Carbonized polymer dots confined active Ru-O sites for boosting electrocatalytic oxygen evolution

IF 8.9 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chinese Chemical Letters Pub Date : 2025-05-29 DOI:10.1016/j.cclet.2025.111393

Da Yue , Tanglue Feng , Zhicheng Zhu , Mingcheng Zhang , Liyuan Chen , Xiao Han , Haizhu Sun , Bai Yang

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Abstract

Designing efficient and stable electrocatalysts for the oxygen evolution reaction (OER) is of paramount importance for many energy-related technologies and devices. Herein, we propose a controlled oxidation pyrolysis strategy to develop carbonized polymer dots (CPDs)-modified Rh-doped RuO₂ electrocatalyst (Rh-RuO₂/CPDs). CPDs act as structure-directing agents, facilitating the formation of small-sized Rh-RuO₂/CPDs nanoparticles and engineering them with abundant defective structures and stable Ru-O sites. The experimental results and theoretical simulation unravel that the modulation effect of CPDs and Rh doping can effectively regulate the electronic structure, valence state and morphology of active Ru-O sites, thereby enhancing the electron transfer at the active site interface and optimizing the chemisorption behavior of oxygen intermediates. The resultant Rh-RuO₂/CPDs demonstrates overpotentials of 168 and 197 mV at 10 mA/cm² for OER in 0.5 mol/L H₂SO₄ and 1.0 mol/L KOH solution, respectively, and long-term catalytic stability.

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碳化聚合物点限制活性Ru-O位点，促进电催化析氧

设计高效、稳定的析氧反应电催化剂对许多能源相关技术和设备至关重要。在此，我们提出了一种可控氧化热解策略来制备碳化聚合物点（CPDs）修饰的掺铑RuO2电催化剂（Rh-RuO2/CPDs）。CPDs作为结构导向剂，促进了小尺寸Rh-RuO2/CPDs纳米颗粒的形成，并使其具有丰富的缺陷结构和稳定的Ru-O位点。实验结果和理论模拟表明，CPDs和Rh掺杂的调制效应可以有效调节活性Ru-O位点的电子结构、价态和形态，从而增强活性位点界面上的电子转移，优化氧中间体的化学吸附行为。在0.5 mol/L H2SO4和1.0 mol/L KOH溶液中，得到的Rh-RuO2/CPDs在10 mA/cm2下的过电位分别为168和197 mV，并具有长期的催化稳定性。

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来源期刊

Chinese Chemical Letters 化学-化学综合

CiteScore

14.10

自引率

15.40%

发文量

8969

审稿时长

1.6 months

期刊介绍： Chinese Chemical Letters (CCL) (ISSN 1001-8417) was founded in July 1990. The journal publishes preliminary accounts in the whole field of chemistry, including inorganic chemistry, organic chemistry, analytical chemistry, physical chemistry, polymer chemistry, applied chemistry, etc.Chinese Chemical Letters does not accept articles previously published or scheduled to be published. To verify originality, your article may be checked by the originality detection service CrossCheck.