Article
Chemistry, Multidisciplinary
Kiho Nishioka, Mizuki Tanaka, Hayato Fujimoto, Toru Amaya, Sensuke Ogoshi, Mamoru Tobisu, Shuji Nakanishi
Summary: In addition to sufficient tolerance against superoxide radical attack, other factors also play a crucial role in the cyclability of Li-O2 batteries. The use of N,N-dimethylacetamide-based electrolyte can enhance the cyclability by quenching O-1(2) and forming highly decomposable Li2O2.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Mengyuan Song, Changhao Tian, Chunguang Chen, Tao Huang, Aishui Yu
Summary: Lithium-oxygen batteries have high energy density, but conventional liquid electrolytes struggle to form a stable solid electrolyte interface (SEI) on the cathode surface for long-term stable cycling. LiBOB is added to the LiTFSI-based electrolyte to solve this issue. The introduction of LiBOB induces the dissociation equilibrium of the lithium salt positively, resulting in an electrolyte with good ionic conductivity. Different amounts of LiBOB exhibit different characteristics in electrochemical performance, with trace amounts improving discharge capacity. The synergistic effect of the LiTFSI-LiBOB dual-salt electrolyte forms a protective SEI, leading to comparable cycling performance.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Wonsung Choi, Kyoung H. Choi, Tae Y. Kim, Toshinori Sugimoto, Youngeal Kim, Shintaro Kitajima, Mokwon Kim, Hyunjin Kim, Hyunpyo Lee, Hyuk Jae Kwon, Heung C. Lee, Dongjoon Lee, Jung O. Park, Jung-Hwa Kim, Seong Y. Park, Dongmin Im
Summary: This paper reports the scalable production of a thin membrane comprising single-crystal SE particles that are bicontinuously embedded in a polymer matrix to form ion-conducting channels. The membrane exhibits high ionic conductivity and enables stable lithium metal stripping and plating, resulting in a high specific energy.
JOURNAL OF POWER SOURCES
(2021)
Article
Nanoscience & Nanotechnology
Linfeng Peng, Shaoqing Chen, Chuang Yu, Chaochao Wei, Cong Liao, Zhongkai Wu, Hsing-Lin Wang, Shijie Cheng, Jia Xie
Summary: This research successfully synthesized O-substituted Li5.5PS4.5-xOxCl1.5 solid electrolytes, among which Li5.5PS4.425O0.075Cl1.5 exhibits high ionic conductivity, improved moisture resistance, and enhanced electrochemical stability in higher voltage windows. Solid-state batteries using Li5.5PS4.425O0.075Cl1.5 show higher capacities and superior cyclability when operated at a high end-of-charge voltage, and exhibit outstanding performance in a wide temperature range.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Zhenkang Wang, Yufeng Cao, Jinqiu Zhou, Jie Liu, Xiaowei Shen, Haoqing Ji, Chenglin Yan, Tao Qian
Summary: This review critically discusses the current status of research on processing robust lithium metal anodes, summarized the strategies to fabricate robust lithium metal anodes with emphasis on the impact on energy density, and proposed future trends and challenges.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Physical
Peiwen Yu, Niaz Ahmad, Chaoyuan Zeng, Lu Lv, Qinxi Dong, Wen Yang
Summary: This study focuses on structural tuning of Li7P3S11 with In2S3 dopant to improve the performance of the electrolyte. The designed Li6.93P2.97In0.02S10.92 electrolyte shows better Li+ conductivity and air stability. In2S3 increases the electrochemical stability window and suppresses the redox decomposition of the electrolyte, resulting in high discharge capacity and low interfacial resistance.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Fengling Zhang, Jingning Lai, Zhengqiang Hu, Anbin Zhou, Huirong Wang, Xin Hu, Lijuan Hou, Bohua Li, Wen Sun, Nan Chen, Li Li, Feng Wu, Renjie Chen
Summary: In this study, a dilute electrolyte containing crown ether additives was tailored to improve the performance of lithium-oxygen batteries (LOBs) by promoting lithium salt dissociation and solvation of Li+ ions. This electrolyte exhibited enhanced electrochemical stability and triggered a solution-mediated Li2O2 growth pathway, leading to a high discharge capacity of 10 828.8 mAh g(carbon)(-1). Furthermore, optimized electrode/electrolyte interfaces promoted the kinetics of oxygen reduction/evolution reactions (ORR/OER) and achieved a dendrite-free Li anode, improving the cycle life of LOBs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Lei Wang, Wei Li, Xinyi Sun, Xiaowei Mu, Chuanchao Sheng, Zhang Wen, Ping He, Haoshen Zhou
Summary: In this study, 1-aminopropyl-3-methylimidazolium bromide (APMImBr) was introduced in dimethyl sulfoxide-based Li-O-2 batteries. The bromide ions act as a redox mediator to catalyze the decomposition of Li2O2 products. Additionally, APMIm(+) serves as a scavenging agent for superoxide radicals and protects the lithium metal anodes with an in situ formed Li3N-rich solid electrolyte interface layer. As a result, the Li-O-2 batteries containing APMImBr exhibited an increased discharge capacity, reduced charge overpotential of approximately 0.61 V, and prolonged cyclic life of over 200 cycles.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
J. Wayne Mullinax, Charles W. Bauschlicher Jr, Kristian B. Knudsen, Pedro L. Arrechea, Rocco P. Viggiano, Donald A. Dornbusch, Justin B. Haskins, Baochau Nguyen, Bryan D. McCloskey, John W. Lawson
Summary: In this study, potential decomposition mechanisms of amide and urea solvents were investigated using density functional theory (DFT). Proton and hydrogen abstraction reactions were examined, and the preferred abstraction sites were identified. It was found that the N-H bond of secondary amides and the α-hydrogen atoms were more susceptible to proton abstraction. Additionally, hydrogen abstraction was more favorable at the N-alkyl substituents and α-hydrogen atoms, resulting in the formation of secondary and tertiary radicals. The presence of a coordinating Li+ ion affected the proton abstraction energies, but not the hydrogen abstraction energies. The study also examined the initial steps of a Baeyer-Villiger oxidation type mechanism and found that barriers for these steps were lower with HO2- as the oxidant compared to LiO2-. A comparison with previous experimental results indicated that no single reaction could be identified as the rate-limiting step for predicting the performance of these solvents in Li-O-2 batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Review
Electrochemistry
Zhuojun Zhang, Xu Xiao, Xingbao Zhu, Peng Tan
Summary: This article mainly focuses on the species transport issues of non-aqueous Li-air batteries, including -Li+ transport across solid surfaces and the electrolyte, O-2 solubility and diffusivity, distribution of intermediates and products, and side reactions by other components from the air. The approaches for enhancing species transport and accelerating reactions are discussed, such as well-designed electrode structures and flowing electrolytes, optimization of reaction interfaces and operating conditions. The aim of this research is to identify the mechanism of transport issues and corresponding challenges and perspectives, guiding the structure design and material selection to achieve high-performance Li-air batteries.
ELECTROCHEMICAL ENERGY REVIEWS
(2023)
Article
Chemistry, Physical
Han Zhang, Ziqi Zeng, Shuping Wang, Yuanke Wu, Changhao Li, Mengchuang Liu, Xinlan Wang, Shijie Cheng, Jia Xie
Summary: A nonflammable diluted highly concentrated electrolyte has been developed to achieve high-voltage and safe lithium metal batteries. This electrolyte exhibits high thermal stability and reduces side reactions and stress crack between the electrolyte and battery materials.
Article
Chemistry, Physical
Florian Gebert, Matilde Longhini, Fosca Conti, Andrew J. Naylor
Summary: The rapid adoption of lithium-ion batteries, especially in transportation, has raised concerns about their safety, particularly regarding the flammable liquid electrolyte. This study identified and tested eight promising non-flammable liquid electrolytes, finding that the phosphorus-free fluorinated solvents outperformed the phosphate and phosphonate-based solvents in terms of performance and capacity retention.
JOURNAL OF POWER SOURCES
(2023)
Article
Nanoscience & Nanotechnology
Bo-Sheng Zhao, Lu Wang, Peng Chen, Sheng Liu, Guo-Ran Li, Ning Xu, Meng-Tao Wu, Xue-Ping Gao
Summary: Glass-ceramic sulfide solid electrolytes like Li7P3S11 are practical propellants for all-solid-state lithium-sulfur batteries, but stability and conductivity issues persist. Through a congener substitution strategy, Li7P3S1 was optimized to Li7P2.9Sb0.1S10.75 with improved chemical stability and high ionic conductivity. The electrolyte exhibited high discharge capacities, remarkable rate performance, and high Coulombic efficiency in the ASSLSB.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Qicheng Zhang, Lei Xu, Xinyang Yue, Jijiang Liu, Xin Wang, Xiaoya He, Zidan Shi, Shuzhang Niu, Wei Gao, Chun Cheng, Zheng Liang
Summary: This study investigates the decomposition kinetics of LiNO3 and proposes a method to tune the inner Helmholtz plane to control the LiNO3 decomposition process. It identifies LiNO as the decomposition intermediate and demonstrates the role of dipole-dipole interaction in facilitating the NO cleavage process, leading to the formation of a Li3N-rich SEI.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Hang Sheng, Xin-Hai Meng, Dong-Dong Xiao, Min Fan, Wan-Ping Chen, Jing Wan, Jilin Tang, Yu-Gang Zou, Fuyi Wang, Rui Wen, Ji-Lei Shi, Yu-Guo Guo
Summary: A stable high-nickel cathode is designed by inducing a dense amorphous Li2CO3 coating layer on the particle surface. This coating layer serves as a physical protection layer and can be transformed into a robust cathode electrolyte interphase (CEI), improving the cathode's interfacial stability and electrochemical performance.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Shichao Ding, Jordan Alysia Barr, Zhaoyuan Lyu, Fangyu Zhang, Maoyu Wang, Peter Tieu, Xin Li, Mark H. Engelhard, Zhenxing Feng, Scott P. Beckman, Xiaoqing Pan, Jin-Cheng Li, Dan Du, Yuehe Lin
Summary: The introduction of phosphorus into Fe-N-C single-atom catalysts enhances the peroxidase-like activity, showing excellent selectivity and stability. A 1D carbon nanowire catalyst with enriched Fe-N-4 active sites and phosphorus doping is designed and synthesized, and it is employed in an enzyme cascade platform for highly sensitive colorimetric detection of the neurotransmitter acetylcholine.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Zhun Dong, Ahmad Mukhtar, Thomas Ludwig, Sneha A. Akhade, ShinYoung Kang, Brandon Wood, Katarzyna Grubel, Mark Engelhard, Tom Autrey, Hongfei Lin
Summary: This study investigates the kinetics of surface-functionalized Pd on carbon catalysts for formate dehydrogenation and the impact of O-functional groups. The study shows that O-functional groups play critical roles in dispersing Pd nanoparticles and decreasing the activation energy, while C-O groups hinder the formation of metallic Pd.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Biochemistry & Molecular Biology
Ewa C. E. Ronnebro, Mark Engelhard, Danny Edwards, Katarzyna Grubel, Anthony Guzman, Randall Storms
Summary: The coating of metal specimens affects the hydrogen gettering performance. This study evaluated the role of post-plating heat treatments on gettering rates, surface composition, and texture. It was found that the pre-heat treatment in air before activation is necessary to avoid slower gettering rates.
Article
Chemistry, Multidisciplinary
Martin Werres, Yaobin Xu, Hao Jia, Chongmin Wang, Wu Xu, Arnulf Latz, Birger Horstmann
Summary: Lithium metal batteries suffer from low cycle life due to the formation of isolated lithium during stripping. The interaction between lithium and solid-electrolyte interphase (SEI) leads to preferred stripping and isolated lithium formation. Cryogenic transmission electron microscopy (cryo TEM) observations confirm that isolated lithium occurs less at higher stripping current densities. To mitigate isolated lithium, a uniform lithium morphology during plating and a homogeneous SEI are indispensable.
Article
Chemistry, Multidisciplinary
Hao Jia, Ju-Myung Kim, Peiyuan Gao, Yaobin Xu, Mark H. Engelhard, Bethany E. Matthews, Chongmin Wang, Wu Xu
Summary: This study systematically investigates and compares localized high-concentration electrolytes (LHCEs) based on five different solvents in lithium-ion batteries (LIBs). The unique solvation structure of LHCEs facilitates the formation of solid electrolyte interphase (SEI) on graphite anode, enabling previously incompatible solvents to achieve reversible lithiation/delithiation. The study also reveals that the long-term cyclability of LIBs can be improved by introducing additives into LHCEs, which results in effective SEIs and cathode electrolyte interphases (CEIs).
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Konstantin Khivantsev, Nicholas R. Jaegers, Hristiyan A. Aleksandrov, Inhak Song, Xavier Isidro Pereira-Hernandez, Mark H. Engelhard, Jinshu Tian, Linxiao Chen, Debora Motta Meira, Libor Kovarik, Georgi N. Vayssilov, Yong Wang, Janos Szanyi
Summary: Atom trapping leads to catalysts with atomically dispersed Ru1O5 sites on (100) facets of ceria, showing excellent activity in catalytic NO oxidation and high NOx storage properties. The Ru1O5 sites exhibit higher stability during calcination and the Ru1/CeO2 catalyst is stable during continuous cycling and in the presence of moisture. In addition, the catalyst shows excellent reactivity for NO reduction by CO at low temperatures. This study highlights the applicability of novel ceria-based single-atom catalysts in NO and CO abatement.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Guangxia Feng, Hao Jia, Yaping Shi, Xu Yang, Yanliang Liang, Mark H. Engelhard, Ye Zhang, Chaojie Yang, Kang Xu, Yan Yao, Wu Xu, Xiaonan Shan
Summary: Reflection interference microscopy enables real-time imaging of the formation and evolution of the solid-electrolyte interphase in batteries, providing valuable insights into its structure and dynamics. The imaging reveals the stratified structure of the interphase, with an inner inorganic layer, an interfacial electrified double layer, and an outer organic-rich layer that is reversible with cycling. The thicknesses of the interphase subcomponents show an inverse correlation, indicating the influence of the inner layer on the formation of the outer layer and lithium nucleation.
NATURE NANOTECHNOLOGY
(2023)
Article
Chemistry, Physical
Isik Su Buyuker, Ben Pei, Hui Zhou, Xia Cao, Zhiao Yu, Sufu Liu, Weiran Zhang, Wu Xu, Ji-Guang Zhang, Zhenan Bao, Yi Cui, Chunsheng Wang, M. Stanley Whittingham
Summary: This study evaluates the electrochemical performance and thermal stability of several advanced electrolytes (mainly ether-based) in high-energy-density lithium-metal batteries. The results show that most ether-based electrolytes have better thermal resilience than carbonate electrolytes. However, extreme voltages can severely destabilize the ether-based electrolytes. Phosphate-based high-concentration electrolytes exhibit improved stability over carbonate electrolytes, even at elevated temperatures. These findings provide valuable guidance for the safety of future electrolyte designs.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Vanessa Lebarbier Dagle, Gregory Collinge, Mohammed Rahmana, Austin Winkelman, Wenda Hu, Jian Zhi Hu, Libor Kovarik, Mark Engelhard, Jennifer Jocz, Yong Wang, Mal-Soon Lee, Vassiliki-Alexandra Glezakou, Debmalya Ray, Roger Rousseau, Robert Dagle
Summary: This study reports on a Cu/ZrO2/SBA-16 catalyst with remarkable olefins selectivity and enhanced stability compared to the Ag/ZrO2/SBA-16 catalyst. Replacing Ag with Cu shifts the reaction pathway of crotonaldehyde hydrogenation, leading to the formation of butyraldehyde. Experimental and computational tools were used to verify the performance and stability advantage of the Cu/ZrO2/SBA-16 catalyst.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Cuixia Cheng, Yadong Zhou, Yaobin Xu, Hao Jia, Jumyeong Kim, Wu Xu, Chongmin Wang, Peiyuan Gao, Zihua Zhu
Summary: We have used experimental and computational methods to study the molecular process of solid-electrolyte interphase (SEI) layer formation under practical conditions. Our findings suggest that the solvation shell structure in the electrolyte has an impact on the mechanism and thickness of the SEI layer.
Article
Multidisciplinary Sciences
Jianghao Zhang, Wenda Hu, Binbin Qian, Houqian Li, Berlin Sudduth, Mark Engelhard, Lian Zhang, Jianzhi Hu, Junming Sun, Changbin Zhang, Hong He, Yong Wang
Summary: In this study, the authors demonstrate that coordinating Pd with alkenyl-type ligands creates an electron-rich environment for selective hydrogenation. The method of forming homogeneous-like Pd catalyst structure with noble metals is crucial for inhibiting side reactions in hydrotreating processes.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Robert F. Hansen, Evan Z. Dalton, Rebecca B. Abney, Mark H. Engelhard, Gerardo Castillo Valdes, Sarah D. Burton, Rosalie K. Chu, Daniel P. Veghte, Swarup China, Yaroslav Losovyj, John B. Cliff, Jonathan D. Raff
Summary: Organicnitrate ester compounds (RONO2) act as sinks for nitrogen oxides (NO x & EQUIV;NO + NO2) and play a crucial role in the formation of ozone and organic aerosols in the lower atmosphere. This study investigates the production of RONO2 in organic aerosols through aqueous phase reactions involving nitronium (NO2 (+)) and humic and fulvic acids. The results provide evidence that NO2 (+) targets the lipid fraction of organic matter and forms stable RONO2 compounds through reactions with terminal alcohols (ROH) and alkenes.
ACS EARTH AND SPACE CHEMISTRY
(2023)
Article
Materials Science, Multidisciplinary
Martin Weiser, Matthew J. Olszta, Mark H. Engelhard, Zihua Zhu, Daniel K. Schreiber
Summary: The transport paths of oxygen during intergranular oxidation in binary Ni-Cr were studied using electron microscopy, atom probe tomography (APT), secondary ion mass spectroscopy, and oxygen tracer exchange experiments. The selective oxidation of Cr was isolated by performing oxidation with a CO/CO2 gas mixture. The results reveal nanometer-scale details of passivation and penetrative intergranular oxidation processes, as well as preferred transport paths at the oxide/alloy interface.
NPJ MATERIALS DEGRADATION
(2023)
Article
Chemistry, Physical
Hyung-Seok Lim, Won-Jin Kwak, Dan Thien Nguyen, Wei Wang, Wu Xu, Ji-Guang Zhang
Summary: Metal-oxygen batteries (MOBs) are promising for energy storage due to safety, low cost, and high energy density. However, the accumulation of discharge products during the oxygen reduction process can hinder the flow of active species, leading to increased impedance and shortened cycle life. A 3D-SOM structure of ruthenium/single-walled carbon nanotubes air electrode is shown to mitigate these effects and enhance the performance of MOBs.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
