Article
Chemistry, Multidisciplinary
Lei Xu, Ye Xiao, Yi Yang, Shi-Jie Yang, Xiao-Ru Chen, Rui Xu, Yu-Xing Yao, Wen-Long Cai, Chong Yan, Jia-Qi Huang, Qiang Zhang
Summary: The relationship between electrical double layer capacitance and electrochemical active surface area of graphite anodes during Li-ion intercalation and Li plating processes is revealed. A lithium plating determination method based on dynamic capacitance measurement is proposed, which allows real-time monitoring of the onset of lithium plating in a working battery.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
He Hao, Miao-Ling Lin, Bo Xu, Heng Wu, Yuechen Wang, Hailin Peng, Ping-Heng Tan, Lianming Tong, Jin Zhang
Summary: The characterization of interlayer coupling in two-dimensional van der Waals heterostructures (vdWHs) is crucial for understanding their quantum behaviors and structural functionalities. Twisted bilayer graphene (tBLG) provides a universal strategy to enhance layer-breathing (LB) phonons in vdWHs. By resonantly exciting electrons in tBLG, LB phonons extended over the entire layers in vdWHs can be strongly coupled, and this coupling can be tuned by the twist angle of tBLG. This method of enhancing LB phonons by tBLG is promising for investigating electron-phonon coupling and interlayer interaction in related vdWHs.
Article
Chemistry, Physical
Suting Weng, Siyuan Wu, Zepeng Liu, Gaojing Yang, Xiaozhi Liu, Xiao Zhang, Chu Zhang, Qiuyan Liu, Yao Huang, Yejing Li, Mehmet N. Ates, Dong Su, Lin Gu, Hong Li, Liquan Chen, Ruijuan Xiao, Zhaoxiang Wang, Xuefeng Wang
Summary: In this study, the staging structure and evolution of lithium-intercalated graphite were revealed at the nanoscale using cryogenic-transmission electron microscopy and other methods. The intercalated lithium ions were found to distribute unevenly, leading to local stress and dislocations in the graphite structure. Each staging compound exhibited macroscopic order but microscopic inhomogeneity, revealing a localized-domains structural model.
Article
Chemistry, Physical
Yuqiang Zeng, Divya Chalise, Yanbao Fu, Joseph Schaadt, Sumanjeet Kaur, Vince Battaglia, Sean D. Lubner, Ravi S. Prasher
Summary: The study utilizes thermal waves for real-time probing of lithium concentration within battery electrodes, providing more spatial information compared to traditional tools, which offers a valuable sensing method for studying electrode degradation.
Review
Chemistry, Multidisciplinary
Giovanni Pizzi, Silvia Milana, Andrea C. Ferrari, Nicola Marzari, Marco Gibertini
Summary: This study focuses on the Raman and infrared spectroscopy of layered materials, presenting a general approach to predict spectroscopic fan diagrams for multilayers composed of identical layers. The method combines a description of normal modes with symmetry arguments to identify optically active modes and provide diagrams for any stack of identical layers.
Article
Multidisciplinary Sciences
Sasawat Jamnuch, Tod A. Pascal
Summary: This study explores the electronic and atomic states of Lithium graphite intercalation compounds (Li-GICs) at different degrees of Lithium loading using simulations. The research finds that the enhancement of Li-ion entropy is due to Lorentzian lithium-ion dynamics and charge fluctuations, which activate low-energy phonon modes. The study also reveals that these features are reflected in spectroscopy, expanding the traditional view of X-ray absorption spectroscopy.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
B. Rais, E. T. Ostrowski, A. Canton, C. H. Skinner, S. Barison, S. Fiameni, B. E. Koel
Summary: Lithium wall conditioning using pellet injection and evaporation in the RFX-mod device showed that lithium evaporation resulted in highly localized lithium deposition with specific features on HR-XPS peaks, indicating hydrogenation of fresh graphite during He plasma discharge exposure. This has implications for density control and the selection of lithium conditioning techniques in magnetic fusion devices.
APPLIED SURFACE SCIENCE
(2021)
Article
Engineering, Environmental
Kai He, Zhi-Yuan Zhang, Fu-Shen Zhang
Summary: The recycling of spent Li-ion batteries is crucial for sustainable development of the battery industry. A process has been developed to prepare graphene and recover lithium from spent graphite, which can be efficiently produced when re-charging spent Li-ion batteries.
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
Shiheng Li, Zhiyang Cui, Chao Wang, Jianming Yu, Zhenda Lu
Summary: A composite layer of poly(acrylic acid) and manganese oxide was coated on SnO2 nanoparticles to address volume variation issues, improving the performance and cycling life of lithium-ion batteries. The protection layer and prelithiation technology effectively suppressed side reactions and solid electrolyte interphases, resulting in stable cycling performance and high Coulombic efficiency.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Andrew L. Davis, Vishwas Goel, Daniel W. Liao, Mark N. Main, Eric Kazyak, John Lee, Katsuyo Thornton, Neil P. Dasgupta
Summary: The study found that the rate capability of composite electrodes in solid-state batteries is often limited, with factors including electrostatic potential and solid-state diffusion. Model systems of graphite/Li6PS5Cl composite electrodes can help researchers understand these limiting factors.
ACS ENERGY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Zhao Wang, Chang Yu, Huawei Huang, Wei Guo, Changtai Zhao, Weicheng Ren, Yuanyang Xie, Jieshan Qiu
Summary: The research introduces a novel field-induced energy accumulation strategy to achieve fast preparation of FeCl3-graphite intercalation compounds, which exhibit high volumetric capacity and self-activation characteristics in lithium storage. These findings provide valuable insights for further exploration of metal chloride-intercalated graphite for lithium storage applications.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Jinkun Wang, Yun Gao, Jianhong Liu, Hongying Liao, Li Wang, Xiangming He
Summary: This study investigates the phase evolution and Li+ diffusion kinetics in lithium-ion batteries through operando X-ray diffraction. By analyzing the behavior and structural changes of NCM811/Graphite cells at different C-rates, practical suggestions for real-time monitoring and identification of electrode state, materials and electrode structural design, and optimization of charging/discharging protocols are proposed.
Article
Chemistry, Physical
Abhi Raj, Ilya A. Shkrob, John S. Okasinski, Marco-Tulio Fonseca Rodrigues, Andrew C. Chuang, Xiang Huang, Daniel P. Abraham
Summary: This study uses energy dispersive X-ray diffraction to analyze the evolution of ordered LixC6 phases in solid electrodes of lithium-ion cells, presenting methods for determining lithium concentration and concentration gradients. Experimental results show that concentration gradients persist in lithiated graphite electrodes even after long periods of open-circuit conditions. A multiphase electrochemical model can explain many observed behaviors, but underestimates concentration gradients in both the oxide cathode and graphite anode.
JOURNAL OF POWER SOURCES
(2021)
Article
Electrochemistry
M. A. Cabanero, M. Hagen, E. Quiroga-Gonzalez
Summary: High spatial resolution in-operando Raman spectroscopy was used to study lithium deposition on graphite electrodes, showing that lithium is deposited and intercalated into graphite simultaneously. After 30 minutes, a second mechanism becomes dominant. The evolution of G and D bands of graphite and the lithium concentration in the electrolyte suggest that EC is slowly consumed after lithium plating begins.
ELECTROCHIMICA ACTA
(2021)
Article
Chemistry, Physical
Jesus Barrio, Angus Pedersen, Jingyu Feng, Saurav Ch Sarma, Mengnan Wang, Alain Y. Li, Hossein Yadegari, Hui Luo, Mary P. Ryan, Maria-Magdalena Titirici, Ifan E. L. Stephens
Summary: Single-atom catalysts, particularly the Fe-N-C family, have emerged as a promising alternative to platinum group metals in fuel cells for the oxygen reduction reaction. This work presents a novel method for the targeted synthesis of dual metal atom catalysts, which can significantly enhance the catalytic activity and efficiency.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Zhen Xu, Jing Wang, Zhenyu Guo, Fei Xie, Haoyu Liu, Hossein Yadegari, Mike Tebyetekerwa, Mary P. Ryan, Yong-Sheng Hu, Maria-Magdalena Titirici
Summary: This study successfully synthesized high-performance hard carbon anodes through a combination of hydrothermal carbonization pre-treatment and high-temperature carbonization. The structure and sodium-ion storage mechanism of the anodes were investigated, and the environmental impacts of hydrothermal pre-treatment and direct carbonization were evaluated. It was found that hydrothermal pre-treatment improves electrochemical performance, increases carbon yields, and reduces carbon emissions.
ADVANCED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Hao Zhang, Jiefeng Diao, Mengzheng Ouyang, Hossein Yadegari, Mingxuan Mao, Mengnan Wang, Graeme Henkelman, Fang Xie, D. Jason Riley
Summary: In this study, trimetallic heterostructured core-shell nanoboxes based on Prussian blue analogues (Ni-Co@Fe-Co PBA) were synthesized and showed remarkable electrocatalytic performance for the hydrogen evolution reaction (HER) in alkaline freshwater and simulated seawater.
Article
Chemistry, Physical
O. Westhead, M. Spry, A. Bagger, Z. Shen, H. Yadegari, S. Favero, R. Tort, M. Titirici, M. P. Ryan, R. Jervis, Y. Katayama, A. Aguadero, A. Regoutz, A. Grimaud, I. E. L. Stephens
Summary: Since 2019, numerous high-profile papers have reported improved efficiency of lithium-mediated electrochemical nitrogen reduction to make ammonia. However, there is a lack of systematic investigation linking bulk electrolyte properties to electrochemical performance and Solid Electrolyte Interphase (SEI) properties. This study reveals that the salt concentration has a remarkable effect on electrolyte stability and the formation of a more stable SEI layer with increasing salt concentration. Higher salt concentrations result in decreased faradaic efficiency due to decreased nitrogen solubility and diffusivity, as well as increased SEI conductivity.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Matthew Spry, Olivia Westhead, Romain Tort, Benjamin Moss, Yu Katayama, Maria-Magdalena Titirici, Ifan E. L. Stephens, Alexander Bagger
Summary: Adding a small amount of water as an electrolyte additive can greatly improve the Faradaic selectivity of nitrogen reduction to ammonia in a lithium-mediated system under ambient conditions.
ACS ENERGY LETTERS
(2023)
Review
Chemistry, Multidisciplinary
Olivia Westhead, Jesus Barrio, Alexander Bagger, James W. Murray, Jan Rossmeisl, Maria-Magdalena Titirici, Rhodri Jervis, Andrea Fantuzzi, Andrew Ashley, Ifan E. L. Stephens
Summary: This Review provides a coherent comparison of recent progress made in dinitrogen fixation on solid electrodes, homogeneous catalysts, and nitrogenases. By establishing the cross-cutting themes and synergies between these systems, we identify viable avenues for future research.
NATURE REVIEWS CHEMISTRY
(2023)
Article
Chemistry, Physical
Amanda S. Petersen, Kim D. Jensen, Hao Wan, Alexander Bagger, Ib Chorkendorff, Ifan E. L. Stephens, Jan Rossmeisl, Maria Escudero-Escribano
Summary: In this study, the effects of phosphate anion poisoning on the oxygen reduction reaction (ORR) activity of Pt-based electrodes were investigated using a computational model and rotating disk electrode measurements. By varying the subsurface Cu content of a Cu/Pt(111) alloy, the *OH binding energies on the surface were tuned through ligand effects, resulting in tuning of the ORR activity. The adsorbed phosphate species on the surface were found to directly affect the adsorption of *OH, and the three-fold binding sites of phosphate anions limited the packing of poisoning phosphate, allowing for *OH adsorption even when the surface was poisoned.
Correction
Chemistry, Multidisciplinary
Olivia Westhead, Jesus Barrio, Alexander Bagger, James W. Murray, Jan Rossmeisl, Maria-Magdalena Titirici, Rhodri Jervis, Andrea Fantuzzi, Andrew Ashley, Ifan E. L. Stephens
NATURE REVIEWS CHEMISTRY
(2023)
Article
Chemistry, Physical
Galo J. Paez Fajardo, Eleni Fiamegkou, James A. Gott, Heng Wang, Israel Temprano, Ieuan D. Seymour, Matthew J. W. Ogley, Ashok S. Menon, Ifan E. L. Stephens, Muhammad Ans, Tien-Lin Lee, Pardeep K. Thakur, Wesley M. Dose, Michael F. L. De Volder, Clare P. Grey, Louis F. J. Piper
Summary: Oxygen loss at high voltages in Ni-rich NMC//graphite Li-ion batteries promotes degradation, and the choice of depth of discharge can further accelerate aging. The study reveals that a lower cutoff voltage does not affect capacity retention when oxygen loss is not promoted, but when NMC surface oxygen loss is induced, deeper depth of discharge leads to pronounced faster aging.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Zamaan Mukadam, Sihang Liu, Angus Pedersen, Jesus Barrio, Sarah Fearn, Saurav Ch. Sarma, Maria-Magdalena Titirici, Soren B. Scott, Ifan E. L. Stephens, Karen Chan, Stefano Mezzavilla
Summary: In this study, Cu and Co single-atom catalysts supported on carbon electrodes were used to investigate the electrochemical reduction of furfural, a biomass-derived chemical. Under mild conditions, hydrofuroin, a valuable precursor to sustainable jet fuels, was selectively produced. The study also revealed insights into the mechanism and stability of the catalysts and provided a blueprint for catalyst design in this reaction.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
O. Westhead, R. Tort, M. Spry, J. Rietbrock, R. Jervis, A. Grimaud, A. Bagger, I. E. L. Stephens
Summary: The verification of the lithium-mediated nitrogen reduction system in 2019 has resulted in an increase in literature on improving the faradaic efficiency, stability, and activity. However, accurately quantifying the overpotential and analyzing voltage losses has been challenging. This study presents a simple method for determining the Reversible Hydrogen Electrode potential in the system and identifies sources of potential losses. The observed minimum overpotential was -3.59 +/- 0.07 V vs. RHE, with a faradaic efficiency of 6.5 +/- 0.2%.
FARADAY DISCUSSIONS
(2023)
Review
Chemistry, Physical
Hans Becker, James Murawski, Dipak V. Shinde, Ifan E. L. Stephens, Gareth Hinds, Graham Smith
Summary: Low temperature water electrolysers are sensitive to water quality and common impurities can affect the device performance and lifetime. Purifying the feed water adds cost and complexity, and failure of purification equipment can cause degradation of the electrolysers. This review provides a comprehensive overview of impurities in operating electrolysers, including their sources, degradation mechanisms, characterization techniques, water purification technologies, and mitigation strategies. It generalizes existing mechanisms, proposes new ones, and offers a framework for considering operational implications.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Chemistry, Multidisciplinary
Angus Pedersen, Jinil Pandya, Grazia Leonzio, Alexey Serov, Andrea Bernardi, Ifan E. L. Stephens, Maria-Magdalena Titirici, Camille Petit, Benoit Chachuat
Summary: This study compares the environmental impacts and economic analysis of using non-Pt-based electrocatalyst Fe-N-C to replace Pt/C in PEMFCs. The findings show that Fe-N-C can reduce environmental damages and human health impacts, but it still faces issues such as electricity consumption and resource depletion. The cost of PEMFC stacks with Fe-N-C cathode would increase compared to those with Pt/C cathode due to the increase in environmental externalities. Continued improvement of Fe-N-C performance is necessary to replace Pt-based cathode catalysts in PEMFCs.
Article
Chemistry, Physical
Angus Pedersen, Alexander Bagger, Jesus Barrio, Frederic Maillard, Ifan E. L. Stephens, Maria-Magdalena Titirici
Summary: Proton exchange membrane fuel cells need to reduce construction costs to improve commercial viability, which can be achieved by eliminating platinum and using single metal atoms coordinated to nitrogen-doped carbon (M-N-C) as alternative electrocatalysts for O-2 reduction. In the past decade, significant progress has been made in the synthesis, characterization, and electrocatalytic performance of M-N-Cs. This Perspective article provides a review of the important achievements in the last decade, discusses current gaps in knowledge, and suggests future research directions. Additionally, it presents a new outlook on M-N-C stability and atomistic understanding using density functional theory simulations.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Jihong Shi, Maxwell Fulford, Hui Li, Mariam Marzook, Maryam Reisjalali, Matteo Salvalaglio, Carla Molteni
Summary: This study investigates the pre-melted quasi-liquid layers (QLLs) on ice surfaces using molecular dynamics simulations. The results show that different order parameters give qualitatively similar trends for the behaviors of the QLLs with temperature. The thickness of the QLLs on the ice surface increases gradually as the temperature increases.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)