Synergistically Mitigating Electron Back-Donation by Single-Atomic Fe–N–C and Alloying to Boost CO-Tolerance of Pt in Hydrogen Oxidation,ACS Catalysis

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Synergistically Mitigating Electron Back-Donation by Single-Atomic Fe–N–C and Alloying to Boost CO-Tolerance of Pt in Hydrogen Oxidation
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-05-25 , DOI: 10.1021/acscatal.3c01466
Zihao Dong _{1,

2} , Yang Nan _{2,

3} , Tang Tang ₁ , Xiao-Zhi Liu ₄ , Jiaju Fu ₁ , Hai-Rui Pan ₁ , Zhe Jiang _{1,

2} , Liang Ding _{1,

2} , Xing Cheng ₁ , Li-Rong Zheng ₅ , Jianan Zhang ₆ , Xiaoxia Chang ₇ , Bingjun Xu ₇ , Jin-Song Hu _{1,

2}

Affiliation

Developing CO-tolerant Pt-based catalysts for the hydrogen oxidation reaction (HOR) is critical for the commercialization of fuel cells and thus receiving increasing interest. Although it is known that weakening the CO adsorption on Pt can improve CO tolerance, efficient strategies are still needed. Inspired by theoretical simulations, we propose here a cascade strategy to synergistically mitigate electron back-donation of Pt 5d → CO 2π* by introducing single-atomic Fe–N–C substrate and alloying, which significantly boosts the CO-tolerance of Pt-based HOR catalysts. The obtained PtNiMo/Fe–N–C can maintain above 80% HOR current density after 2000 s in 1000 ppm CO/H₂, substantially outperforming control catalysts and ranking among the state-of-the-art catalysts. The in situ surface-enhanced infrared adsorption spectroscopy validates that the effectively weakened CO adsorption contributes to improved CO tolerance. This strategy opens up opportunities for designing advanced HOR catalysts with desired CO tolerance.

中文翻译：

单原子 Fe-N-C 和合金化协同减轻电子回馈以提高 Pt 在氢氧化中的 CO 耐受性

开发用于氢氧化反应 (HOR) 的耐 CO 铂基催化剂对于燃料电池的商业化至关重要，因此受到越来越多的关注。尽管众所周知削弱 Pt 上的 CO 吸附可以提高 CO 耐受性，但仍然需要有效的策略。受理论模拟的启发，我们在此提出了一种级联策略，通过引入单原子 Fe-N-C 基底和合金化来协同减轻 Pt 5 d → CO 2 π *的电子回馈，从而显着提高 Pt 的 CO 耐受性基于 HOR 催化剂。所得PtNiMo/Fe-N-C在1000 ppm CO/H _{2中2000 s后仍能保持80%以上的HOR电流密度}，大大优于控制催化剂并跻身最先进的催化剂之列。原位表面增强红外吸收光谱验证了有效减弱的CO吸附有助于提高CO耐受性。该策略为设计具有所需 CO 耐受性的先进 HOR 催化剂提供了机会。

更新日期：2023-05-25

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