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Atomically Dispersed Ru-doped Ti4O7 Electrocatalysts for Chlorine Evolution Reaction with a Universal Activity
Small ( IF 13.3 ) Pub Date : 2024-04-19 , DOI: 10.1002/smll.202401248
Woonghee Lee 1, 2 , Seokhyun Choung 3 , Seok Kim 2, 4 , Jiyun Hong 5 , Doyeon Kim 2 , William A. Tarpeh 1 , Jeong Woo Han 3 , Kangwoo Cho 2, 6
Affiliation  

Chlorine has been supplied by the chlor-alkali process that deploys dimensionally stable anodes (DSAs) for the electrochemical chlorine evolution reaction (ClER). The paramount bottlenecks have been ascribed to an intensive usage of precious elements and inevitable competition with the oxygen evolution reaction. Herein, a unique case of Ru2+-O4 active motifs anchored on Magnéli Ti4O7 (Ru-Ti4O7) via a straightforward wet impregnation and mild annealing is reported. The Ru-Ti4O7 performs radically active ClER with minimal deployment of Ru (0.13 wt%), both in 5 m NaCl (pH 2.3) and 0.1 m NaCl (pH 6.5) electrolytes. Scanning electrochemical microscopy demonstrates superior ClER selectivity on Ru-Ti4O7 compared to the DSA. Operando X-ray absorption spectroscopy and density functional theory calculations reveal a universally active ClER (over a wide range of pH and [Cl]), through a direct adsorption of Cl on Ru2+-O4 sites as the most plausible pathway, together with stabilized ClO* at low [Cl] and high pH.

中文翻译:

原子分散的钌掺杂 Ti4O7 电催化剂用于具有通用活性的氯析出反应

氯是通过氯碱工艺提供的,该工艺为电化学析氯反应 (ClER) 使用尺寸稳定的阳极 (DSA)。最重要的瓶颈归因于贵重元素的密集使用以及不可避免的与析氧反应的竞争。在此,报道了通过简单的湿浸渍和温和退火将Ru 2+ -O 4活性基序锚定在Magnéli Ti 4 O 7 (Ru-Ti 4 O 7 )上的独特案例。 Ru-Ti 4 O 7在 5 m NaCl (pH 2.3) 和 0.1 m NaCl (pH 6.5) 电解质中以最少的 Ru (0.13 wt%) 部署执行自由基活性 ClER 。扫描电化学显微镜显示与 DSA 相比, Ru-Ti 4 O 7具有优异的 ClER 选择性。 Operando X 射线吸收光谱和密度泛函理论计算揭示了普遍活跃的 ClER(在广泛的 pH 和 [Cl - ] 范围内),通过将 Cl -直接吸附在 Ru 2+ -O 4位点上作为最可能的途径,以及在低 [Cl - ] 和高 pH 条件下稳定的 ClO*。
更新日期:2024-04-19
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