Research Progress of TiO2-Based Photocatalytic CO2 Reduction

doi:10.19894/j.issn.1000-0518.230369

Chinese Journal of Applied Chemistry ›› 2024, Vol. 41 ›› Issue (5): 637-658.DOI: 10.19894/j.issn.1000-0518.230369

• Review • Previous Articles

Research Progress of TiO₂-Based Photocatalytic CO₂ Reduction

Bing-Jie WAN¹, Xiao-Xue LIU¹, Lin-Guang QI¹, Chang-Chao JIA¹(), Jian LIU¹^,²()

^1.College of Materials Science and Engineering，Qingdao University of Science and Technology，Qingdao 266042，China
^2.Qingdao Institute of Biomass Energy and Bioprocess Technology，Chinese Academy of Sciences，Key Laboratory of Photoelectric Conversion and Utilization of Solar Energy，Qingdao New Energy Shandong Laboratory，Qingdao 266101，China

Received:2023-11-24 Accepted:2024-03-15 Published:2024-05-01 Online:2024-06-03
Contact: Chang-Chao JIA,Jian LIU
About author:jiachangchao@qust.edu.cn
liujian@qibebt.ac.cn
Supported by:
the Qingdao Natural Science Foundation(23-2-1-250-zyyd-jch);China Postdoctoral Science Foundation(2022M711743);the National Natural Science Foundation of China(22175104);the Natural Science Foundation of Shandong Province(ZR2019ZD47);the Education Department of Shandong Province(2019KJC006)

Abstract

Abstract:

The search for alternatives to fossil fuels has received a great deal of attention based on the urgency of reducing CO₂ levels in the atmosphere and the demand for energy at this stage. Solar energy is the world's most abundant renewable energy source， and photocatalysis is a sunlight-driven chemical reaction process carried out on the surface of the photocatalyst. The realization of the carbon cycle is an urgent need for the development of human society. Photocatalysis has the advantages of low energy consumption and mild reaction conditions， and realizing the resource utilization of CO₂ by simulating natural photosynthesis， which is one of the most promising means to solve this problem， and is of great significance for realizing carbon neutrality. The central issue in the case is the development of efficient， environmentally friendly and inexpensive catalysts. Titanium dioxide （TiO₂） is favored in photocatalysis because of its high catalytic activity and excellent chemical stability. However， some bottlenecks still restrict the photocatalytic activity. Various methods have been tried to optimize the photocatalytic performance. This article summarizes the photocatalytic CO₂ reduction based on TiO₂ photocatalysts in recent years， which helps to comprehensively understand and grasp the research progress and trends in this field. This paper mainly discusses the mechanism of photocatalytic CO₂ reduction， reaction system， and the research progress of TiO₂-based catalysts in photocatalytic CO₂ reduction. The active sites of TiO₂-based photocatalysts are elaborated， focusing on the applications of titanium-oxo clusters， the construction of Lewis acid-base pairs， the establishment of heterojunctions， and the modulation of surface wettability. These strategies can not only increase the effective active sites on the catalyst surface， but also effectively enhance the separation efficiency of electron-hole pairs， so as to improve the photocatalytic CO₂ reduction performance. Finally， the future opportunities and challenges in this field are prospected.

Key words: Titanium dioxide, Photocatalysis, Carbon dioxide reduction, Titanium-oxo cluster, Active site, Wettability

CLC Number:

O643

Bing-Jie WAN, Xiao-Xue LIU, Lin-Guang QI, Chang-Chao JIA, Jian LIU. Research Progress of TiO₂-Based Photocatalytic CO₂ Reduction[J]. Chinese Journal of Applied Chemistry, 2024, 41(5): 637-658.

Figures/Tables 14

Fig.1 Publications （A） and citations （B） of TiO2-based photocatalysts in the field of CO2 reduction during last 10 years （The data are achieved on the search results from the Web of Science 2023.11）

Fig.2 Schematic illustration of photocatalytic CO2 reduction

Fig.3 Schematic diagram of the energy level structure of common semiconductor photocatalysts

Table 1 Reaction potential energy required for CO2 conversion to form different products

Product	Reaction	E/V（vs.NHE）
Hydrogen	2H₂O + 2e^- $→ ?$ 2OH^- + H₂	-0.41
Methane	CO₂ + 8H⁺+ 8e ^- $→ ?$ CH₄ +2H₂O	-0.24
Carbon monoxide	CO₂ + 2H ⁺ + 2e ^- $→ ?$ CO + H₂O	-0.51
Methanol	CO₂ + 6H ⁺ + 6e ^- $→ ?$ CH₃OH + H₂O	-0.38
Formic acid	CO₂ + 2H ⁺ + 2e ^- $→ ?$ HCOOH	-0.61
Methanal	CO₂+ 4H⁺+ 4e ^- $→ ?$ HCHO + H₂O	-0.48
Ethylene	2CO₂ + 12H⁺ + 12e ^- $→ ?$ C₂H₄+4H₂O	-0.34
Ethane	2CO₂ + 14H ⁺ + 14e ^- $→ ?$ C₂H₆ + 4H₂O	-0.27
Ethanol	2CO₂ + 12H⁺ + 12e^- $→ ?$ C₂H₅OH + 3H₂O	-0.33
Oxalate	2CO₂ + 2H ⁺ + 2e ^- $→ ?$ H₂C₂O₄	-0.87

Table 1 Reaction potential energy required for CO2 conversion to form different products

Product	Reaction	E/V（vs.NHE）
Hydrogen	2H₂O + 2e^- $→ ?$ 2OH^- + H₂	-0.41
Methane	CO₂ + 8H⁺+ 8e ^- $→ ?$ CH₄ +2H₂O	-0.24
Carbon monoxide	CO₂ + 2H ⁺ + 2e ^- $→ ?$ CO + H₂O	-0.51
Methanol	CO₂ + 6H ⁺ + 6e ^- $→ ?$ CH₃OH + H₂O	-0.38
Formic acid	CO₂ + 2H ⁺ + 2e ^- $→ ?$ HCOOH	-0.61
Methanal	CO₂+ 4H⁺+ 4e ^- $→ ?$ HCHO + H₂O	-0.48
Ethylene	2CO₂ + 12H⁺ + 12e ^- $→ ?$ C₂H₄+4H₂O	-0.34
Ethane	2CO₂ + 14H ⁺ + 14e ^- $→ ?$ C₂H₆ + 4H₂O	-0.27
Ethanol	2CO₂ + 12H⁺ + 12e^- $→ ?$ C₂H₅OH + 3H₂O	-0.33
Oxalate	2CO₂ + 2H ⁺ + 2e ^- $→ ?$ H₂C₂O₄	-0.87

Fig.4 Schematic diagram of photocatalytic CO2 reduction system in （A） gas-solid system，（B） solid-liquid system and （C） gas-liquid-solid system

Fig.5 （A） Schematic diagram of Pt/o-PCN three-phase photocatalytic system；（B） Photocatalytic activity and selectivity of Pt/o-PCN to carbon products［46］；（C） Schematic diagram of Ag-TiO2 three-phase photocatalytic system supported by gas-liquid-solid interface；（D） CO2 reduction products at Ag-TiO2-GDL［47］；（E） Schematic diagram of an integrated photoenzyme catalytic system with a hydrophilic and hydrophobic layer on the membrane；（F） Schematic diagram of CO2 reduction catalyzed by photoenzyme［52］

Fig.6 （A） Molecular configuration of TiO2；（B） illustration of the pentagonal ｛Ti（Ti5）｝ building units； the Ti—O core structures of （C） PTC-49V and （D） PTC-49H； illustration of the highlighted anatase-type ｛Ti8O14｝ moiety in （E） PTC-49H and （F） anatase TiO2［58］；（G） Molecular structure diagram of Ti42［59］

Fig.7 （A） Structural and polyhedral relationships between PTi16， PTi12 and original heteroatom Keggin structure［60］ and （B） the morphology and molecular structure of Ti6， Ti8-Fcdc and Ti6-Fcdc［62］

Fig.8 （A） Schematic illustration of the classical Lewis acid-base pair；（B） Reactivity of FLPs in single-site Bi3+ substituted Bi x In2–x O3［70］；（C） c-TiO2@a-TiO2-x （OH）y heterogeneous surface FLPs［71］ and （D） the surface of TiO2-x is hindered by Lewis acid-base pairs［72］

Fig.9 Schematic for engineering the electronic band structure of semiconductors［88］

Table 2 Photocatalytic CO2 reduction performance of TiO2 loaded with different metals

Photocatalyst	Reduction system	Light source for photocatalytic reaction	Product	Yield/（μmol·g^-1·h^-1）	Selectivity/%	Year∣Ref.
Cu/3DOM-TiO₂	Gas-solid	300 W Xe lamp with a UV filter （320~780 nm）	CH₄	43.15	83.3	2022∣［35］
Cu/3DOM-TiO₂	Solid-liquid	300 W Xe lamp with a UV filter （320~780 nm）	C₂H₄	6.99	58.4	2022∣［35］
Cu/TiO₂	Gas-solid	300 W Xe lamp UV enhanced	CO	15.27	95.9	2022∣［105］
Cu NCs/TiO₂	Gas-solid	300 W Xe lamp	CO	40.3	93	2022∣［106］
H-TiO₂@Cu	Gas-solid	300 W Xe lamp	CO	23.5	84.5	2021∣［107］
Cu-O/Ti_0.91O₂-SL	Solid-liquid	300 W Xe lamp	CO	61.0	84.4	2023∣［108］
Cu-Ti-OVs/Ti_0.91O₂-SL	Solid-liquid	300 W Xe lamp	C₂H₄ C₃H₈	7.6 13.8	17.8 32.4	2023∣［108］
Au/TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CO	608	99	2022∣［109］
Au-TiO₂-C₃N₄	Gas-solid	300 W Xe lamp， 420 nm cut-off	CH₄	140	--	2018∣［110］
Au-NG-TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CH₄	83.72	--	2022∣［111］
AuCu-TiO_2-x NSs	Gas-solid	300 W Xe lamp	CH₄	22.47	90.55	2021∣［112］
Cu_0.8Au_0.2/TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CH₄ C₂H₄	3578.9 369.8	77.1 11.9	2021∣［113］
Ag/TiO₂	Solid-liquid	300 W Xe lamp	CO	0.58	100	2021∣［114］
Ag-TiO₂-GDL	Gas-liquid-solid	300 W Xe lamp with a UV filter （＜400 nm）	CO CH₄	205.1 100.6	65.4 32.0	2022∣［47］
Ag-TiO₂	Solid-liquid	300 W Xe lamp with a UV filter （＜400 nm）	CO CH₄	23.9 14.5	19.4 11.8	2022∣［47］
1% Pt/TiO₂ nanocrystals	Gas-solid	300 W Xe lamp with a UV filter （320~780 nm）	CH₄	4.6	--	2017∣［115］
Pt-TiO_2-_x	Gas-solid	300 W Xe lamp	CO CH₄	54.2 66.4	--	2019∣［116］
0.4% Pt/Ti³⁺-TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CH₄	80	--	2017∣117］
Pd_0.2Ag_0.04/TiO₂	Gas-solid	300 W Xe lamp with a UV filter （＜400 nm）	CO C₂H₅OH CH₄	17 13 4	--	2017∣［118］
Pd-HPP-TiO₂	Gas-solid	300 W Xe lamp with a UV filter （325~780 nm）	CO CH₄	34 48	-- 59	2022∣［119］
Pd-HCPs-TiO₂	Gas-solid	300 W Xe lamp	CH₄	237.4	99.9	2021∣［120］

Table 2 Photocatalytic CO2 reduction performance of TiO2 loaded with different metals

Photocatalyst	Reduction system	Light source for photocatalytic reaction	Product	Yield/（μmol·g^-1·h^-1）	Selectivity/%	Year∣Ref.
Cu/3DOM-TiO₂	Gas-solid	300 W Xe lamp with a UV filter （320~780 nm）	CH₄	43.15	83.3	2022∣［35］
Cu/3DOM-TiO₂	Solid-liquid	300 W Xe lamp with a UV filter （320~780 nm）	C₂H₄	6.99	58.4	2022∣［35］
Cu/TiO₂	Gas-solid	300 W Xe lamp UV enhanced	CO	15.27	95.9	2022∣［105］
Cu NCs/TiO₂	Gas-solid	300 W Xe lamp	CO	40.3	93	2022∣［106］
H-TiO₂@Cu	Gas-solid	300 W Xe lamp	CO	23.5	84.5	2021∣［107］
Cu-O/Ti_0.91O₂-SL	Solid-liquid	300 W Xe lamp	CO	61.0	84.4	2023∣［108］
Cu-Ti-OVs/Ti_0.91O₂-SL	Solid-liquid	300 W Xe lamp	C₂H₄ C₃H₈	7.6 13.8	17.8 32.4	2023∣［108］
Au/TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CO	608	99	2022∣［109］
Au-TiO₂-C₃N₄	Gas-solid	300 W Xe lamp， 420 nm cut-off	CH₄	140	--	2018∣［110］
Au-NG-TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CH₄	83.72	--	2022∣［111］
AuCu-TiO_2-x NSs	Gas-solid	300 W Xe lamp	CH₄	22.47	90.55	2021∣［112］
Cu_0.8Au_0.2/TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CH₄ C₂H₄	3578.9 369.8	77.1 11.9	2021∣［113］
Ag/TiO₂	Solid-liquid	300 W Xe lamp	CO	0.58	100	2021∣［114］
Ag-TiO₂-GDL	Gas-liquid-solid	300 W Xe lamp with a UV filter （＜400 nm）	CO CH₄	205.1 100.6	65.4 32.0	2022∣［47］
Ag-TiO₂	Solid-liquid	300 W Xe lamp with a UV filter （＜400 nm）	CO CH₄	23.9 14.5	19.4 11.8	2022∣［47］
1% Pt/TiO₂ nanocrystals	Gas-solid	300 W Xe lamp with a UV filter （320~780 nm）	CH₄	4.6	--	2017∣［115］
Pt-TiO_2-_x	Gas-solid	300 W Xe lamp	CO CH₄	54.2 66.4	--	2019∣［116］
0.4% Pt/Ti³⁺-TiO₂	Gas-solid	300 W Xe lamp with an AM 1.5G filter	CH₄	80	--	2017∣117］
Pd_0.2Ag_0.04/TiO₂	Gas-solid	300 W Xe lamp with a UV filter （＜400 nm）	CO C₂H₅OH CH₄	17 13 4	--	2017∣［118］
Pd-HPP-TiO₂	Gas-solid	300 W Xe lamp with a UV filter （325~780 nm）	CO CH₄	34 48	-- 59	2022∣［119］
Pd-HCPs-TiO₂	Gas-solid	300 W Xe lamp	CH₄	237.4	99.9	2021∣［120］

Fig.10 The electronic interactions at a single Cu atom and the surrounding TiO2：（A） Schematic alignments of the d orbital splitting of a metal atom in a coordinate complex；（B） Structure and schematic illustration of the density of states of Cu1/TiO2 and pristine TiO2；（C） DFT energetics of oxygen vacancy formation［124］

Fig.11 Schematic illustration of electron-hole pair separation under different types of heterojunction：（A） Typr-Ⅱ? scheme；（B） Traditional Z-scheme；（C） All-solid state Z-scheme；（D） Direct Z-scheme；（E） S-scheme photoresponse

Fig.12 （A） Schematic diagram of superhydrophobic TiO2 nanowire system and reaction interface microenvironment；（B） Schematic diagram of hydrophobic TiO2 photocatalytic CO2 reduction reaction system and （C） Schematic diagram of CO2 solubility in three-phase and two-phase systems［149］

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Research Progress of TiO₂-Based Photocatalytic CO₂ Reduction

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