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yexuqing木蟲之王 (文學(xué)泰斗)
太陽系系主任
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[交流]
ve thermal expansion and oxygen-redox electrochemistry
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ve thermal expansion and oxygen-redox electrochemistry 負(fù)熱膨脹和氧氧化還原電化學(xué) ▲ 作者：Bao Qiu, Yuhuan Zhou, Haoyan Liang, Minghao Zhang, Kexin Gu, Tao Zeng, Zhou Zhou, Wen Wen, Ping Miao, Lunhua He, Yinguo Xiao, Sven Burke, Zhaoping Liu & Ying Shirley Meng ▲ 鏈接： https://www.nature.com/articles/s41586-025-08765-x ▲ 摘要： 由于材料的熱力學(xué)和電化學(xué)性質(zhì)之間錯綜復(fù)雜的相互作用，材料內(nèi)部的結(jié)構(gòu)紊亂產(chǎn)生了令人著迷的現(xiàn)象。氧氧化還原（OR）電化學(xué)提供了容量限制的突破，同時引起結(jié)構(gòu)紊亂，降低了電化學(xué)可逆性。固體熱膨脹的傳統(tǒng)解釋依賴于格律乃森關(guān)系，將膨脹系數(shù)與晶格的非調(diào)和性聯(lián)系起來。然而，由于這種系統(tǒng)中未探索的動態(tài)無序-有序轉(zhuǎn)變，這種范式可能不適用于OR材料。 研究者發(fā)現(xiàn)，OR活性材料中存在負(fù)熱膨脹，其系數(shù)值為?14.4(2)× 10?6℃?1，這歸因于熱驅(qū)動的無序-有序轉(zhuǎn)變。OR行為的調(diào)制不僅可以精確控制材料的熱膨脹系數(shù)，而且為零熱膨脹功能材料的設(shè)計建立了一個實用的框架。 他們還證明了材料內(nèi)部結(jié)構(gòu)無序的恢復(fù)也可以通過電化學(xué)驅(qū)動力來完成。通過調(diào)整截止電壓，對放電電壓變化的評估表明，幾乎可達100%結(jié)構(gòu)恢復(fù)。 這一發(fā)現(xiàn)為通過操作電化學(xué)過程將OR活性材料恢復(fù)到原始狀態(tài)提供了一條途徑，提出了一種新的緩解策略來解決電壓衰減的持續(xù)挑戰(zhàn)。 ▲ Abstract： Structural disorder within materials gives rise to fascinating phenomena, attributed to the intricate interplay of their thermodynamic and electrochemical properties. Oxygen-redox (OR) electrochemistry offers a breakthrough in capacity limits, while inducing structural disorder with reduced electrochemical reversibility. The conventional explanation for the thermal expansion of solids relies on the Grüneisen relationship, linking the expansion coefficient to the anharmonicity of the crystal lattice6. However, this paradigm may not be applicable to OR materials due to the unexplored dynamic disorder–order transition in such systems. Here we reveal the presence of negative thermal expansion with a large coefficient value of ?14.4(2)?×?10?6°C?1in OR active materials, attributing this to thermally driven disorder–order transitions. The modulation of OR behaviour not only enables precise control over the thermal expansion coefficient of materials, but also establishes a pragmatic framework for the design of functional materials with zero thermal expansion. Furthermore, we demonstrate that the reinstatement of structural disorder within the material can also be accomplished through the electrochemical driving force. By adjusting the cut-off voltages, evaluation of the discharge voltage change indicates a potential for nearly 100% structure recovery. This finding offers a pathway for restoring OR active materials to their pristine state through operando electrochemical processes, presenting a new mitigation strategy to address the persistent challenge of voltage decay. |
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