改变掺杂 B 的铁铜双原子催化剂的氧气吸附模型,实现高效氧气还原

IF 3.8 3区 化学 Q2 CHEMISTRY, PHYSICAL ChemCatChem Pub Date : 2024-09-04 DOI:10.1002/cctc.202401272
Jianglong Guo, Qizheng An, Xu Zhang, Yuhao Zhang, Jingjing Jiang, Jing Zhang, Baojie Li, Xupeng Qin, Wei Wang, Qinghua Liu
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引用次数: 0

摘要

由于单原子催化剂(SAC)的活性位点孤立,在涉及多个中间体和反应途径的催化反应过程(如氧还原反应(ORR))中,SAC 的催化动力学往往不能令人满意。为了解决这一瓶颈并提高 SAC 的 ORR 性能,我们开发了一种掺硼的铁铜双原子催化剂(Fe-Cu-B/NC)。这种催化剂旨在调节氧吸附模型,并调整氧中间产物在金属位点的吸附强度。原位同步辐射红外光谱显示,Fe-Cu-B/NC 催化剂通过桥式吸附模式促进了氧中间体在 Fe-Cu 双位点上的吸附,从而更有利于 O-O 键的裂解。同时,原位电化学阻抗谱显示,吸附模式的转变可以加速中间产物的动力学过程,进一步提高催化效率。因此,Fe-Cu-B/NC 表现出良好的 ORR 活性和较强的耐久性,在碱性介质中进行 ORR 过程 10 小时后,其初始电流密度仍能保持 90%。
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Altering Oxygen Adsorption Model on B‐Doped Fe‐Cu Dual‐Atom Catalysts for Efficient Oxygen Reduction
Due to isolated active sites of single‐atom catalysts (SACs), the catalytic kinetics of SACs are often unsatisfactory in those catalytic reaction processes involving multiple intermediates and reaction pathways, such as the oxygen reduction reaction (ORR). To address this bottleneck and enhance the ORR performance of SACs, we developed a boron‐doped Fe‒Cu dual‐atom catalyst (Fe‒Cu‒B/NC). This catalyst is designed to modulate the oxygen adsorption model and adjust the adsorption strength of oxygen intermediates at the metal sites. In situ synchrotron infrared spectroscopy demonstrated that the Fe‒Cu‒B/NC catalyst facilitates the adsorption of oxygen intermediates on the Fe‒Cu dual sites through a bridge adsorption model, which is more favorable for O–O bond cleavage. Meanwhile, in situ electrochemical impedance spectroscopy revealed that the transformation of the adsorption model can accelerate the kinetics of intermediate species, further enhancing the catalytic efficiency. As a result, Fe‒Cu‒B/NC exhibits good ORR activity and strong durability, retaining 90% of its initial current density after 10 hours of the ORR process in alkaline media.
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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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