Article
Chemistry, Multidisciplinary
Yinger Xiang, Xinyu Hu, Xue Zhong, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji
Summary: This study proposes a strategy of hierarchical double carbon/Sb composite to enhance the performance of Sb anode. The composite employs carbon spheres to encapsulate Sb nanoparticles with strong interfacial chemical bonds, and utilizes graphene as a conductive network to connect the composite materials. The hierarchical double carbon/Sb composite shows excellent rate and long cycling performance, and provides theoretical guidance for the development of metal anodes.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Laidong Zhou, J. David Bazak, Baltej Singh, Chang Li, Abdeljalil Assoud, Nancy M. Washton, Vijayakumar Murugesan, Linda F. Nazar
Summary: We have discovered a new fast-ion conductor, Na3B5S9, that exhibits a high Na ion total conductivity of 0.80 mS cm(-1) (sintered pellet; cold-pressed pellet=0.21 mS cm(-1)). This material has a unique structure consisting of corner-sharing B10S20 supertetrahedral clusters that create a framework supporting 3D Na ion diffusion channels. The study reveals the importance of a disordered Na ion sublattice and well-connected Na ion migration pathways in dictating Na ion diffusion.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Mark E. Wolf, Elizabeth A. Doty, Justin M. Turney, Henry F. Schaefer
Summary: This study examines tetrahedrane molecules with phosphorus substitution through experimental and theoretical approaches, revealing little change in the geometric parameters of the (CH)(3) moiety under pnictogen substitution, but significant alterations in Pn-C bonds and C-Pn-C bond angles. Delocalization of electrons into substituent antibonding orbitals is found to enhance the energetic favorability of the tetrahedrane structure, weakening Pn-C bonds, particularly with heavier pnictogens.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Review
Chemistry, Multidisciplinary
Rahul Deb, P. Balakrishna, Moumita Majumdar
Summary: The Group 15 Pn(I) cations, isoelectronic with donor-stabilized carbones, exhibit weak nucleophilicity despite having two lone pairs of electrons due to their inherent positive charge. Enhancing their Lewis basicity with strongly electron-donating ligands and chelating cyclic ligand systems has proven effective in increasing their nucleophilicity. Recent achievements in isolating fleeting Sb(I) and Bi(I) cations have been discussed, along with a discussion on the syntheses, structure, bonding situations, and reactivity of the Pn(I) cations, providing an outlook on their periodic trends and future applications.
CHEMISTRY-AN ASIAN JOURNAL
(2021)
Article
Engineering, Environmental
Dong-Keun Yu, Cheol-Min Park
Summary: Various approaches have been introduced to obtain Sb-based composites for high-performance NIB anodes, including amorphous C-containing Sb composites, Sb-based intermetallic compounds, and Na-inactive metal carbide and amorphous C-containing Sb composites. These composites showed highly reversible, stable capacity and fast rate capability, making them potential new anode materials for high-performance NIBs.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Xiaoming Zhang, Luojiang Zhang, Wenyong Zhang, Song Xue, Yongbing Tang
Summary: A novel SDIB using Cu3P particles confined in conductive P-doped carbon layers as the anode is developed, showing outstanding performance in terms of ion diffusion kinetics, volume variation effects, rate performance, and cycling stability, making it one of the best reported SDIBs.
JOURNAL OF POWER SOURCES
(2022)
Article
Electrochemistry
Afifa Sadaqat, Ghulam Ali, Mahmood ul Hasan, Faiza Jan Iftikhar, Sidra Khalid, Uzma Khalique, Shumaila Karamat
Summary: In this study, a FeS2/carbon hybrid composite was prepared for sodium-ion batteries (SIBs) as a negative electrode. The FeS2/C composite exhibited excellent structural reliability, sodium storage capacity, and rate performance. The synergistic interaction among FeS2 particles sited on the conductive sheets of mesoporous carbon matrix contributed to the improved adsorption of sodium ions, good rate capacity, and cycling stability.
ELECTROCHIMICA ACTA
(2023)
Article
Chemistry, Multidisciplinary
Chang Liu, Xin Fu, Shuzhen Liao, Guoqiang Zou, Hai Yang
Summary: Heterointerface engineering is an effective approach to enhance the energy density of alkali-ion batteries, but constructing heterogeneous composites with abundant interfaces remains a significant challenge for sodium-ion batteries (SIBs).
Article
Chemistry, Physical
Roman Zettl, Sarah Lunghammer, Bernhard Gadermaier, Athmane Boulaoued, Patrik Johansson, H. Martin R. Wilkening, Ilie Hanzu
Summary: This study reports a new hybrid Li+ and Na+ conducting SSE based on the MIL-121 MOF structure, with ion exchange functionalizing the free carboxylic units along the 1D pores. The ion dynamics were investigated using impedance spectroscopy and NMR spin-lattice relaxation, revealing a transition from correlated to uncorrelated motion at higher temperature. The findings suggest potential development of high-performance MOF-based hybrid SSEs for ASSBs.
ADVANCED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Arturo Espinosa Ferao, Alicia Rey Planells
Summary: Accurate ring strain energy (RSE) values were reported for sixty-six parent pnictogeniranes with two other identical p-block elements, El(2)Pn. A decrease in RSE was found to be correlated with an increase in the p character of the AO used in endocyclic bonds, particularly in groups 15 and 16. The higher -NICS(1) values also parallel the presence of atom-centred diatropic currents, mostly arising from the lone pairs. Only in the case of pnictogenaditrieliranes Tr(2)Pn (Tr=B, Al, Ga), the decrease of -NICS(1) is related to lower Huckel-type 2 pi-electron aromaticity in group 13.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Ding-Ren Shi, Zulipiya Shadike, Tian Wang, Si-Yu Yang, He-Yi Xia, Yu-Ke Wang, Ji-Li Yue, Enyuan Hu, Seong-Min Bak, Xin-Yang Yue, Yong-Ning Zhou, Lu Ma, Sanjit Ghose, Tianpin Wu, Qing-Hua Zhang, Zhe Xing, Yan-Ning Zhang, Lei Zheng, Lin Gu, Xiao-Qing Yang, Zheng-Wen Fu
Summary: This paper introduces a new layered chalcogenide, NaCrSSe, based on dual anionic-redox reaction, which exhibits high capacity and fast kinetics. The material shows low polarization and high energy efficiencies of around 92%, with a superior high-rate charge capacity even at 4000 mA g(-1).
JOURNAL OF POWER SOURCES
(2021)
Article
Chemistry, Multidisciplinary
Philipp Deng, Alfred Rabenbauer, Kathrin Vosseler, Janio Venturini, Tom Nilges
Summary: Pnp-switchable semiconductor materials can change their electronic properties through a temperature-dependent phase transition, enabling the construction of unconventional one-compound diodes. This study utilizes pnp-switchable AgCuS to create a functional one-compound diode, which demonstrates reversibility and flexibility for diode operation. The material's electrical, thermal, and diode properties are fully characterized, and its performance is discussed in relation to Ag18Cu3Te11Cl3, the first one-compound diode operating near room temperature.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Kavish Kaup, Abdeljalil Assoud, Jue Liu, Linda F. Nazar
Summary: Lithium thioborate halides are a new class of fast lithium-ion conducting materials with a superadamantanoid structure, exhibiting high ionic conductivities up to 1.4 mS cm(-1) that can be effectively tuned by the polarizability of the halide anion within the channels.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Mayanak K. Gupta, Jingxuan Ding, Naresh C. Osti, Douglas L. Abernathy, William Arnold, Hui Wang, Zachary Hood, Olivier Delaire
Summary: By investigating the phonons in Na3PS4 and their coupling to fast sodium diffusion, key anharmonic phonon modes controlling the diffusion process were identified at the Brillouin zone boundary of the anharmonically stabilized cubic phase. Detailed insights into the dynamic mechanism of fast sodium diffusion were provided, offering a pathway to search for further sodium solid electrolytes.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Physical
W. Peter Kalisvaart, Madhusudan Chaudhary, Amit Bhattacharya, Vladimir K. Michaelis, Jillian M. Buriak
Summary: Antimony and bismuth are attractive candidates for replacing graphite in Li-ion battery anodes as they can alloy with lithium. The Li-Sb-Bi ternary system has been studied and ternary alloys with different Sb mole fractions were synthesized. These alloys exhibit cubic crystal structures but show a tendency towards phase segregation at certain mole fractions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Chang Li, Ryan Kingsbury, Laidong Zhou, Abhinandan Shyamsunder, Kristin A. Persson, Linda F. Nazar
Summary: In this study, the harmful H+ intercalation in aqueous zinc batteries is successfully suppressed by tuning the solvation structure, leading to reversible cycling of the battery.
ACS ENERGY LETTERS
(2022)
Article
Energy & Fuels
Laidong Zhou, Tong-Tong Zuo, Chun Yuen Kwok, Se Young Kim, Abdeljalil Assoud, Qiang Zhang, Juergen Janek, Linda F. Nazar
Summary: A series of new lithium mixed-metal chlorospinels are reported as solid electrolytes for all-solid-state lithium batteries, which exhibit high ionic conductivity and low electronic conductivity, showing potential for high-performance all-solid-state lithium batteries.
Review
Nanoscience & Nanotechnology
Zhizhen Zhang, Linda F. Nazar
Summary: This article discusses the fundamental principles of designing superionic conductors and how to enhance cation diffusion through the role of framework anion rotational dynamics. By studying the interaction between cations and anions, it is hoped to achieve super-high conductivity in solid electrolytes.
NATURE REVIEWS MATERIALS
(2022)
Article
Chemistry, Physical
Laidong Zhou, Qiang Zhang, Linda F. Nazar
Summary: We report on a new family of halide-deficient and Li-rich argyrodite fast-ion conductors, which demonstrate high ionic conductivities due to the disordered Li ion sublattice and sulfur/halogen anion site disorder. The influence of aliovalent anion substitution in Li6PS5X (X = Cl, Br, I) on Li-ion concentration and disorder is explored. The findings highlight the importance of attaining a disordered Li ion sublattice and sulfur/halogen anion site disorder for enhancing the ionic conductivity in argyrodites.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Tong-Tong Zuo, Felix Walther, Jun Hao Teo, Raffael Ruess, Yubo Wang, Marcus Rohnke, Daniel Schroeder, Linda F. Nazar, Juergen Janek
Summary: Lithium argyrodite-type electrolytes are promising due to their high ionic conductivity and processability. The influence of halogenation on electrochemical decomposition and chemical degradation mechanism at the cathode interface is investigated. The results show that halogenation leads to increased electrochemical decomposition, more gaseous degradation products, and a decreased interfacial resistance, resulting in higher cell performance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Chun Yuen Kwok, Shiqi Xu, Ivan Kochetkov, Laidong Zhou, Linda F. F. Nazar
Summary: A Li2S/LiVS2 core-shell cathode architecture design is reported for all-solid-state Li-S batteries, which improves the kinetics of Li2S cathode by using the shell as a charge-carrier transport vehicle and electron transfer mediator. The solid-state Li2S cell exhibits good rate capability and capacity retention at room temperature, and high active material loading is demonstrated with stable capacity retention. However, the cycle life is limited under high active material loading.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Erika P. P. Ramos, Abdeljalil Assoud, Laidong Zhou, Abhinandan Shyamsunder, Daniel Rettenwander, Linda F. F. Nazar
Summary: We have reported a new ion conductor, Na11Sn2SbSe12, which could be a possible candidate for a solid catholyte in composite cathodes for all-solid state Na-batteries. It possesses a room temperature ionic conductivity of 0.15 ± 0.03 mS cm(-1) and an activation energy of 0.39 ± 0.02 eV. Through a combination of Rietveld refinement and electrochemical impedance spectroscopy, we have investigated the sulfide solid solutions, Na11Sn2SbS12-xSex (x = 1 and 6), to understand the structure-property relationships governing ion transport in these materials.
Article
Chemistry, Multidisciplinary
Laidong Zhou, J. David Bazak, Baltej Singh, Chang Li, Abdeljalil Assoud, Nancy M. Washton, Vijayakumar Murugesan, Linda F. Nazar
Summary: We have discovered a new fast-ion conductor, Na3B5S9, that exhibits a high Na ion total conductivity of 0.80 mS cm(-1) (sintered pellet; cold-pressed pellet=0.21 mS cm(-1)). This material has a unique structure consisting of corner-sharing B10S20 supertetrahedral clusters that create a framework supporting 3D Na ion diffusion channels. The study reveals the importance of a disordered Na ion sublattice and well-connected Na ion migration pathways in dictating Na ion diffusion.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Chang Li, Ryan Kingsbury, Arashdeep Singh Thind, Abhinandan Shyamsunder, Timothy T. Fister, Robert F. Klie, Kristin A. Persson, Linda F. Nazar
Summary: The authors report a eutectic electrolyte that enables selective Zn2+ intercalation at the cathode and highly reversible Zn metal plating/stripping at the anode, resulting in a high-capacity Zn anode-free cell. By suppressing proton co-intercalation and dendrite growth, the authors achieve a benchmark performance in aqueous Zn-metal batteries, with high coulombic efficiency and long cycle life.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Laidong Zhou, Tongtong Zuo, Chang Li, Qiang Zhang, Jurgen Janek, Linda F. F. Nazar
Summary: We report two new families of lithium metal chloride solid electrolytes, Li(3-x)Zr(x)(M)(1-x)Cl-6 (0≤x≤0.8; M = Ho or Lu), with high ionic conductivities of up to 1.8 mS cm(-1) and a low activation energy of 0.34 eV. Structural elucidation reveals the Li ion distribution in three different compounds. All-solid-state batteries with Li2.6Zr0.4(Ho/Lu)0.6Cl-6 solid electrolytes and NCM85 cathodes show stable cycling up to 4.6 V, with stable cathode interphases formed.
ACS ENERGY LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Abhinandan Shyamsunder, Max Palmer, Ivan R. Kochetkov, Jeff S. Sakamoto, Linda F. Nazar
Summary: Conventional Li-S batteries rely on liquid electrolytes, while new electron pair donor (EPD) solvents provide higher sulfur solubility and better sulfur utilization. However, their instability requires the use of an ion-conductive membrane. This study found that even trace amounts of LiOH on the LLTZO surface react with sulfur in EPD solvents, leading to the formation of a resistive layer that impedes Li+ transport. However, modifying the LLZO surface with protective phosphate groups reduces charge-transfer resistance and inhibits the reaction between LiOH and sulfur. The electrolyte cells constructed based on this concept exhibit high sulfur utilization and good stability.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Yangyang Huang, Laidong Zhou, Chang Li, Zhuo Yu, Linda F. Nazar
Summary: A simple organic coating concept utilizing a nanometric layer of waxy soap has been reported to stabilize argyrodite material and suppress its oxidative degradation at high voltage, achieving good cycling stability and capacity retention.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Chang Li, Rishabh D. Guha, Abhinandan Shyamsunder, Kristin A. Persson, Linda F. Nazar
Summary: We report a solvent-designed Mg(TFSI)2 electrolyte that facilitates ion pair dissociation, nanoscale Mg nucleation/growth, and dendrite-free Mg plating/stripping at 2 mA h cm-2, enabling full cell operation up to 3.5 V at a 2C rate for 400 cycles.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Ivan Kochetkov, Tong-Tong Zuo, Raffael Ruess, Baltej Singh, Laidong Zhou, Kavish Kaup, Juergen Janek, Linda Nazar
Summary: A deep understanding of the interaction between the surface of cathode materials and solid electrolytes is crucial for designing advanced solid-state batteries. This study explores the impact of cationic metal substitution on the interfacial chemistry in Li-M-Cl solid electrolytes and establishes a platform for evaluating the stability of new halide solid electrolytes in SSB cells.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
