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yexuqing木蟲之王 (文學泰斗)
太陽系系主任
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[交流]
液電池TEM中帶電固液界面的原子動力學
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液電池TEM中帶電固液界面的原子動力學 ▲ 作者：Qiubo Zhang, Zhigang Song, Xianhu Sun, Yang Liu, Jiawei Wan, Sophia B. Betzler, Qi Zheng, Junyi Shangguan, Karen C. Bustillo, Peter Ercius, Prineha Na ▲ 鏈接： https://www.nature.com/articles/s41586-024-07479-w ▲ 摘要： 帶電固液界面在與能源、生物和地球化學相關(guān)的各種電化學過程中起著關(guān)鍵作用。帶電界面上的電子和質(zhì)量傳遞可能導致結(jié)構(gòu)改變，從而顯著影響反應途徑。例如，電催化劑在反應過程中的表面重組會對催化機理和反應產(chǎn)物產(chǎn)生實質(zhì)性的影響。 盡管它很重要，但直接探測電偏置下固液界面的原子動力學是具有挑戰(zhàn)性的，因為它被埋在液體電解質(zhì)中，而且目前通過液體進行原位成像的技術(shù)空間分辨率有限。研究者開發(fā)了用于透射電子顯微鏡（TEM）的先進聚合物電化學液體電池，能夠直接監(jiān)測銅催化二氧化碳電還原反應（CO2ERs）過程中ESLIs的原子動力學。 研究者觀察揭示了一個波動的液體狀無定形界面。它發(fā)生可逆的晶—非晶結(jié)構(gòu)轉(zhuǎn)變，并沿通電銅表面流動，從而通過界面層介導結(jié)晶銅表面重構(gòu)和質(zhì)量損失。實時觀察和理論計算的結(jié)合揭示了由電荷激活的電解質(zhì)表面反應引起的非晶化介導的重組機制。通過利用原位成像能力，該的結(jié)果為探索原子動力學及其在涉及ESLIs的廣泛系統(tǒng)中的影響提供了許多機會。 ▲ Abstract： Electrified solid–liquid interfaces (ESLIs) play a key role in various electrochemical processes relevant to energy, biology and geochemistry. The electron and mass transport at the electrified interfaces may result in structural modifications that markedly influence the reaction pathways. For example, electrocatalyst surface restructuring during reactions can substantially affect the catalysis mechanisms and reaction products. Despite its importance, direct probing the atomic dynamics of solid–liquid interfaces under electric biasing is challenging owing to the nature of being buried in liquid electrolytes and the limited spatial resolution of current techniques for in situ imaging through liquids. Here, with our development of advanced polymer electrochemical liquid cells for transmission electron microscopy (TEM), we are able to directly monitor the atomic dynamics of ESLIs during copper (Cu)-catalysed CO2 electroreduction reactions (CO2ERs). Our observation reveals a fluctuating liquid-like amorphous interphase. It undergoes reversible crystalline–amorphous structural transformations and flows along the electrified Cu surface, thus mediating the crystalline Cu surface restructuring and mass loss through the interphase layer. The combination of real-time observation and theoretical calculations unveils an amorphization-mediated restructuring mechanism resulting from charge-activated surface reactions with the electrolyte. Our results open many opportunities to explore the atomic dynamics and its impact in broad systems involving ESLIs by taking advantage of the in situ imaging capability. |
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