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Abstract The ability to control the electrode interfaces in an electrochemical energy storage system is essential for achieving the desired electrochemical performance. However, achieving this ability requires an in-depth understanding of the detailed interfacial nanostructures of the electrode under electrochemical operating conditions. In-situ transmission electron microscopy (TEM) is one of the most powerful techniques for revealing electrochemical energy storage mechanisms with high spatiotemporal resolution and high sensitivity in complex electrochemical environments. These attributes play a unique role in understanding how ion transport inside electrode nanomaterials and across interfaces under the dynamic conditions within working batteries. This review aims to gain an in-depth insight into the latest developments of in-situ TEM imaging techniques for probing the interfacial nanostructures of electrochemical energy storage systems, including atomic-scale structural imaging, strain field imaging, electron holography, and integrated differential phase contrast imaging. Significant examples will be described to highlight the fundamental understanding of atomic-scale and nanoscale mechanisms from employing state-of-the-art imaging techniques to visualize structural evolution, ionic valence state changes, and strain mapping, ion transport dynamics. The review concludes by providing a perspective discussion of future directions of the development and application of in-situ TEM techniques in the field of electrochemical energy storage systems. 

Abstract The ability to control phase structures and surface sites of ultrasmall alloy nanoparticles under reaction conditions is essential for preparing catalysts by design. This is, however, challenging due to limited understanding of the atomic‐scale phases and their correlation with the ensemble‐averaged structures and activities of catalysts during catalytic reactions. We reveal here a dynamic structural stability of alumina‐supported ultrasmall and equiatomic copper‐gold alloy nanoparticles under reaction conditions as a model system in the in situ/operando study. In situ atomic‐scale morphological tracking under oxygen reveals temperature‐dependent dynamic crystalline‐amorphous dual‐phase structures, showing dynamic stability over an elevated temperature range. This atomic‐scale dynamic phase stability coincides with a “conversion plateau” observed for carbon monoxide oxidation on the catalyst. It is substantiated by the stable lattice ordering/disordering structures and surface sites with oscillatory characteristics shown by operando ensemble‐average structural tracking of the catalyst during the oxidation reaction. The understanding of the atomic‐scale dynamic phase structures in correlation with the ensemble‐average dynamic ordering/disordering phase structures and surface sites provides fresh insights into the unique synergy of the supported alloy nanoparticles. This understanding has implications for the design and structural tuning of active and stable ultrasmall alloy catalysts under elevated temperatures. 

Abstract Proton exchange‐membrane fuel cell (PEMFC) is a clean and efficient type of energy storage device. However, the sluggish reaction rate of the cathode oxygen reduction reaction (ORR) has been a significant problem in its development. This review reports the recent progress of advanced electrocatalysts focusing on the interface/surface electronic structure and exploring the synergistic relationship of precious‐based and non‐precious metal‐based catalysts and support materials. The support materials contain non‐metal (C/N/Si, etc.) and metal‐based structures, which have demonstrated a crucial role in the synergistic enhancement of electrocatalytic properties, especially for high‐temperature fuel cell systems. To improve the strong interaction, some exciting synergistic strategies by doping and coating heterogeneous elements or connecting polymeric ligands containing carbon and nitrogen were also shown herein. Besides the typical role of the crystal surface, phase structure, lattice strain, etc., the evolution of structure‐performance relations was also highlighted in real‐time tests. The advanced in situ characterization techniques were also reviewed to emphasize the accurate structure‐performance relations. Finally, the challenge and prospect for developing the ORR electrocatalysts were concluded for commercial applications in low‐ and high‐temperature fuel cell systems. 

Abstract As one of the noninvasive screening and diagnostic tools for human breath monitoring of various diseases, chemiresistive devices with nanomaterials as the sensing interfaces for detecting volatile organic compounds (VOCs) have attracted increasing interests. A key challenge for the practical applications is an effective integration of all components in a system level. By integrating with the system components, it provides reliable and rapid results as a fast‐screening method for healthcare, safety, and environmental monitoring. This paper highlights some of the latest developments in chemiresistive sensors designed for the detection of VOCs and human breaths. It begins with a brief introduction to the fundamental principles of chemiresistive sensors with nanoparticle‐structured sensing interfaces. This is followed by a discussion of the recent fabrication methods, with an emphasis on nanostructured materials. Some of the recent examples will be highlighted in terms of recent innovative approaches to sensor applications and system integrations. Challenges and opportunities will also be discussed for the advancement and refinement of the chemiresistive sensor technologies in breath screening and monitoring of diseases. 

Abstract The advancement of clean energy and environment depends strongly on the development of efficient catalysts in a wide range of heterogeneous catalytic reactions, which has benefited from transmission electron microscopic techniques in determining the atomic‐scale morphologies and structures. However, it is the morphology and structure under the catalytic reaction conditions that determine the performance of the catalyst, which has captured a surge of interest in developing and applying in situ/operando transmission electron microscopic techniques in heterogeneous catalysis. The major theme of this review is to highlight some of the most recent insights into heterogeneous catalysts under the relevant reaction conditions using in situ/operando transmission electron microscopic techniques. Rather than a comprehensive overview of the basic principles of in situ/operando techniques, this review focuses on the insights into the atomic‐scale/nanoscale details of various catalysts ranging from single‐component to multicomponent catalysts under heterogeneous catalytic, electrocatalytic, and photocatalytic reaction conditions involving both gas–solid and liquid–solid interfaces. This focus is coupled with discussions of the correlation of the atomic, molecular, and nanoscale morphology, composition, and structure with the catalytic properties under the reaction conditions, shining light on the challenges and opportunities in design of nanostructured catalysts for clean and sustainable energy applications.