Review of the Real-Time Monitoring Technologies for Lithium Dendrites in Lithium-Ion Batteries.

Lithium-ion batteries (LIBs) have the advantage of high energy density, which has attracted the wide attention of researchers. Nevertheless, the growth of lithium dendrites on the anode surface causes short life and poor safety, which limits their application. Therefore, it is necessary to deeply understand the growth mechanism of lithium dendrites. Here, the growth mechanism of lithium dendrites is briefly summarized, and the real-time monitoring technologies of lithium dendrite growth in recent years are reviewed. The real-time monitoring technologies summarized here include in situ X-ray, in situ Raman, in situ resonance, in situ microscopy, in situ neutrons, and sensors, and their representative studies are summarized. This paper is expected to provide some guidance for the research of lithium dendrites, so as to promote the development of LIBs.

Toward Durable CO2 Electroreduction with Cu-Based Catalysts via Understanding Their Deactivation Modes.

The technology of CO2 electrochemical reduction (CO2ER) provides a means to convert CO2, a waste greenhouse gas, into value-added chemicals. Copper is the most studied element that is capable of catalyzing CO2ER to obtain multicarbon products, such as ethylene, ethanol, acetate, etc., at an appreciable rate. Under the operating condition of CO2ER, the catalytic performance of Cu decays because of several factors that alters the surface properties of Cu. In this review, these factors that cause the degradation of Cu-based CO2ER catalysts are categorized into generalized deactivation modes, that are applicable to all electrocatalytic systems. The fundamental principles of each deactivation mode and the associated effects of each on Cu-based catalysts are discussed in detail. Structure- and composition-activity relationship developed from recent in situ/operando characterization studies are presented as evidence of related deactivation modes in operation. With the aim to address these deactivation modes, catalyst design and reaction environment engineering rationales are suggested. Finally, perspectives and remarks built upon the recent advances in CO2ER are provided in attempts to improve the durability of CO2ER catalysts.

Electrocatalysis Mechanism and Structure-Activity Relationship of Atomically Dispersed Metal-Nitrogen-Carbon Catalysts for Electrocatalytic Reactions.

Atomically dispersed metal-nitrogen-carbon catalysts (M-N-C) have been widely used in the field of energy conversion, which has already attracted a huge amount of attention. Due to their unsaturated d-band electronic structure of the center atoms, M-N-C catalysts can be applied in different electrocatalytic reactions by adjusting their own microscopic electronic structures to achieve the optimization of the structure-activity relationship. Consequently, it is of great significance for the revelation of electrocatalytic mechanism and structure-activity relationship of M-N-C catalysts. Thus, this review first introduces the relative research methods, including in situ/operando characterization techniques and theoretical calculation methods. Furthermore, clarifying the electrocatalytic mechanism and structure-activity relationship of M-N-C catalysts in different electrochemical energy conversion reactions is focused. Moreover, the future research directions are pointed out based on the discussion. This review will provide good guidance to systematically study the catalytic mechanism of single-atom catalysts and reasonably design the single-atom catalysts.

Oxygen Evolution Electrocatalysts for the Proton Exchange Membrane Electrolyzer: Challenges on Stability.

Hydrogen generated by proton exchange membrane (PEM) electrolyzer holds a promising potential to complement the traditional energy structure and achieve the global target of carbon neutrality for its efficient, clean, and sustainable nature. The acidic oxygen evolution reaction (OER), owing to its sluggish kinetic process, remains a bottleneck that dominates the efficiency of overall water splitting. Over the past few decades, tremendous efforts have been devoted to exploring OER activity, whereas most show unsatisfying stability to meet the demand for industrial application of PEM electrolyzer. In this review, systematic considerations of the origin and strategies based on OER stability challenges are focused on. Intrinsic deactivation of the material and the extrinsic balance of plant-induced destabilization are summarized. Accordingly, rational strategies for catalyst design including doping and leaching, support effect, coordination effect, strain engineering, phase and facet engineering are discussed for their contribution to the promoted OER stability. Moreover, advanced in situ/operando characterization techniques are put forward to shed light on the OER pathways as well as the structural evolution of the OER catalyst, giving insight into the deactivation mechanisms. Finally, outlooks toward future efforts on the development of long-term and practical electrocatalysts for the PEM electrolyzer are provided.

Decoding of Oxygen Network Distortion in a Layered High-Rate Anode by In Situ Investigation of a Single Microelectrode.

Sluggish conversion reactions severely impair the rate capability for lithium storage, which is the main disadvantage of the conversion-type anode materials. Here, the microplatform based on a single microelectrode is designed and utilized for the fundamental understanding of the conversion reaction. The kinetic-favorable layered structure of the anode material is on-site synthesized in the microplatform. The in situ characterization reveals that introducing an oxygen network distortion in the layered oxide anode effectively circumvents the severe passivation of the electrode material by lithium oxide, thus leading to highly reversible conversion reactions. As a result, the high-rate capability of the conversion-type anode materials is realized. The on-site synthesis strategy is further applied in the large-scale synthesis of nanomaterials for lithium-ion batteries. As such, oxide nanorods with the layered structure are synthesized by a facile chemical strategy, showing high rate performance (574 mAh g-1 at 10 A g-1). This work unveils the beneficial effect of oxygen network distortion in the layered anode for conversion reactions over cycling, thus providing an alternative strategy to enhance the rate capability of conversion-type anodes for lithium storage.