当前位置: X-MOL 学术Nat. Commun. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Introducing Brønsted acid sites to accelerate the bridging-oxygen-assisted deprotonation in acidic water oxidation
Nature Communications ( IF 14.7 ) Pub Date : 2022-08-18 , DOI: 10.1038/s41467-022-32581-w
Yunzhou Wen 1 , Cheng Liu 2 , Rui Huang 1 , Hui Zhang 3 , Xiaobao Li 3 , F Pelayo García de Arquer 4 , Zhi Liu 3, 5 , Youyong Li 2 , Bo Zhang 1
Affiliation  

Oxygen evolution reaction (OER) consists of four sequential proton-coupled electron transfer steps, which suffer from sluggish kinetics even on state-of-the-art ruthenium dioxide (RuO2) catalysts. Understanding and controlling the proton transfer process could be an effective strategy to improve OER performances. Herein, we present a strategy to accelerate the deprotonation of OER intermediates by introducing strong Brønsted acid sites (e.g. tungsten oxides, WOx) into the RuO2. The Ru-W binary oxide is reported as a stable and active iridium-free acidic OER catalyst that exhibits a low overpotential (235 mV at 10 mA cm−2) and low degradation rate (0.014 mV h−1) over a 550-hour stability test. Electrochemical studies, in-situ near-ambient pressure X-ray photoelectron spectroscopy and density functional theory show that the W-O-Ru Brønsted acid sites are instrumental to facilitate proton transfer from the oxo-intermediate to the neighboring bridging oxygen sites, thus accelerating bridging-oxygen-assisted deprotonation OER steps in acidic electrolytes. The universality of the strategy is demonstrated for other Ru-M binary metal oxides (M = Cr, Mo, Nb, Ta, and Ti).



中文翻译:

引入布朗斯台德酸位点加速酸性水氧化中的桥氧辅助去质子化

析氧反应 (OER) 由四个连续的质子耦合电子转移步骤组成,即使在最先进的二氧化钌 (RuO 2 ) 催化剂上,其动力学也很缓慢。了解和控制质子转移过程可能是提高 OER 性能的有效策略。在此,我们提出了一种通过在RuO 2中引入强布朗斯台德酸位点(例如氧化钨,WO x )来加速OER 中间体去质子化的策略。据报道,Ru-W 二元氧化物是一种稳定且活性的无铱酸性 OER 催化剂,具有低过电势(10 mA cm -2时为 235 mV )和低降解速率(0.014 mV h -1) 超过 550 小时的稳定性测试。电化学研究、原位近环境压力 X 射线光电子能谱和密度泛函理论表明,WO-Ru Brønsted 酸位有助于促进质子从含氧中间体转移到相邻的桥接氧位点,从而加速桥接-酸性电解质中的氧辅助去质子化 OER 步骤。其他 Ru-M 二元金属氧化物(M = Cr、Mo、Nb、Ta 和 Ti)证明了该策略的普遍性。

更新日期:2022-08-19
down
wechat
bug