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Oxygen-Bridged Long-Range Dual Sites Boost Ethanol Electrooxidation by Facilitating C–C Bond Cleavage
Nano Letters ( IF 9.6 ) Pub Date : 2023-08-25 , DOI: 10.1021/acs.nanolett.3c02319
Yao Wang 1 , Meng Zheng 2 , Yunrui Li 3 , Juan Chen 4 , Jinyu Ye 5 , Chenliang Ye 2 , Shuna Li 4 , Jin Wang 2 , Yongfa Zhu 6, 7 , Shi-Gang Sun 5 , Dingsheng Wang 7
Nano Letters ( IF 9.6 ) Pub Date : 2023-08-25 , DOI: 10.1021/acs.nanolett.3c02319
Yao Wang 1 , Meng Zheng 2 , Yunrui Li 3 , Juan Chen 4 , Jinyu Ye 5 , Chenliang Ye 2 , Shuna Li 4 , Jin Wang 2 , Yongfa Zhu 6, 7 , Shi-Gang Sun 5 , Dingsheng Wang 7
Affiliation
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Optimizing the interatomic distance of dual sites to realize C–C bond breaking of ethanol is critical for the commercialization of direct ethanol fuel cells. Herein, the concept of holding long-range dual sites is proposed to weaken the reaction barrier of C–C cleavage during the ethanol oxidation reaction (EOR). The obtained long-range Rh–O–Pt dual sites achieve a high current density of 7.43 mA/cm2 toward EOR, which is 13.3 times that of Pt/C, as well as remarkable stability. Electrochemical in situ Fourier transform infrared spectroscopy indicates that long-range Rh–O–Pt dual sites can increase the selectivity of C1 products and suppress the generation of a CO intermediate. Theoretical calculations further disclose that redistribution of the surface-localized electron around Rh–O–Pt can promote direct oxidation of −OH, accelerating C–C bond cleavage. This work provides a promising strategy for designing oxygen-bridged long-range dual sites to tune the activity and selectivity of complicated catalytic reactions.
中文翻译：
氧桥长程双位点通过促进 C-C 键断裂促进乙醇电氧化
优化双位点原子间距离以实现乙醇C-C键断裂对于直接乙醇燃料电池的商业化至关重要。在此，提出了持有长程双位点的概念，以削弱乙醇氧化反应（EOR）过程中C-C裂解的反应势垒。所获得的长程Rh-O-Pt双位点在EOR方面实现了7.43 mA/cm 2的高电流密度，是Pt/C的13.3倍，并且具有出色的稳定性。电化学原位傅里叶变换红外光谱表明，长程Rh-O-Pt双位点可以提高C1产物的选择性并抑制CO中间体的生成。理论计算进一步表明，Rh-O-Pt周围表面局域电子的重新分布可以促进-OH的直接氧化，加速C-C键断裂。这项工作为设计氧桥长程双位点以调节复杂催化反应的活性和选择性提供了一种有前途的策略。
更新日期：2023-08-25
中文翻译：
氧桥长程双位点通过促进 C-C 键断裂促进乙醇电氧化
优化双位点原子间距离以实现乙醇C-C键断裂对于直接乙醇燃料电池的商业化至关重要。在此，提出了持有长程双位点的概念，以削弱乙醇氧化反应（EOR）过程中C-C裂解的反应势垒。所获得的长程Rh-O-Pt双位点在EOR方面实现了7.43 mA/cm 2的高电流密度，是Pt/C的13.3倍，并且具有出色的稳定性。电化学原位傅里叶变换红外光谱表明，长程Rh-O-Pt双位点可以提高C1产物的选择性并抑制CO中间体的生成。理论计算进一步表明，Rh-O-Pt周围表面局域电子的重新分布可以促进-OH的直接氧化，加速C-C键断裂。这项工作为设计氧桥长程双位点以调节复杂催化反应的活性和选择性提供了一种有前途的策略。
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