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Tuning oxygen vacancy for efficient CO2 electroreduction over CeO2 supported SnO2
Chemical Engineering Science ( IF 4.1 ) Pub Date : 2024-11-13 , DOI: 10.1016/j.ces.2024.120933
Zhanpeng Liang, Hai Liu, Yaxin Jin, Jianlong Lin, Zhihui Liu, Tianxiang Yan, Sheng Zhang

CO2 electroreduction is favorable in neutral or alkaline aqueous solutions, where H2O serves as the proton source, suffering from sluggish dynamics. Herein, we synthesize a series of SnO2-CeO2 with different oxygen vacancy (Ov) concentration, regulating the H2O dissociation, to synchronize with the CO2 reduction. The optimal SnO2-CeO2 catalyst, with a moderate Ov concentration, exhibits a formate Faradic efficiency of nearly 93 % and maintains for more than 46 h at a current density of 100 mA/cm2. The catalyst with lower Ov concentration results in weak H2O dissociation, thus enhancing the energy barrier of *OCHO generation, while higher Ov concentration leads to excessive proton, exacerbating the hydrogen evolution reaction (HER), as supported by DFT calculation and in situ attenuated total reflection-Fourier transform infrared spectra (ATR-FTIR). This study underscores the significance of Ov concentration in determining the ability of water dissociation over supported electrocatalysts, providing valuable insights for the development of more efficient electrocatalyst.

中文翻译:


调整氧空位以实现对 CeO2 负载的 SnO 2 的高效 CO2 电还原



CO2 电还原在中性或碱性水溶液中是有利的,其中 H2O 作为质子源,动力学缓慢。在此,我们合成了一系列具有不同氧空位 (Ov) 浓度的 SnO2-CeO 2,调节 H2O 解离,以同步 CO2 还原。最佳的 SnO2-CeO 2 催化剂,具有中等 Ov 浓度,表现出近 93 % 的甲酸盐法拉第效率,并在 100 mA/cm2 的电流密度下保持 46 小时以上。Ov 浓度较低的催化剂导致弱 H2O 解离,从而增强 *OCHO 生成的能量势垒,而较高的 Ov 浓度导致质子过多,加剧析氢反应 (HER),正如 DFT 计算和原位衰减全反射傅里叶变换红外光谱 (ATR-FTIR) 所支持的那样。本研究强调了 Ov 浓度在确定负载型电催化剂上水解离能力的重要性,为开发更高效的电催化剂提供了有价值的见解。
更新日期:2024-11-13
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