Dissolution-redeposition dynamics as a universal restructuring mechanism of electrocatalysts.

Blaž Tomc, Milutin Smiljanić, Mitja Kostelec, Mejrema Nuhanović, Muhammad Zahid, Leonard Moriau, Ana Rebeka Kamšek, Aleš Marsel, Miha Hotko, Nik Maselj, Ante Matošin, Ana Herceg, Lazar Bijelić, Ožbej Vodeb, Anja Logar, Madis Lüsi, Jan Ocepek, Angelja Kjara Surca, Črtomir Donik, Irena Paulin, Matjaž Godec, Luka Suhadolnik, Francisco Ruiz-Zepeda, Primož Jovanovič, Martin Šala, Marjan Bele, Nejc Hodnik
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Abstract

Electrocatalysts are often assumed to be structurally stable; yet in practice, they continuously dissolve and restructure, directly affecting the number and nature of active sites and therefore performance. Although dissolution-redeposition-driven evolution is well recognized in some electrocatalysis communities, others still interpret activity and selectivity as properties of static surfaces. We argue that across electrocatalytic technologies, especially under demanding industrially relevant timescales, "static" electrocatalysts are a myth: even parts-per-billion metal fluxes can cumulatively change surface structure, poison membranes, degrade supports, and thus shift device performance. Controlling these changes requires a mechanistic understanding of when dissolution, transport, and redeposition are promoted or suppressed by, for instance, potential, pH, reactants, or local microenvironments. Here, we unify evidence for restructuring across metal and metal-derived catalysts under various electrochemical reactions, highlight common driving forces, and summarize the appropriate tools to quantify it. Ultimately, electrocatalysts should be evaluated, designed, and interpreted as dynamically stable materials and not as static electrochemical interfaces.

溶解-再沉积动力学是电催化剂的普遍重组机制。
电催化剂通常被认为结构稳定;然而在实践中,它们不断地溶解和重组,直接影响活性位点的数量和性质,从而影响性能。虽然溶解-重定位驱动的进化在一些电催化群落中得到了很好的认可,但其他人仍然将活性和选择性解释为静态表面的性质。我们认为,在电催化技术中,特别是在苛刻的工业相关时间尺度下,“静态”电催化剂是一个神话:即使是十亿分之一的金属通量也可以累积改变表面结构,毒性膜,降解支撑,从而改变设备性能。控制这些变化需要了解溶解、转运和再沉积何时受到电位、pH、反应物或局部微环境等因素的促进或抑制。在这里,我们统一了各种电化学反应下金属和金属衍生催化剂重组的证据,突出了共同的驱动力,并总结了量化它的适当工具。最终,电催化剂应该被评价、设计和解释为动态稳定的材料,而不是静态的电化学界面。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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