and theoretical calculations reveal that partial substitution of Se with N disrupts the octahedral coordination of Ni atoms in NiSe,leading to the reduced degeneracy and upward shift of e_(g) orbitals of Ni 3 d states.As a consequence,the bonding strength of N-substituted NiSe(N-NiSe)with LiPSs is enhanced,which facilitates the interfacial charge transfer kinetics and accelerates the LiPSs redox kinetics.Therefore,the Li-S batteries assembled with N-NiSe present a high capacity of 682.6 mAh g^(-1) at a high rate of 5 C and a high areal capacity of 6.5 mAh cm^(-2)at a high sulfur loading of 6 mg cm^(-2).This work provides a promising strategy to develop efficient transition-metal based electrocatalysts for Li-S batteries through e_(g) orbital modulation.

关键词： Li-S batteries eg orbitals modulation Ligand engineering Shuttle effect redox kinetics

Cellulose nanofiber-derived carbon aerogel for advanced room-temperature sodium–sulfur batteries

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Carbon Energy 2023年第1期5卷 1-15页

作者： Wu Yang Wang Yang Ren Zou Yongfa Huang Haihong Lai Zehong Chen Xinwen Peng State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhouChina

Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodium and sulfur.However,the diffusion of polysulfides and sluggish kinetics of conversion reactions are still major challenges for their application.Herein,we developed a powerful and functional separator to inhibit the shuttle effect by coating a lightweight three-dimensional cellulose nanofiber-derived carbon aerogel on a glass fiber separator(denoted NSCA@GF).The hierarchical porous structures,favorable electronic conductivity,and three-dimensional interconnected network of N,S-codoped carbon aerogel endow a multifunctional separator with strong polysulfide anchoring capability and fast reaction kinetics of polysulfide conversion,which can act as the barrier layer and an expanded current collector to increase sulfur utilization.Moreover,the hetero-doped N/S sites are believed to strengthen polysulfide anchoring capability via chemisorption and accelerate the redox kinetics of polysulfide conversion,which is confirmed from experimental and theoretical results.As a result,the assembled Na–S coin cells with the NSCA@GF separator showed a high reversible capacity(788.8 mAh g^(−1) at 0.1 C after 100 cycles)and superior cycling stability(only 0.059%capacity decay per cycle over 1000 cycles at 1 C),thereby demonstrating the significant potential for application in high-performance RT/Na–S batteries.

关键词： carbon aerogel cellulose nanofiber N,S codoping redox kinetics sodium–sulfur batteries

Bidirectionally catalytic polysulfide conversion by high-conductive metal carbides for lithium-sulfur batteries

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Journal of Energy Chemistry 2022年第4期31卷 73-81页

作者： Genlin Liu Cheng Yuan Pan Zeng Chen Cheng Tianran Yan Kehua Dai Jing Mao Liang Zhang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123JiangsuChina College of Chemistry Tianjin Normal UniversityTianjin 300387China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina

Utilizing catalysts to accelerate the redox kinetics of lithium polysulfides (LiPSs) is a promising strategy to alleviate the shuttle effect of lithium–sulfur (Li–S) batteries.Nevertheless,most of the reported catalysts are only effective for LiPSs reduction,resulting in the devitalization of catalysts over extended cycles as a consequence of the continuous accumulation of Li_(2)S passivation layer.The situation gets even worse when employing mono-directional catalyst with poor electron conductivity because the charge transfer for the decomposition of solid Li_(2)S is severely hampered.Herein,a high-conductive and dualdirectional catalyst Co_(3)C decorated on porous nitrogen-doped graphene-like structure and carbon nanotube (Co_(3)C@PNGr-CNT) is fabricated as sulfur host,which not only promotes the precipitation of Li_(2)S from Li PSs during discharge but also facilitates the decomposition of Li;S during subsequent charge,as evidenced by the reduced activation energies for both reduction and oxidation processes.Furthermore,the long-term catalytic stability of Co_(3)C is corroborated by the reversible evolution of Co–C bond length over extended cycles as observed from X-ray absorption fine structure results.As a consequence,the fabricated Co_(3)C@PNGr-CNT/S cathode delivers a low capacity decay of 0.043%per cycle over 1000 cycles at 2C.Even at high sulfur loading (15.6 mg cm^(-2)) and low electrolyte/sulfur (E/S) ratio (~8μL mg^(-1))conditions,the battery still delivers an outstanding areal capacity of 11.05 m Ah cm^(-2) after 40 cycles.This work provides a rational strategy for designing high-efficient bidirectional catalyst with single component for high-performance Li-S batteries.

关键词： Li-S batteries redox kinetics Cobalt carbide Bidirectional catalyst Shuttle effect

Quantitative defect regulation of heterostructures for sulfur catalysis toward fast and long lifespan lithium-sulfur batteries

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Nano Research 2022年第9期15卷 7925-7932页

作者： Saisai Qiu Xinqi Liang Shuwen Niu Qingguo Chen Gongming Wang Minghua Chen Key Laboratory of Engineering Dielectric and Applications(Ministry of Education) School of Electrical and Electronic EngineeringHarbin University of Science and TechnologyHarbin 150080China Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science&Technology of ChinaHefei 230026China

The advancement of lithium-sulfur(Li-S)batteries is severely retarded by lithium polysulfides(LiPSs)shuttling behavior and sluggish redox kinetics.Herein,the heterogeneous composite with defective Bi_(2)Se_(3−x)nanosheets and porous nitrogen-doped carbon(Bi_(2)Se_(3−x)/NC)is prepared by selenizing bismuth metal-organic frameworks as a multifunctional sulfur host.The highly efficient immobilization-conversion on LiPSs is realized by the synergistic effect of structure construction strategy and defect engineering.It is found that Bi_(2)Se_(3−x)with the suitable amount of selenium vacancies achieves the best electrochemical performance due to the advantages of its structure and composition.These results confirm the intrinsic correlation between defects and catalysis,which are revealed by computational and experimental studies.Due to these superiorities,the developed sulfur electrodes exhibited admirable stability and a fairly lower capacity decay rate of approximately 0.0278%per cycle over 1,000 cycles at a 3 C rate.Even at the high sulfur loading of 6.2 mg·cm^(−2),the cathode still demonstrates a high discharge capacity of 455 mAh·g^(−1)at 1 C.This work may enlighten the development of mechanism investigation and design principles regarding sulfur catalysis toward high-performance Li-S batteries.

关键词： lithium-sulfur(Li-S)batteries lithium polysulfides(LiPSs) shuttle effect redox kinetics selenium vacancy sulfur catalysis

Enhancing anchoring and catalytic conversion of polysulfides by nitrogen deficient cobalt nitride for advanced lithium-sulfur batteries

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Journal of Energy Chemistry 2022年第10期31卷 407-415,I0010页

作者： Min Luo Yu Bai Rui Sun Meixiu Qu Mengyuan Wang Zhanfeng Yang Zhenhua Wang Wang Sun Kening Sun Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory for Chemical Power Source and Green Catalysis School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

While lithium-sulfur(Li-S)battery has attracted remarkable attention owing to the high theoretical capacity,its practical application is still hindered by the shuttle and sluggish conversion kinetics of intermediate lithium polysulfides(Li PSs).Defect engineering,which can regulate the electronic structure and in turn influence the surface adsorption and catalytic capability,has been regarded as a feasible strategy to deal with the above challenges.However,few studies on nitrogen vacancies and their mechanisms are reported.Herein,cobalt nitride with nitrogen vacancies grown on multi-walled carbon nanotube(CNTCo N-VN)is designed and applied as the separator modification material to investigate the enhancing mechanism of nitrogen vacancies on Li-S batteries.The experimental evidence and theoretical calculation indicate that the introduction of nitrogen vacancies into cobalt nitride can enhance the chemical affinity to Li PSs and effectively hamper the shuttle effect.Meanwhile the reduced band gap of the d-band center of Co and p-band center of N for CNT-Co N-VNand the promoted diffusion of Li^(+) can expedite the solid-liquid and liquid-liquid conversions of sulfur species.Due to these superiorities,the cell with CNT-Co NVNmodified separator delivers a favorable initial capacity of 901 m Ah g^(-1)and a capacity of 660 m Ah g^(-1)can be achieved after 250 cycles at 2 C.This work explores the application of metal nitride with nitrogen vacancies and sheds light on the development of functional separators for high-efficient Li-S batteries.

关键词： Cobalt nitride Nitrogen vacancy redox kinetics Separators Li-S batteries