Photo-Assisted Catalytic CO2 Hydrogenation to CO with Nearly 100% Selectivity over Rh/TiO2 Catalysts,Energy & Fuels

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Photo-Assisted Catalytic CO2 Hydrogenation to CO with Nearly 100% Selectivity over Rh/TiO2 Catalysts
Energy & Fuels ( IF 5.2 ) Pub Date : 2022-12-16 , DOI: 10.1021/acs.energyfuels.2c03604
Yunxiang Tang ₁ , Simeng Wu ₁ , Yanxiang Wang ₁ , Lixiang Song ₂ , Zhengyi Yang ₁ , Chan Guo ₁ , Jiurong Liu ₁ , Fenglong Wang _{1,

3}

Affiliation

Photo-assisted catalytic CO₂ hydrogenation represents a promising route to convert CO₂ into value-added chemicals under mild conditions, but challenges remain in the design and development of highly active and selective catalysts. Herein, we synthesized highly efficient catalysts comprising Rh nanoparticles supported on TiO₂ nanosheets for photo-assisted catalytic CO₂ hydrogenation, which achieved a high CO production rate of 20.6 mmol g_cat^–1 h^–1 (5.15 mol g_Rh^–1 h^–1) with nearly 100 % selectivity and excellent stability at 250 °C under light irradiation, outperforming most reported metal-based catalysts. X-ray photoelectron spectroscopy revealed that the electrons transfer from Rh nanoparticles to TiO₂, hinting a strong interaction between Rh and the TiO₂ support. Under illumination, the accumulated hot electrons on TiO₂ surfaces could effectively promote the activation of CO₂ molecules. In situ diffuse reflectance infrared Fourier transform spectroscopy results revealed that formate was the critical intermediate in the reverse water–gas shift reaction process, and light irradiation could effectively facilitate the activation and conversion of reactants and intermediate species, thereby improving CO production. This work provides a new strategy for the integration of solar and thermal energy for an efficient RWGS reaction under mild conditions.

中文翻译：

与 Rh/TiO2 催化剂相比，光辅助催化 CO2 加氢制 CO 的选择性接近 100%

光辅助催化 CO _{2加氢是一种在温和条件下将 CO}₂转化为增值化学品的有前途的途径，但在设计和开发高活性和选择性催化剂方面仍然存在挑战。_{在此，我们合成了包含负载在 TiO 2}纳米片上的Rh 纳米颗粒的高效催化剂，用于光辅助催化 CO ₂加氢，实现了 20.6 mmol g _cat^–1 h ^–1（5.15 mol g _Rh^–1 h ^{– 1个}) 在 250 °C 的光照射下具有接近 100% 的选择性和出色的稳定性，优于大多数报道的金属基催化剂。X 射线光电子能谱显示电子从 Rh 纳米粒子转移到 TiO _{2 ，暗示 Rh 和 TiO}₂载体之间存在强烈的相互作用。在光照下，TiO ₂表面积累的热电子可以有效促进CO ₂分子的活化。就地漫反射红外傅里叶变换光谱结果表明，甲酸盐是逆水煤气变换反应过程中的关键中间体，光照射可以有效促进反应物和中间物种的活化和转化，从而提高CO的产量。这项工作为整合太阳能和热能以在温和条件下进行高效的 RWGS 反应提供了一种新策略。

更新日期：2022-12-16

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