4.8 Article

Multiscale operando X-ray investigations provide insights into electro-chemo-mechanical behavior of lithium intercalation cathodes

Journal

APPLIED ENERGY
Volume 299, Issue -, Pages -

Publisher

ELSEVIER SCI LTD
DOI: 10.1016/j.apenergy.2021.117315

Keywords

Lithium-ion battery; X-ray scattering; Transmission X-ray microscopy; Operando measurement; Electro-chemo-mechanical behavior; Surface engineering

Funding

  1. National Science Foundation (NSF) CAREER Award [CMMI1751605]
  2. Scott Institute Seed Grants
  3. Carnegie Mellon University
  4. National Defense Science and Engineering Graduate (NDSEG) Fellowship
  5. National Science Foundation [DEAC0206CH11357]
  6. Advanced Photon Source, Argonne National Laboratory [DEAC0206CH11357]

Ask authors/readers for more resources

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.
The electrochemical performance and cycle life of lithium-ion batteries (LIBs) depend on the electrochemical, chemical, and mechanical behavior of electrodes and electrolytes. Despite extensive studies conducted previously, challenges exist to decouple these behaviors, capture the evolution of electro-chemo-mechanical behavior in realistic conditions, and correlate atomic-scale stress evolution to micro-scale bulk mechanical degradation. Here, we report multiscale operando techniques to investigate polydisperse battery electrodes by integrating volume-averaged quantitative synchrotron X-ray scattering with high-resolution transmission X-ray microscopy (TXM). The former provides us information spanning a wide spatial range, from Angstrom-level atomic structures to micrometer-level particle scales, while the latter provides time-resolved 2D images of the particles during cycling. The complementarity of the two operando techniques is demonstrated by an over-lithiation test of LiCoO2 electrodes, where particles crack and eventually pulverize. Additionally, the techniques are applied to study LiCoO2 cycling stability from 3.0 V to 4.5 V. Operando X-ray scattering result shows nanometer-scale Applied Energy 299 (2021) features keep forming in LiCoO2 electrodes during cycling, resulting in an increased projected area observed by the TXM experiment. The formation of such features is inhibited by a polymer coating on the electrode, leading to vastly improved cycling stability. The polymer coating alleviates LiCoO2 surface deterioration, reduces side product generation, and inhibits LiCoO2 particles volume expansion during the cycling test. These operando multimodal X-ray techniques presented herein thus offer a novel, multiscale diagnostic modality for studying existing and emerging battery materials, aiding the development of next-generation LIBs.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Engineering, Manufacturing

Parametric analysis to quantify process input influence on the printed densities of binder jetted alumina ceramics

Edgar Mendoza Jimenez, Daming Ding, Laisuo Su, Aparna R. Joshi, Aarti Singh, B. Reeja-Jayan, Jack Beuth

ADDITIVE MANUFACTURING (2019)

Article Materials Science, Multidisciplinary

Engineering lithium-ion battery cathodes for high-voltage applications using electromagnetic excitation

Laisuo Su, Shikhar Krishn Jha, Xin Li Phuah, Jiang Xu, Nathan Nakamura, Haiyan Wang, John S. Okasinski, B. Reeja-Jayan

JOURNAL OF MATERIALS SCIENCE (2020)

Article Nanoscience & Nanotechnology

Tailoring Electrode-Electrolyte Interfaces in Lithium-Ion Batteries Using Molecularly Engineered Functional Polymers

Laisuo Su, Jamie L. Weaver, Mitchell Groenenboom, Nathan Nakamura, Eric Rus, Priyanka Anand, Shikhar Krishn Jha, John S. Okasinski, Joseph A. Dura, B. Reeja-Jayan

Summary: Tailoring electrode-electrolyte interfaces (EEIs) using nanoscale polymer thin films deposited via chemical vapor deposition (CVD) can enhance the rate of Li+ transport and improve the charging speed of LiCoO2 in lithium-ion batteries (LIBs). PEDOT coatings form chemical bonds with LiCoO2, reducing Co dissolution and inhibiting electrolyte decomposition, leading to a significant increase in the cycle life of LiCoO2.

ACS APPLIED MATERIALS & INTERFACES (2021)

Article Chemistry, Physical

Operando Particle-Scale Characterization of Silicon Anode Degradation during Cycling by Ultrahigh-Resolution X-ray Microscopy and Computed Tomography

Paul Choi, Bharathy S. Parimalam, Laisuo Su, B. Reeja-Jayan, Shawn Litster

Summary: By combining 2D operando transmission X-ray radiograph sequences with 3D in situ X-ray computed tomography, this study characterized the behavior of a composite silicon anode during cycling in lithium-ion batteries. The X-ray signal attenuation over Si particles decreased with increased lithiation at low cycling rates, whereas increased attenuation was observed at electrode scale during high cycling rates. The simultaneous imaging of a large number of particles in close proximity was a useful feature of this operando imaging technique.

ACS APPLIED ENERGY MATERIALS (2021)

Article Chemistry, Multidisciplinary

High-efficiency, anode-free lithium-metal batteries with a close-packed homogeneous lithium morphology

Laisuo Su, Harry Charalambous, Zehao Cui, Arumugam Manthiram

Summary: Advanced electrolytes can improve the electrochemical performance of anode-free lithium-metal batteries by forming denser and better-packed lithium morphologies, enabling uniform lithium plating over the electrode area and reducing capacity fade. However, the mechanisms by which electrolytes improve performance are still not well understood.

ENERGY & ENVIRONMENTAL SCIENCE (2022)

Article Chemistry, Physical

Protection of Cobalt-Free LiNiO2 from Degradation with Localized Saturated Electrolytes in Lithium-Metal Batteries

Laisuo Su, Eunmi Jo, Arumugam Manthiram

Summary: In this study, a localized saturated electrolyte (LSE) was proposed for developing LiNiO2 cathodes and it was found that LSE can enhance the cycling stability of lithium-metal batteries, protect the surface of the cathode material from degradation, and promote the formation of a robust Li morphology.

ACS ENERGY LETTERS (2022)

Article Green & Sustainable Science & Technology

One-Dimensional Numerical Simulation of Pt-Co Alloy Catalyst Aging for Proton Exchange Membrane Fuel Cells

Yunjie Yang, Minli Bai, Laisuo Su, Jizu Lv, Chengzhi Hu, Linsong Gao, Yang Li, Yubai Li, Yongchen Song

Summary: This paper proposes a one-dimensional degradation model for the Pt-Co alloy catalyst in the cathode catalytic layer of a PEMFC, which can track the catalyst size evolution in real time and demonstrate the catalyst degradation during operation. The results show that severe dissolution of particles near the CCL/membrane leads to uneven aging of the Pt-Co alloy catalyst along the CCL thickness direction. Furthermore, it is found that a slight change in the upper potential limit can cause great harm to the catalyst performance and service life after a certain threshold. The study also reveals that operating temperature affects the Pt mass loss on the carbon support near the CCL/membrane side, but has little effect on the remaining Pt mass near the CCL/GDL side.

SUSTAINABILITY (2022)

Article Multidisciplinary Sciences

Intercalation-type catalyst for non-aqueous room temperature sodium-sulfur batteries

Jiarui He, Amruth Bhargav, Laisuo Su, Harry Charalambous, Arumugam Manthiram

Summary: By coupling the intercalation-type catalyst, MoTe2, with the conversion-type active material, sulfur, a new hybrid positive electrode material was created, which exhibited high discharge capacity and excellent cycling stability under high sulfur loading and lean electrolyte conditions.

NATURE COMMUNICATIONS (2023)

Article Energy & Fuels

Numerical Simulations for Indirect and Direct Cooling of 54 V LiFePO4 Battery Pack

Yulong Li, Zhifu Zhou, Laisuo Su, Minli Bai, Linsong Gao, Yang Li, Xuanyu Liu, Yubai Li, Yongchen Song

Summary: This study used three-dimensional thermal simulations to investigate the cooling effects of different methods on a lithium-ion battery pack. It found that single-phase direct cooling with fluorinated liquid can effectively control the temperature and temperature uniformity of the battery pack. The study also proposed two-phase immersion cooling as a promising new cooling method.

ENERGIES (2022)

Article Energy & Fuels

Cycle life prediction of lithium-ion batteries based on data-driven methods

Laisuo Su, Mengchen Wu, Zhe Li, Jianbo Zhang

Summary: This study demonstrates the capability of machine learning techniques to accurately predict the cycle life of lithium-ion batteries by capturing hidden features in complex, nonlinear systems.

ETRANSPORTATION (2021)

Article Multidisciplinary Sciences

Designing reliable electrochemical cells for operando lithium-ion battery study

Laisuo Su, Paul Choi, Bharathy S. Parimalam, Shawn Litster, B. Reeja-Jayan

Summary: Operando experiments are gaining attention in lithium-ion battery studies for capturing non-equilibrium and fast-transient processes during electrochemical reactions. Designing a suitable and reliable electrochemical cell is crucial for ensuring accurate results, as poorly designed in-situ cells may introduce artifacts and lead to misleading data. This study introduces the steps and details of a specific type of in-situ cell, the modified coin cell, which has shown reliability in various operando experiments.

METHODSX (2021)

Article Chemistry, Physical

Linking far-from-equilibrium defect structures in ceramics to electromagnetic driving forces

Nathan Nakamura, Laisuo Su, Han Wang, Noam Bernstein, Shikhar Krishn Jha, Elizabeth Culbertson, Haiyan Wang, Simon J. L. Billinge, C. Stephen Hellberg, B. Reeja-Jayan

Summary: Exposure to EM fields during materials synthesis can lead to rapid crystallization and phase transitions. Low-energy EM fields can influence atomic structural arrangements, with phase stability mediated by oxygen vacancy-induced structural distortions dependent on local electric field intensity. The link between field strength and atomic structure opens up new possibilities for exploring phase space and material properties.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

Article Chemistry, Physical

In situsynchrotron pair distribution function analysis to monitor synthetic pathways under electromagnetic excitation

Nathan Nakamura, Laisuo Su, Jianming Bai, Sanjit Ghose, B. Reeja-Jayan

JOURNAL OF MATERIALS CHEMISTRY A (2020)

Article Energy & Fuels

Theoretical and experimental investigation on the advantages of auxetic nonlinear vortex-induced vibration energy harvesting

Shitong Fang, Houfan Du, Tao Yan, Keyu Chen, Zhiyuan Li, Xiaoqing Ma, Zhihui Lai, Shengxi Zhou

Summary: This paper proposes a new type of nonlinear VIV energy harvester (ANVEH) that compensates for the decrease in peak energy output at low wind speeds by introducing an auxiliary structure. Theoretical and experimental results show that ANVEH performs better than traditional nonlinear VIV energy harvesters under various system parameter variations.

APPLIED ENERGY (2024)

Article Energy & Fuels

Evaluation method for the availability of solar energy resources in road areas before route corridor planning

Wei Jiang, Shuo Zhang, Teng Wang, Yufei Zhang, Aimin Sha, Jingjing Xiao, Dongdong Yuan

Summary: A standardized method was developed to evaluate the availability of solar energy resources in road areas, which combined the Analytic Hierarchy Process (AHP) and the Geographic Information System (GIS). By analyzing critical factors and using a multi-indicator evaluation method, the method accurately evaluated the utilization of solar energy resources and guided the optimal location selection for road photovoltaic (PV) projects. The results provided guidance for the application of road PV projects and site selection for route corridors worldwide, promoting the integration of transportation and energy.

APPLIED ENERGY (2024)

Article Energy & Fuels

Impacts of PTL coating gaps on cell performance for PEM water electrolyzer

Chang Liu, Jacob A. Wrubel, Elliot Padgett, Guido Bender

Summary: The study investigates the effects of coating defects on the performance of the anode porous transport layer (PTL) in water electrolyzers. The results show that an increasing fraction of uncoated regions on the PTL leads to decreased cell performance, with continuous uncoated regions having a more severe impact compared to multiple thin uncoated strips.

APPLIED ENERGY (2024)

Article Energy & Fuels

Coordinated pricing mechanism for parking clusters considering interval-guided uncertainty-aware strategies

Marcos Tostado-Veliz, Xiaolong Jin, Rohit Bhakar, Francisco Jurado

Summary: In this paper, a coordinated charging price mechanism for clusters of parking lots is proposed. The research shows that enabling vehicle-to-grid characteristics can bring significant economic benefits for users and the cluster coordinator, and vehicle-to-grid impacts noticeably on the risk-averse character of the uncertainty-aware strategies. The developed pricing mechanism can reduce the cost for users, avoiding to directly translate the energy cost to charging points.

APPLIED ENERGY (2024)

Article Energy & Fuels

The establishment of evaluation systems and an index for energy superpower

Duan Kang

Summary: Building an energy superpower is a key strategy for China and a long-term goal for other countries. This study proposes an evaluation system and index for measuring energy superpower, and finds that China has significantly improved its ranking over the past 21 years, surpassing other countries.

APPLIED ENERGY (2024)

Article Energy & Fuels

A model-based study of the evolution of gravel layer permeability under the synergistic blockage effect of sand particle transport and secondary hydrate formation

Fucheng Deng, Yifei Wang, Xiaosen Li, Gang Li, Yi Wang, Bin Huang

Summary: This study investigated the synergistic blockage mechanism of sand and hydrate in gravel filling layer and the evolution of permeability in the layer. Experimental models and modified permeability models were established to analyze the effects of sand particles and hydrate formation on permeability. The study provided valuable insights for the safe and efficient exploitation of hydrate reservoirs.

APPLIED ENERGY (2024)

Article Energy & Fuels

Energy optimization for HVAC systems in multi-VAV open offices: A deep reinforcement learning approach

Hao Wang, Xiwen Chen, Natan Vital, Edward Duffy, Abolfazl Razi

Summary: This study proposes a HVAC energy optimization model based on deep reinforcement learning algorithm. It achieves 37% energy savings and ensures thermal comfort for open office buildings. The model has a low complexity, uses a few controllable factors, and has a short training time with good generalizability.

APPLIED ENERGY (2024)

Article Energy & Fuels

Asymmetry stagger array structure ultra-wideband vibration harvester integrating magnetically coupled nonlinear effects

Moyue Cong, Yongzhuo Gao, Weidong Wang, Long He, Xiwang Mao, Yi Long, Wei Dong

Summary: This study introduces a multi-strategy ultra-wideband energy harvesting device that achieves high power output without the need for external power input. By utilizing asymmetry, stagger array, magnetic coupling, and nonlinearity strategies, the device maintains a stable output voltage and high power density output at non-resonant frequencies. Temperature and humidity monitoring are performed using Bluetooth sensors to adaptively assess the device.

APPLIED ENERGY (2024)

Article Energy & Fuels

Enhancement of hydrogen production via optimizing micro-structures of electrolyzer on a microfluidic platform

Tianshu Dong, Xiudong Duan, Yuanyuan Huang, Danji Huang, Yingdong Luo, Ziyu Liu, Xiaomeng Ai, Jiakun Fang, Chaolong Song

Summary: Electrochemical water splitting is crucial for hydrogen production, and improving the hydrogen separation rate from the electrode is essential for enhancing water electrolyzer performance. However, issues such as air bubble adhesion to the electrode plate hinder the process. Therefore, a methodology to investigate the two-phase flow within the electrolyzer is in high demand. This study proposes using a microfluidic system as a simulator for the electrolyzer and optimizing the two-phase flow by manipulating the micro-structure of the flow.

APPLIED ENERGY (2024)

Article Energy & Fuels

A novel day-ahead scheduling model to unlock hydropower flexibility limited by vibration zones in hydropower-variable renewable energy hybrid system

Shuo Han, Yifan Yuan, Mengjiao He, Ziwen Zhao, Beibei Xu, Diyi Chen, Jakub Jurasz

Summary: Giving full play to the flexibility of hydropower and integrating more variable renewable energy is of great significance for accelerating the transformation of China's power energy system. This study proposes a novel day-ahead scheduling model that considers the flexibility limited by irregular vibration zones (VZs) and the probability of flexibility shortage in a hydropower-variable renewable energy hybrid generation system. The model is applied to a real hydropower station and effectively improves the flexibility supply capacity of hydropower, especially during heavy load demand in flood season.

APPLIED ENERGY (2024)

Article Energy & Fuels

Archery-inspired catapult mechanism with controllable energy release for efficient ultralow-frequency energy harvesting

Zhen Wang, Kangqi Fan, Shizhong Zhao, Shuxin Wu, Xuan Zhang, Kangjia Zhai, Zhiqi Li, Hua He

Summary: This study developed a high-performance rotary energy harvester (AI-REH) inspired by archery, which efficiently accumulates and releases ultralow-frequency vibration energy. By utilizing a magnetic coupling strategy and an accumulator spring, the AI-REH achieves significantly accelerated rotor speeds and enhanced electric outputs.

APPLIED ENERGY (2024)

Article Energy & Fuels

A novel combined probabilistic load forecasting system integrating hybrid quantile regression and knee improved multi-objective optimization strategy

Yi Yang, Qianyi Xing, Kang Wang, Caihong Li, Jianzhou Wang, Xiaojia Huang

Summary: In this study, a novel hybrid Quantile Regression (QR) model is proposed for Probabilistic Load Forecasting (PLF). The model integrates causal dilated convolution, residual connection, and Bidirectional Long Short-Term Memory (BiLSTM) for multi-scale feature extraction. In addition, a Combined Probabilistic Load Forecasting System (CPLFS) is proposed to overcome the inherent flaws of relying on a single model. Simulation results show that the hybrid QR outperforms traditional models and CPLFS exceeds the best benchmarks in terms of prediction accuracy and stability.

APPLIED ENERGY (2024)

Article Energy & Fuels

Capacity fade prediction for vanadium redox flow batteries during long-term operations

Wen-Jiang Zou, Young-Bae Kim, Seunghun Jung

Summary: This paper proposes a dynamic prediction model for capacity fade in vanadium redox flow batteries (VRFBs). The model accurately predicts changes in electrolyte volume and capacity fade, enhancing the competitiveness of VRFBs in energy storage applications.

APPLIED ENERGY (2024)

Article Energy & Fuels

State-of-charge balancing strategy of battery energy storage units with a voltage balance function for a Bipolar DC mircrogrid

Yuechao Ma, Shengtie Wang, Guangchen Liu, Guizhen Tian, Jianwei Zhang, Ruiming Liu

Summary: This paper focuses on the balance of state of charge (SOC) among multiple battery energy storage units (MBESUs) and bus voltage balance in an islanded bipolar DC microgrid. A SOC automatic balancing strategy is proposed considering the energy flow relationship and utilizing the adaptive virtual resistance algorithm. The simulation results demonstrate the effectiveness of the proposed strategy in achieving SOC balancing and decreasing bus voltage unbalance.

APPLIED ENERGY (2024)

Article Energy & Fuels

Deep clustering of reinforcement learning based on the bang-bang principle to optimize the energy in multi-boiler for intelligent buildings

Raad Z. Homod, Basil Sh. Munahi, Hayder Ibrahim Mohammed, Musatafa Abbas Abbood Albadr, Aissa Abderrahmane, Jasim M. Mahdi, Mohamed Bechir Ben Hamida, Bilal Naji Alhasnawi, A. S. Albahri, Hussein Togun, Umar F. Alqsair, Zaher Mundher Yaseen

Summary: In this study, the control problem of the multiple-boiler system (MBS) is formulated as a dynamic Markov decision process and a deep clustering reinforcement learning approach is applied to obtain the optimal control policy. The proposed strategy, based on bang-bang action, shows superior response and achieves more than 32% energy saving compared to conventional fixed parameter controllers under dynamic indoor/outdoor actual conditions.

APPLIED ENERGY (2024)