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在铂周围构建一氧化碳免疫水解离位点以在高一氧化碳浓度环境中实现稳定运行。

Constructing CO-immune water dissociation sites around Pt to achieve stable operation in high CO concentration environment.

作者信息

Long Daojun, Liu Yongduo, Ping Xinyu, Chen Fadong, Tao Xiongxin, Xie Zhenyang, Wang Minjian, Wang Meng, Li Li, Guo Lin, Chen Siguo, Wei Zidong

机构信息

College of Chemistry and Chemical Engineering, State Key Laboratory of Advanced Chemical Power Sources (SKL-ACPS), Chongqing University, Chongqing, China.

Research Institute of Petroleum Processing Co., Ltd., SINOPEC, Beijing, China.

出版信息

Nat Commun. 2024 Sep 16;15(1):8105. doi: 10.1038/s41467-024-51562-9.

DOI:10.1038/s41467-024-51562-9
PMID:39285182
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11405863/
Abstract

The serious problem of carbon monoxide (CO) poisoning on the surface of Pt-based catalysts has long constrained the commercialization of proton exchange membrane fuel cells (PEMFCs). Regeneration of Pt sites by maintaining CO scavenging ability through precise construction of the surface and interface structure of the catalyst is the key to obtaining high-performance CO-resistant catalysts. Here, we used molybdenum carbide (MoC) as the support for Pt and introduced Ru single atoms (SA-Ru) at the Pt-MoC interface to jointly decrease the CO adsorption strength on Pt. More importantly, the MoC and SA-Ru are immune to CO poisoning, which continuously assists in the oxidation of adsorbed CO by generating oxygen species from water dissociation. These two effects combine to confer this anode catalyst (SA-Ru@Pt/MoC) remarkable CO tolerance and the ability to operate stably in fuel cell with high CO concentration (power output 85.5 mW cm@20,000 ppm CO + H - O), making it possible to directly use the cheap reformed hydrogen as the fuel for PEMFCs.

摘要

长期以来,铂基催化剂表面一氧化碳(CO)中毒这一严重问题一直制约着质子交换膜燃料电池(PEMFC)的商业化。通过精确构建催化剂的表面和界面结构来维持CO清除能力,从而实现铂位点的再生,是获得高性能抗CO催化剂的关键。在此,我们使用碳化钼(MoC)作为铂的载体,并在Pt-MoC界面引入钌单原子(SA-Ru),以共同降低CO在铂上的吸附强度。更重要的是,MoC和SA-Ru对CO中毒免疫,它们通过水离解产生氧物种,持续协助吸附的CO氧化。这两种效应相结合,赋予了这种阳极催化剂(SA-Ru@Pt/MoC)卓越的CO耐受性以及在高CO浓度(20,000 ppm CO + H₂O时功率输出85.5 mW cm⁻²)的燃料电池中稳定运行的能力,使得直接使用廉价的重整氢气作为PEMFC的燃料成为可能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/659248dba48f/41467_2024_51562_Fig7_HTML.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/659248dba48f/41467_2024_51562_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/502037f3c18d/41467_2024_51562_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/c4708f993119/41467_2024_51562_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/db1eaa94be2b/41467_2024_51562_Fig3_HTML.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/e0a587048299/41467_2024_51562_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/b637d3987357/41467_2024_51562_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58e9/11405863/659248dba48f/41467_2024_51562_Fig7_HTML.jpg

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本文引用的文献

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Electron Localization in Rationally Designed PtPd Single-Atom Alloy Catalyst Enables High-Performance Li-O Batteries.合理设计的PtPd单原子合金催化剂中的电子定位实现高性能锂氧电池
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Kinetically matched C-N coupling toward efficient urea electrosynthesis enabled on copper single-atom alloy.
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Unconventional Bilateral Compressive Strained Ni-Ir Interface Synergistically Accelerates Alkaline Hydrogen Oxidation.非传统的双边压缩应变 Ni-Ir 界面协同加速碱性氢氧化。
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