Article
Chemistry, Physical
Alice J. Merryweather, Quentin Jacquet, Steffen P. Emge, Christoph Schnedermann, Akshay Rao, Clare P. Grey
Summary: Understanding the ion intercalation and degradation mechanisms is crucial for developing high-rate battery electrodes. Operando optical scattering microscopy is used to study single-particle kinetic state-of-charge heterogeneities and cracking in high-rate Li-ion anode materials. This study demonstrates the power of optical scattering microscopy in tracking rapid non-equilibrium processes that would be inaccessible with established characterization techniques.
Article
Chemistry, Multidisciplinary
W. J. Legerstee, M. Boekel, S. Boonstra, E. M. Kelder
Summary: An Atomic Force Microscope (AFM) was combined with a special designed glovebox system and coupled to a Galvanostat/Potentiostat to allow measurements on electrochemical properties for battery research. The study found two dry methods to add lithium to the probe tip for use as an active element in measurements. The developed active probe method can be extended to techniques combining AFM measurements with mapping of electrochemical processes with spatial resolution.
FRONTIERS IN CHEMISTRY
(2021)
Article
Energy & Fuels
Laisuo Su, Paul Choi, Nathan Nakamura, Harry Charalambous, Shawn Litster, Jan Ilavsky, B. Reeja-Jayan
Summary: This study utilizes multiscale operando techniques to investigate battery electrodes, integrating synchrotron X-ray scattering and high-resolution transmission X-ray microscopy. Through an over-lithiation test of LiCoO2 electrodes, the complementarity of the two operando techniques is demonstrated, and the mechanism of the polymer coating in improving cycling stability is discovered.
Review
Chemistry, Multidisciplinary
Marm B. Dixit, Jun-Sang Park, Peter Kenesei, Jonathan Almer, Kelsey B. Hatzell
Summary: This paper highlights the importance of solid-state batteries in achieving electrification of the transportation sector, while also discussing challenges such as electro-chemo-mechanical degradation affecting performance metrics. Characterizing and understanding the solid|solid interfaces in solid-state batteries is crucial for designing high energy density, durable solid-state batteries.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Physical
Paul Choi, Bharathy Parimalam, Yubai Li, Shawn Litster
Summary: This study uses high-resolution in-situ/operando Zernike phase contrast X-ray microscopy to directly observe the lithium electrodeposition process and characterizes it using TXM and CT imaging techniques. The results reveal the nucleation and deposition mechanisms of lithium and provide comprehensive morphology of the resulting structure. The study emphasizes the importance of in-situ/operando characterization of commercially-relevant configurations in developing practical dendrite mitigation strategies.
JOURNAL OF POWER SOURCES
(2023)
Review
Energy & Fuels
Xinan Yan, Jun Huang, Limin Guo, Chuntai Liu, Shaojun Dong, Zhangquan Peng
Summary: Various advanced characterization technologies have been employed to understand and improve the electrochemical performance of aprotic lithium-oxygen batteries, with isotope labeling proving to be a particularly powerful technique. This review focuses on the current understanding of reactions and chemistry in Li-O-2 batteries using isotope-labeling techniques, emphasizing the formation mechanism of product species and identification of reaction interfaces. The authors call for isotope-labeling-related kinetic analysis to clarify remaining controversial issues.
Article
Chemistry, Physical
Andreas Strasser, Alexander Adam, Jiahao Li
Summary: Reducing the charging time is important for increasing the acceptance of electric vehicles. This paper introduces a new method that allows the detection of the onset of lithium plating in automotive lithium-ion batteries using online electrochemical impedance spectroscopy. The detection is based on observing the real part of the impedance across the state of charge during the charging procedure.
JOURNAL OF POWER SOURCES
(2023)
Review
Chemistry, Physical
Yao Yang, Julian Feijoo, Valentin Briega-Martos, Qihao Li, Mihail Krumov, Stefan Merkens, Giuseppe De Salvo, Andrey Chuvilin, Jianbo Jin, Haowei Huang, Christopher J. Pollock, Miquel B. Salmeron, Cheng Wang, David A. Muller, Hector D. Abruna, Peidong Yang
Summary: This review summarizes the recent advances in operando electrochemical liquid-cell scanning transmission electron microscopy and correlative synchrotron X-ray methods, which can comprehensively study reaction dynamics across multiple spatiotemporal scales. To encourage widespread adoption of these advanced methods, the review highlights the need for benchmarking electrochemistry in confined and heterogeneous liquid environments with minimal beam-induced damage.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
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
Multidisciplinary Sciences
Yao Yang, Sheena Louisia, Sunmoon Yu, Jianbo Jin, Inwhan Roh, Chubai Chen, Maria V. Fonseca Guzman, Julian Feijoo, Peng-Cheng Chen, Hongsen Wang, Christopher J. Pollock, Xin Huang, Yu-Tsun Shao, Cheng Wang, David A. Muller, Hector D. Abruna, Peidong Yang
Summary: This study presents a comprehensive investigation of the structural dynamics of Cu nanocatalysts during the electrochemical synthesis of fuels and chemicals. The presence of active Cu nanograins under CO2 reduction conditions and their role in supporting C-C coupling reactions were observed. Quantitative structure-activity correlation revealed that a higher fraction of Cu nanograins leads to higher selectivity for C2+ products. This research provides a powerful platform for advancing our understanding of the complex structural evolution of nanocatalysts under electrochemical conditions.
Article
Nanoscience & Nanotechnology
Mihail R. Krumov, Shuangyan Lang, Lucas Johnson, Hector D. Abruna
Summary: The solid electrolyte interphase (SEI) has a significant impact on the stability and cycling performance of highly reactive battery electrodes. This study uses microscopic, time-resolved operando methods to characterize and understand the SEI formation and degradation processes. The research findings reveal the potential for stable anode passivation at lower potentials and highlight the bidirectional relationship between the SEI and lithium plating-stripping.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Bastian Krueger, Konstantin Kimon Rucker, Gunther Wittstock
Summary: The reoxidation of Li2O2 in Li-O-2 cells is a high overpotential reaction, and using redox mediators can decrease the overpotential, reduce the formation of reactive oxygen species, and convert all the Li2O2. The rate constants of the redox reaction between the mediators and Li2O2 vary with different electrolytes, and the rate constants in ionic liquids are lower than in ether-based electrolytes.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Miao He, Jianping Long, Minglu Li, Ruixin Zheng, Anjun Hu, Dayue Du, Yu Yan, Zhiqun Ran, Longfei Ren, Runjing Li, Chuan Zhao, Xiaojuan Wen, Haoyang Xu, Chaozhu Shu
Summary: Electronic structural engineering, through introduction of exotic dopant and vacancy, enhances the catalytic activity of CoSe2 nanosheets for oxygen redox reactions. Fe dopant and Co defects promote electron delocalization and reduce the adsorption energy of LiO2 intermediate, improving the electrocatalytic activity. The synergistic effect between Co vacancy and Fe dopant optimizes the electronic structure of Co ion and reduces the energy barrier of oxygen electrode reactions. Lithium-oxygen batteries based on Fe-CoSe2-V-Co electrodes exhibit high Coulombic efficiency, large discharge capacity, and excellent cycling life.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Review
Chemistry, Physical
Shiwei Tao, Ming Li, Miaoqiang Lyu, Lingbing Ran, Roger Wepf, Ian Gentle, Ruth Knibbe
Summary: This paper reviews the opportunities and obstacles of closed-cell in operando TEM systems and compares them with open-cell configurations. By observing the processes in closed-cell configurations, a more reliable understanding of the electrochemical setups of most ion batteries under development can be obtained. However, the closed-cell configuration sacrifices imaging resolution.
Article
Chemistry, Physical
Kazuhiko Mukai, Takamasa Nonaka, Takeshi Uyama
Summary: Research revealed a two-phase reaction scheme in lithium titanium oxide during lithium-ion battery operation, with distinct structural transformations observed at different scales. Linear, reversible changes in bond distance between titanium and oxygen atoms were observed at the atomic scale, while hysteresis in lattice parameter between discharge and charge reactions was noted at the microscale. These differences in structural changes were attributed to variances in spatial resolutions between XAS and XRD techniques.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Physical
Zhihua Zhai, Yan Wang, Conghui Si, Pan Liu, Wanfeng Yang, Guanhua Cheng, Zhonghua Zhang
Summary: A novel self-templating strategy was developed to synthesize one-dimensional nanoporous RhNi alloy nanowires. The RhNi nanowires exhibited excellent electrocatalytic activity and stability for hydrogen evolution reaction. This study provides a new solution for the preparation of highly active and stable electrocatalysts in clean energy systems.
Article
Chemistry, Multidisciplinary
Qiwen Zhang, Yixuan Hu, Haofei Wu, Xiaoran Zhao, Mingliang Wang, Sihong Wang, Ruohan Feng, Qing Chen, Fang Song, Mingwei Chen, Pan Liu
Summary: The article reports on a eutectic dealloying strategy to activate porous spinel NiFe2O4 nanowires with multivalent cation substitutions. The obtained NiFeXO4 exhibits superior electrocatalytic performance for the oxygen evolution reaction, delivering a benchmark current density and high stability. This is attributed to lattice distortion and electronic coupling, as well as the absorption of H2O molecules facilitated by the multication substitution strategy.
Article
Materials Science, Multidisciplinary
Yidi Shen, Kolan Madhav Reddy, Jun Li, Mingwei Chen, Qi An
Summary: We investigated the deformation mechanisms in superhard boron carbide (B4C) using a combination of molecular dynamics simulations and transmission electron microscopy experiments. Interestingly, we observed an anomalous quasi-plastic deformation in B4C under ideal shear deformation along the (111)[112] slip system. This behavior can be attributed to the formation and propagation of slip bands, which are stabilized by newly formed bonding during deformation. On the other hand, the dislocation-like mechanism mediated amorphization was observed in B4C under shear deformation along other slip systems.
Article
Chemistry, Multidisciplinary
Kemeng Ji, Guohong Liang, Yuhao Shen, Hongxing Dai, Jiuhui Han, Yoshikazu Ito, Takeshi Fujita, Jun-ichi Fujita, Chengyang Wang, Mingming Chen
Summary: Ordered porous functional materials, including microporous metal-organic frameworks and mesoporous silica, have been extensively studied for their unique physiochemical properties and broad potential applications. However, the lack of ordered macroporous materials, especially those with high crystallinity, hinders the extension of these advantages to a larger scale. Through a co-sacrificial template sequential pyrolysis process, a three-dimensionally ordered macroporous framework material, OMGCs, has been developed, consisting of well-crystallized graphenic carbon and uniformly dispersed metallic nanocrystals. These OMGCs exhibit a low-temperature formation mechanism and may greatly expand the family of ordered porous framework materials for emerging applications.
CELL REPORTS PHYSICAL SCIENCE
(2023)
Article
Engineering, Environmental
Linghui Li, Satoshi Hagiwara, Cheng Jiang, Haruki Kusaka, Norinobu Watanabe, Takeshi Fujita, Fumiaki Kuroda, Akiyasu Yamamoto, Masashi Miyakawa, Takashi Taniguchi, Hideo Hosono, Minoru Otani, Takahiro Kondo
Summary: The current energy crisis and environmental problems associated with fossil fuel use have led to a growing interest in the development of robust, low-cost, and high-performance electrocatalysts for oxygen evolution reaction (OER) in alkaline media. In this study, an OER electrocatalyst is prepared by hybridizing rhombohedral boron monosulfide with graphene, resulting in improved electronic conductivity. The catalytic activity of this electrocatalyst surpasses that of most previously reported counterparts, with an overpotential of 250 mV at 10 mA cm-2. These findings open up possibilities for designing electrocatalysts composed of abundant elements for various renewable energy applications.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Dechao Chen, Jiao Lan, Feng Xie, Jin Peng, Ming Peng, Chen Sun, Zengxi Wei, Shuangliang Zhao, Mengjia Wang, Pan Liu, Lili Han, Yongwen Tan
Summary: Researchers have prepared a nanoporous Ru-doped ReSe2 catalyst with controllable selenium vacancies by regulating the amount of Ru dopants. The catalyst exhibits excellent performance in the N2 reduction reaction, with high Faradaic efficiency and NH3 yield rate. The study also provides insights into the synergistic effect of Ru dopants and selenium vacancies on regulating the proton coverage on the ReSe2 surface and enhancing the overall catalytic performance.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Materials Science, Multidisciplinary
Jing Feng, Yanfeng Han, Xiaocang Han, Xiaodong Wang, Shuangxi Song, Baode Sun, Mingwei Chen, Pan Liu
Summary: Titanium diboride (TiB2) is an effective grain refiner for Al alloys, but the atomic kinetics of heterogeneous nucleation of Al on TiB2 are still unknown. In this study, atomic-scale observations were made to investigate the heterogeneous nucleation and growth kinetics of Al on self-formed TiB2 particles. It was found that an ordered Al monolayer forms on the Ti-terminated {0001}(TiB2) surface, and then an island-shaped Al nucleus with {111} stacking is initiated without a Ti-rich buffer layer. The interfacial lattice mismatch causes significant out-of-plane strain, which gradually decreases as the Al nucleus grows in layers. TiB2 particles stabilize the Al nuclei rather than promoting their free growth into grains when the experimental undercooling is below a certain threshold. These findings provide insights into the atomic-scale mechanisms of heterogeneous nucleation and growth of Al with the participation of TiB2 and the strain-dependent growth kinetics of Al nuclei.
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
(2023)
Article
Materials Science, Multidisciplinary
Christopher Florencio Aleman, Jiecheng Lyu, Mehmet A. Noyan, Kathleen M. McCreary, Jiuhui Han, Isaac Johnson, Qingyang Gao, Maximilian Niebur, Berend T. Jonker, Mingwei Chen
Summary: A three-dimensional nanoarchitectured hexagonal boron nitride (hBN) is developed with integrated single photon emitters (SPEs) generated from native defects. The structure consists of a continuous 2D hBN sheet with built-in convex and concave curvatures, promoting the formation of optically active and thermally stable defects. The 3D hBN eliminates substrate disturbance and minimizes lattice strain heterogeneity, resulting in narrow spectral distribution of SPEs.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Samuel Jeong, Tatsuhiko Ohto, Tomohiko Nishiuchi, Yuki Nagata, Jun-ichi Fujita, Yoshikazu Ito
Summary: To realize advanced fuel-cell technology, proton exchange membranes with high proton conductivity and low crossover of fuel molecules are required. In this study, a simple yet powerful method is proposed to optimize the crossover-conductivity relationship by using sulfanilic-functionalized holey graphenes supported by a Nafion membrane. The results show significant reduction in crossover and proton conductivity, indicating potential for application in advanced fuel cells that use methanol and formic acid as chemical fuels.
Article
Chemistry, Physical
Takashi Hihara, Yasuyuki Banno, Makoto Nagata, Takeshi Fujita, Hideki Abe
Summary: Atmosphere-treated Pd/CeO2 shows improved catalytic performance in the remediation of lean-burn exhausts at temperatures <300℃. The improvement is attributed to the oxidative decomposition of PdCx species during catalysis, which creates surface Pd sites to promote the remediation process.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Materials Science, Multidisciplinary
Baichen Lin, Yanyi Zhang, Hongjian Zhang, Haofei Wu, Junda Shao, Jian Shao, Kai Liu, Shanquan Chen, Chao Zhou, Xianlong Cheng, Jingyu Lu, Kailong Hu, Yan Huang, Weiwei Zhao, Pan Liu, Jixin Zhu, Hua-Jun Qiu, Zuhuang Chen
Summary: Two-dimensional (2D) metals have attracted significant attention for their unique properties and potential applications. However, the fabrication of atomically thin 2D metals remains challenging. In this study, we demonstrate a general method to fabricate freestanding, high-quality 2D metals with large aspect ratios and controllable thickness using Pt as a model system.
ACS MATERIALS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Peng Cui, Tongheng Wang, Xuhai Zhang, Xinyao Wang, Haofei Wu, Yangkun Wu, Chongyang Ba, Yuqiao Zeng, Pan Liu, Jianqing Jiang
Summary: This study successfully developed single crystalline NiFeCu oxide catalysts with a hierarchical porous structure by combining a rapid epitaxial formation method with dynamic bubble-templated electrodeposition. The structure promotes electron transportation and retards oxygen atom diffusion, while providing ideal channels for oxygen bubble release. As a result, the catalysts exhibited higher efficiency and stability in catalyzing the oxygen evolution reaction compared to commercial catalysts at an industrial scale.
Article
Chemistry, Physical
Tomoya Yoshizaki, Takeshi Fujita
Summary: This study fabricated and characterized nanoporous high-entropy alloy catalysts using dealloying, and investigated their thermal stabilities and phase separation behaviors. A network visualization technique was employed to discern the affinity of different elements in extreme mixing states, providing valuable insights for the design of novel thermally-stable high-entropy alloys and catalysts.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Materials Science, Ceramics
Chuchu Yang, Bin Feng, Naoya Shibata, Yuichi Ikuhara
Summary: The effect of different annealing atmospheres on the atomic structures and dopant segregation behaviors in alumina grain boundaries was studied. It was found that the atomic structure of Ti-doped grain boundaries is symmetric in reducing atmosphere, while it becomes asymmetric with further annealing in air.
JOURNAL OF THE CERAMIC SOCIETY OF JAPAN
(2023)
Article
Chemistry, Multidisciplinary
Mengjia Wang, Ruichun Luo, Yuxin Liu, Xiaoran Zhao, Xiaodong Zhuang, Wen Wu Xu, Mingwei Chen, Pan Liu
Summary: The interface engineering of 2D transition metal dichalcogenides (2D-TMDs) and metals is an efficient method to adjust their electrical and optoelectronic properties. In this study, a 2D non-van der Waals (vdW) Mo-rich phase was discovered during the growth of molybdenum disulfide (MoS2) from a Mo-Au surface alloy in a S-poor environment. This Mo-rich phase preferentially nucleates between the outermost 2D MoS2 and a 3D nanostructured Au substrate, leading to a n-type contact interface with an ultralow transition energy barrier height.
