Enhanced formic acid production for CO<sub>2</sub> photocatalytic reduction over Pd/H-TiO<sub>2</sub> catalyst

doi:10.1007/s11705-024-2485-2

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (11) : 134 https://doi.org/10.1007/s11705-024-2485-2

Enhanced formic acid production for CO₂ photocatalytic reduction over Pd/H-TiO₂ catalyst

Huimin Gao¹, Jinpeng Zhang¹, Fangyuan Zhang¹, Jieying Jing^1,²(

), Wen-Ying Li¹(

)

¹. State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China
². Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan 030000, China

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Abstract

The photocatalytic reduction of CO₂ into formic acid is a feasible approach to alleviate the effects of global climate change and achieve chemical energy storage. It is important to design highly active photocatalysts to improve the selectivity and yield of formic acid. In this study, TiO₂-based catalysts were prepared and loaded with Pd nanoparticles via an impregnation process. The Pd/H-TiO₂ catalyst demonstrated superior CO₂ reduction activity and a high formic acid production rate of 14.14 mmol_cat·g^–1·h^–1. The excellent catalytic performance observed in the presence of a Pd/H-TiO₂ catalyst is ascribed to the synergy between O_v and Pd. The presence of O_v led to increase in CO₂ adsorption while Pd loading enhanced the photogenerated electron-hole pair separation. Electron transfer from H-TiO₂ to Pd also contributed to CO₂ activation.

Keywords CO₂ reduction formic acid photocatalysis TiO₂ catalyst

Corresponding Author(s): Jieying Jing,Wen-Ying Li

Just Accepted Date: 04 June 2024 Issue Date: 08 August 2024

Cite this article:

Wen-Ying Li,Jieying Jing,Fangyuan Zhang, et al. Enhanced formic acid production for CO₂ photocatalytic reduction over Pd/H-TiO₂ catalyst[J]. Front. Chem. Sci. Eng., 2024, 18(11): 134.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2485-2
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I11/134

Fig.1 (a) XRD patterns of TiO₂ at different hydrogenation temperatures and Pd/H-TiO₂, (b) TEM image of catalysts, (c) HRTEM image of Pd/H-TiO₂, (d) EDS elemental mapping of Pd/H-TiO₂.

Fig.2 XPS spectra of (a) Ti 2p, (b) O 1s, (c) Pd 3d, and (d) EPR of TiO₂, H-TiO₂, and Pd/H-TiO₂ obtained at room temperature.

Fig.3 (a) HCOOH production rate within 1 h with different catalysts, (b) cyclic stability of the Pd/H-TiO₂ catalyst.

Fig.4 (a) UV-vis spectra of various photocatalysts, (b) Tauc plots, (c) Mott-Schottky curves at 2000 Hz, (d) band structures.

Model	d( $O C O 2$ - $T i T i O 2$ )/?	d( $C C O 2$ - $O C O 2$ )/?	d( $C C O 2$ - $O T i O 2$ )/?	∠CO₂(O-C-O)/(° )	d(Pd- $C C O 2$ )/?	E_ads/eV
CO₂-TiO₂	2.21/2.21	1.26/1.26	1.42	135.8	–	–0.104
CO₂-H-TiO₂- O_v1	2.23/2.20	1.25/1.26	1.41	134.8	–	–0.357
CO₂-H-TiO₂- O_v2	2.20/2.30	1.26/1.24	1.45	136.9	–	? 0.312
CO₂-H-TiO₂-O_v12^a)	2.21/2.20	1.25/1.26	1.44	136.7	–	? 0.379
CO₂-Pd/TiO₂	–	1.23/1.22	–	145.4	2.05	? 0.412
CO₂-Pd/H-TiO₂-O_v1	–	1.28/1.22	–	134.3	2.04	? 0.885
CO₂-Pd/H-TiO₂-O_v2	–	1.23/1.23	–	145.4	2.01	? 0.600
CO₂-Pd/H-TiO₂-O_v12	–	1.24/1.23	–	143.2	2.01	? 0.114

Tab.1 Adsorption geometry and energy of CO₂ adsorbed on TiO₂ or Pd/H-TiO₂ surface

Fig.5 (a–c) Adsorption configurations of CO₂ with and without O_v and Pd and the charge density difference upon CO₂ adsorption. Yellow and cyan represent electron accumulation and loss, respectively, isosurfaces = 0.0002 e·Bohr^–3.

Fig.6 (a) Transient photocurrent response, (b) PL spectra of TiO₂, H-TiO₂, and Pd/H-TiO₂.

Fig.7 DRIFTS spectra of the Pd/H-TiO₂ catalyst after the photocatalytic reaction.

Fig.8 Mechanism of the photocatalysis of CO₂ to produce HCOOH.

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