Dynamic Intercalation-Conversion Site Supported Ultrathin 2D Mesoporous SnO2/SnSe2 Hybrid as Bifunctional Polysulfide Immobilizer and Lithium Regulator for Lithium-Sulfur Chemistry.

The practical application of lithium-sulfur batteries is impeded by the polysulfide shuttling and interfacial instability of the metallic lithium anode. In this work, a twinborn ultrathin two-dimensional graphene-based mesoporous SnO2/SnSe2 hybrid (denoted as G-mSnO2/SnSe2) is constructed as a polysulfide immobilizer and lithium regulator for Li-S chemistry. The as-designed G-mSnO2/SnSe2 hybrid possesses high conductivity, strong chemical affinity (SnO2), and a dynamic intercalation-conversion site (LixSnSe2), inhibits shuttle behavior, provides rapid Li-intercalative transport kinetics, accelerates LiPS conversion, and decreases the decomposition energy barrier for Li2S, which is evidenced by the ex situ XAS spectra, in situ Raman, in situ XRD, and DFT calculations. Moreover, the mesoporous G-mSnO2/SnSe2 with lithiophilic characteristics enables homogeneous Li-ion deposition and inhibits Li dendrite growth. Therefore, Li-S batteries with a G-mSnO2/SnSe2 separator achieve a favorable electrochemical performance, including high sulfur utilization (1544 mAh g-1 at 0.2 C), high-rate capability (794 mAh g-1 at 8 C), and long cycle life (extremely low attenuation rate of 0.0144% each cycle at 5 C over 2000 cycles). Encouragingly, a 1.6 g S/Ah-level pouch cell realizes a high energy density of up to 359 Wh kg-1 under a lean E/S usage of 3.0 μL mg-1. This work sheds light on the design roadmap for tackling S-cathode and Li-anode challenges simultaneously toward long-durability Li-S chemistry.

[1]  Yongchun Zou,et al.  Crystalline Molybdenum Carbide−Amorphous Molybdenum Oxide Heterostructures: In Situ Surface Reconfiguration and Electronic States Modulation for Li−S Batteries , 2022, Energy Storage Materials.

[2]  I. Manke,et al.  P‐Doped NiTe2 with Te‐Vacancies in Lithium–Sulfur Batteries Prevents Shuttling and Promotes Polysulfide Conversion , 2022, Advanced materials.

[3]  Xing Ma,et al.  Ionic‐Liquid‐Assisted Synthesis of N, F, and B Co‐Doped CoFe2O4−x on Multiwalled Carbon Nanotubes with Enriched Oxygen Vacancies for Li–S Batteries , 2021, Advanced Functional Materials.

[4]  Li Li,et al.  Engineering Catalytic CoSe–ZnSe Heterojunctions Anchored on Graphene Aerogels for Bidirectional Sulfur Conversion Reactions , 2021, Advanced science.

[5]  Tianran Yan,et al.  Utilizing the Built‐in Electric Field of p–n Junctions to Spatially Propel the Stepwise Polysulfide Conversion in Lithium–Sulfur Batteries , 2021, Advanced materials.

[6]  Nan Wang,et al.  Towards High Performance Li–S Batteries via Sulfonate‐Rich COF‐Modified Separator , 2021, Advanced materials.

[7]  Yan Yu,et al.  Achieving stable Na metal cycling via polydopamine/multilayer graphene coating of a polypropylene separator , 2021, Nature Communications.

[8]  I. Manke,et al.  A Highly Conductive COF@CNT Electrocatalyst Boosting Polysulfide Conversion for Li–S Chemistry , 2021, ACS Energy Letters.

[9]  B. Han,et al.  Highly efficient CO2 electroreduction to methanol via atomically dispersed Sn coupled with defective CuO catalysts. , 2021, Angewandte Chemie.

[10]  Xingwen Yu,et al.  Thickness-independent scalable high-performance Li-S batteries with high areal sulfur loading via electron-enriched carbon framework , 2021, Nature Communications.

[11]  Yongzhu Fu,et al.  Isomeric Organodithiol Additives for Improving Interfacial Chemistry in Rechargeable Li-S Batteries. , 2021, Journal of the American Chemical Society.

[12]  Renjie Chen,et al.  Self‐Assembly of 0D–2D Heterostructure Electrocatalyst from MOF and MXene for Boosted Lithium Polysulfide Conversion Reaction , 2021, Advanced materials.

[13]  Bing Sun,et al.  Atomic-scale regulation of anionic and cationic migration in alkali metal batteries , 2021, Nature Communications.

[14]  Yuen Wu,et al.  Amorphization-induced surface electronic states modulation of cobaltous oxide nanosheets for lithium-sulfur batteries , 2021, Nature Communications.

[15]  Chaoqi Zhang,et al.  Tubular CoFeP@CN as a Mott–Schottky Catalyst with Multiple Adsorption Sites for Robust Lithium−Sulfur Batteries , 2021, Advanced Energy Materials.

[16]  A. Yu,et al.  “Sauna” Activation toward Intrinsic Lattice Deficiency in Carbon Nanotube Microspheres for High‐Energy and Long‐Lasting Lithium–Sulfur Batteries , 2021, Advanced Energy Materials.

[17]  Xiujian Chou,et al.  Interfacial Engineering of Bifunctional Niobium (V)‐Based Heterostructure Nanosheet Toward High Efficiency Lean‐Electrolyte Lithium–Sulfur Full Batteries , 2021, Advanced Functional Materials.

[18]  Zhonglin Li,et al.  The Electrostatic Attraction and Catalytic Effect Enabled by Ionic–Covalent Organic Nanosheets on MXene for Separator Modification of Lithium–Sulfur Batteries , 2021, Advanced materials.

[19]  Guofu Zhou,et al.  Deciphering interpenetrated interface of transition metal oxides/phosphates from atomic level for reliable Li/S electrocatalytic behavior , 2021 .

[20]  Guofu Zhou,et al.  Strain Engineering of a MXene/CNT Hierarchical Porous Hollow Microsphere Electrocatalyst for a High-Efficiency Lithium Polysulfide Conversion Process. , 2021, Angewandte Chemie.

[21]  K. Amine,et al.  A high-energy and long-cycling lithium–sulfur pouch cell via a macroporous catalytic cathode with double-end binding sites , 2020, Nature Nanotechnology.

[22]  Jingyu Sun,et al.  3D Printing of a V8C7–VO2 Bifunctional Scaffold as an Effective Polysulfide Immobilizer and Lithium Stabilizer for Li–S Batteries , 2020, Advanced materials.

[23]  Qianqian Wang,et al.  Rational Design of Multifunctional Integrated Host Configuration with Lithiophilicity‐Sulfiphilicity toward High‐Performance Li–S Full Batteries , 2020, Advanced Functional Materials.

[24]  A. Manthiram,et al.  3D CoSe@C Aerogel as a Host for Dendrite‐Free Lithium‐Metal Anode and Efficient Sulfur Cathode in Li–S Full Cells , 2020, Advanced Energy Materials.

[25]  Guangmin Zhou,et al.  Bidirectional Catalysts for Liquid–Solid Redox Conversion in Lithium–Sulfur Batteries , 2020, Advanced materials.

[26]  Yanglong Hou,et al.  Enhanced Polysulfide Regulation via Porous Catalytic V2O3/V8C7 Heterostructures Derived from Metal-Organic Frameworks towards High-Performance Li-S Batteries. , 2020, ACS nano.

[27]  Lifang Jiao,et al.  Heterostructure SnSe2/ZnSe@PDA Nanobox for Stable and Highly Efficient Sodium‐Ion Storage , 2020, Advanced Energy Materials.

[28]  Qinghua Zhang,et al.  Lattice Distortion in Hollow Multi-shelled Structures for Efficient Visible Light CO2 Reduction with SnS2/SnO2 Junction. , 2020, Angewandte Chemie.

[29]  Xiaojun Wu,et al.  A Dual‐Functional Conductive Framework Embedded with TiN‐VN Heterostructures for Highly Efficient Polysulfide and Lithium Regulation toward Stable Li–S Full Batteries , 2019, Advanced materials.

[30]  Jingde Li,et al.  Low‐Bandgap Se‐Deficient Antimony Selenide as a Multifunctional Polysulfide Barrier toward High‐Performance Lithium–Sulfur Batteries , 2019, Advanced materials.

[31]  Shenglin Xiong,et al.  Sulfiphilic Few‐Layered MoSe2 Nanoflakes Decorated rGO as a Highly Efficient Sulfur Host for Lithium‐Sulfur Batteries , 2019, Advanced Energy Materials.

[32]  R. Knibbe,et al.  Sandwich‐Like Ultrathin TiS2 Nanosheets Confined within N, S Codoped Porous Carbon as an Effective Polysulfide Promoter in Lithium‐Sulfur Batteries , 2019, Advanced Energy Materials.

[33]  Liumin Suo,et al.  Intercalation-conversion hybrid cathodes enabling Li–S full-cell architectures with jointly superior gravimetric and volumetric energy densities , 2019, Nature Energy.

[34]  Yanli Wang,et al.  Two-dimensional porous carbon-coated sandwich-like mesoporous SnO2/graphene/mesoporous SnO2 nanosheets towards high-rate and long cycle life lithium-ion batteries , 2019, Chemical Engineering Journal.

[35]  L. Wan,et al.  Cobalt in Nitrogen-Doped Graphene as Single-Atom Catalyst for High-Sulfur Content Lithium-Sulfur Batteries. , 2019, Journal of the American Chemical Society.

[36]  Haihui Wang,et al.  2D MoN-VN Heterostructure To Regulate Polysulfides for Highly Efficient Lithium-Sulfur Batteries. , 2018, Angewandte Chemie.

[37]  C. Wolverton,et al.  Atomic‐Scale Observation of Electrochemically Reversible Phase Transformations in SnSe2 Single Crystals , 2018, Advanced materials.

[38]  J. Goodenough,et al.  Inhibiting Polysulfide Shuttling with a Graphene Composite Separator for Highly Robust Lithium-Sulfur Batteries , 2018, Joule.

[39]  Z. Huang,et al.  SnSe2 Quantum Dot/rGO composite as high performing lithium anode , 2018 .

[40]  Jiaqi Huang,et al.  Sulfur Nanodots Stitched in 2D "Bubble-Like" Interconnected Carbon Fabric as Reversibility-Enhanced Cathodes for Lithium-Sulfur Batteries. , 2017, ACS nano.

[41]  Cheol‐Min Park,et al.  Tin Selenides with Layered Crystal Structures for Li-Ion Batteries: Interesting Phase Change Mechanisms and Outstanding Electrochemical Behaviors. , 2017, ACS applied materials & interfaces.

[42]  Feng Li,et al.  Conductive porous vanadium nitride/graphene composite as chemical anchor of polysulfides for lithium-sulfur batteries , 2017, Nature Communications.

[43]  Yitai Qian,et al.  SnS2- Compared to SnO2-Stabilized S/C Composites toward High-Performance Lithium Sulfur Batteries. , 2016, ACS applied materials & interfaces.

[44]  Zhe Yuan,et al.  Powering Lithium-Sulfur Battery Performance by Propelling Polysulfide Redox at Sulfiphilic Hosts. , 2016, Nano letters.

[45]  Liang Zhan,et al.  Graphene‐Based Porous Silica Sheets Impregnated with Polyethyleneimine for Superior CO2 Capture , 2013, Advanced materials.