1. Enhanced Electrochemical CO2 Reduction to Formate over Phosphate‐Modified In: Water Activation and Active Site Tuning.
- Author
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Wei, Zhiming, Ding, Jie, Wang, Ziyi, Wang, Anyang, Zhang, Li, Liu, Yuhang, Guo, Yuzheng, Yang, Xuan, Zhai, Yueming, and Liu, Bin
- Subjects
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ELECTROLYTIC reduction , *ATTENUATED total reflectance , *HYDROGEN evolution reactions , *INFRARED absorption , *DENSITY functional theory , *INFRARED spectroscopy - Abstract
Electrochemical CO2 reduction reaction (CO2RR) offers a sustainable strategy for producing fuels and chemicals. However, it suffers from sluggish CO2 activation and slow water dissociation. In this work, we construct a (P−O)δ− modified In catalyst that exhibits high activity and selectivity in electrochemical CO2 reduction to formate. A combination of in situ characterizations and kinetic analyses indicate that (P−O)δ− has a strong interaction with K+(H2O)n, which effectively accelerates water dissociation to provide protons. In situ attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) measurements together with density functional theory (DFT) calculations disclose that (P−O)δ− modification leads to a higher valence state of In active site, thus promoting CO2 activation and HCOO* formation, while inhibiting competitive hydrogen evolution reaction (HER). As a result, the (P−O)δ− modified oxide‐derived In catalyst exhibits excellent formate selectivity across a broad potential window with a formate Faradaic efficiency as high as 92.1 % at a partial current density of ~200 mA cm−2 and a cathodic potential of −1.2 V vs. RHE in an alkaline electrolyte. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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