Crystal facet evolution of spinel Co3O4 nanosheets in acidic oxygen evolution catalysis,Catalysis Science & Technology

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Crystal facet evolution of spinel Co3O4 nanosheets in acidic oxygen evolution catalysis
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2023-06-29 , DOI: 10.1039/d3cy00713h
Ziyang Sheng ₁ , Sihong Wang ₁ , Qu Jiang ₁ , Yuanman Ni ₁ , Chaoran Zhang ₁ , Ashfaq Ahmad ₁ , Fang Song ₁

Affiliation

Few earth-abundant catalysts can catalyze the oxygen evolution reaction (OER) in acid with satisfactory durability, due to the significant dissolution of transition metals. Disclosing the deactivation mechanism is the prerequisite for the rational design of durable OER electrocatalysts. Here, we establish the link between catalytic deactivation and the crystal facet's evolution of an archetypical acidic OER catalyst of spinel Co₃O₄, by correlating electrochemical response with facet evolution during electrolysis. We establish a complete picture of the crystal facet's evolution throughout the whole course. Low-index crystal facets of {110}, {100}, and {211} are prone to dissolve, whereas the high-index ones including {311} and {402} emerge along with the concurrent transition of the catalytic mechanism. Combining electrochemical analysis, facet probing, and theoretical calculation, we unveil that the etching of the most unstable {110} facets (only medium active) significantly accelerates the dissolution of the most active {100} facets and the most durable {111} facets adjacent to them. Our discovery highlights the destructive effect of unstable facets with only moderate activity, which has always been overlooked before. Additionally, the decoupling of the most active facets from the most stable ones suggests that the activity–durability tradeoff could be addressed by facet engineering.

中文翻译：

酸性析氧催化中尖晶石 Co3O4 纳米片的晶面演化

由于过渡金属的显着溶解，很少有地球丰富的催化剂能够在酸中催化析氧反应（OER）并具有令人满意的耐久性。揭示失活机制是合理设计耐用OER电催化剂的前提。_{在这里，我们建立了尖晶石 Co 3} O ₄典型酸性 OER 催化剂的催化失活和晶面演化之间的联系，通过将电化学响应与电解过程中的晶面演化相关联。我们建立了整个过程中晶面演化的完整图景。{110}、{100}和{211}等低折射率晶面容易溶解，而包括{311}和{402}在内的高折射率晶面则随着催化机制的同时转变而出现。结合电化学分析、刻面探测和理论计算，我们发现最不稳定的{110}面（仅中等活性）的蚀刻显着加速了最活跃的{100}面和邻近的最耐用的{111}面的溶解给他们。我们的发现强调了仅具有中等活动的不稳定面的破坏性影响，这在以前一直被忽视。此外，

更新日期：2023-06-29

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