二氧化钛基光催化剂用于二氧化碳还原和太阳燃料的生产

doi:10.1016/S1872-2067(21)64045-7

催化学报 ›› 2022, Vol. 43 ›› Issue (10): 2500-2529.DOI: 10.1016/S1872-2067(21)64045-7

二氧化钛基光催化剂用于二氧化碳还原和太阳燃料的生产

张涛^a^,^†, 韩晓驰^a^,^†, Nhat Truong Nguyen^b, 杨磊^a, 周雪梅^a^,^*()

^a四川大学化学工程学院, 四川成都 610065, 中国
^b加拿大康考迪亚大学, 吉娜科迪工程和计算机科学学院, 化学与材料工程系, 蒙特利尔, 加拿大

收稿日期:2022-01-10 接受日期:2022-03-03 出版日期:2022-10-18 发布日期:2022-09-30
通讯作者: 周雪梅
作者简介:^†共同第一作者.
基金资助:
国家自然科学基金(22108179)

TiO₂-based photocatalysts for CO₂ reduction and solar fuel generation

Tao Zhang^a^,^†, Xiaochi Han^a^,^†, Nhat Truong Nguyen^b, Lei Yang^a, Xuemei Zhou^a^,^*()

^aSchool of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan, China
^bDepartment of Chemical and Materials Engineering, Gina Cody School of Engineering and Computer Science, Concordia University, Montreal, QC H3G 2W1, Canada

Received:2022-01-10 Accepted:2022-03-03 Online:2022-10-18 Published:2022-09-30
Contact: Xuemei Zhou
About author:^†Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22108179)

摘要/Abstract

摘要：

化石燃料的过度开发和利用加剧了大气中二氧化碳的排放, 是导致全球气候变化严重和生态碳平衡破坏的因素之一. 利用可持续太阳能驱动的光催化技术可以将二氧化碳转化为一系列高附加值化学品, 如甲烷、甲酸、甲醛和甲醇等燃料, 因此被认为是解决能源危机和全球变暖的有效途径之一. 迄今为止, 在被开发利用的光催化剂中, 二氧化钛作为一种经济廉价、无毒、稳定和可持续的金属氧化物, 是多相光催化二氧化碳还原体系的研究重点.

本文重点综述了二氧化钛光催化剂在二氧化碳还原领域的最新研究进展, 阐述了其改性策略, 包括异质结的制备、表面功能修饰、能带结构调节和形貌设计等, 目的在于提高二氧化碳还原产物的选择性和转化率. 对二氧化钛在液相光电催化和气相光热催化二氧化碳还原的基本原理进行总结. 对三种二氧化碳还原反应体系进行讨论, 其主要内容包括: (1)阐述光催化、光电催化以及光热催化还原二氧化碳的热力学和动力学基本原理; (2)针对不同体系, 分析提高二氧化钛催化活性和还原产物选择性的方法, 包括表面改性、贵金属沉积和阴/阳离子掺杂; (3)探究密度泛函理论在二氧化碳还原中的应用, 包括但不限于二氧化碳还原的路径调控、关键中间体的吸附构型和和自由能的计算; (4)总结利用二氧化钛催化二氧化碳还原的不同方法的差异, 并分析其发展前景和挑战. 综上, 本文系统综述了二氧化钛在还原二氧化碳的相关工作, 详细分析了在光催化、光电催化和光热催化体系中二氧化碳还原的反应机制和反应原理, 为二氧化碳的催化转化和二氧化钛基光催化剂合理设计提供了参考.

关键词: 二氧化钛, 多相催化, 二氧化碳还原, 太阳燃料

Abstract:

Solar-driven CO₂ reduction is an efficient way to convert sustainable solar energy and massive CO₂ to renewable solar fuels, such as CH₄, HCOOH, HCHO, and CH₃OH, etc. Up to now, significant research efforts have been devoted to exploring the reaction path and developing the photocatalysts. In heterogeneous photocatalysis, among the semiconductor-based photocatalysts, titania (TiO₂), as an inexpensive and practically sustainable metal oxides, remains the most extensively studied photocatalyst over the past decades. In this review, we summarize the most recent advances in the solar-driven CO₂ reduction using TiO₂-based photocatalysts, which include the fabrication of heterojunction, surface functional modification, band structure engineering, and morphology design, aiming to improve the CO₂ conversion efficiency and selectivity to the desired product. Additionally, photoelectrochemical and photothermal approaches are introduced and the fundamental principles to activate and enhance the performance of TiO₂ for the specific reaction are discussed. The exploration of the solar-driven approaches and discussion on the underlying mechanism allow the comprehensive understanding of CO₂ photoreduction, that can lead to a rational design and synthesis of TiO₂-based photocatalysts.

Key words: TiO₂, Heterogeneous catalysis, CO₂ reduction, Solar fuel

张涛, 韩晓驰, Nhat Truong Nguyen, 杨磊, 周雪梅. 二氧化钛基光催化剂用于二氧化碳还原和太阳燃料的生产[J]. 催化学报, 2022, 43(10): 2500-2529.

Tao Zhang, Xiaochi Han, Nhat Truong Nguyen, Lei Yang, Xuemei Zhou. TiO₂-based photocatalysts for CO₂ reduction and solar fuel generation[J]. Chinese Journal of Catalysis, 2022, 43(10): 2500-2529.

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图/表 41

Fig. 1. The global change of temperature and CO2 concentration in the atmosphere in the 19th century (grey curve). The red bars and blue bars indicate the temperature above and below the average temperature, respectively. Original graph by Dr. Howard Diamond (NOAA ARL), and re-drawn from NOAA Climate.gov [12].

Fig. 2. The Latimer-Frost diagram for CO2 reduction in a homogeneous neutral aqueous solution via multiple electron and proton reaction paths: (a) C1 products; (b) C2+ products. Re-draw from data in references [9,30,31].

Fig. 3. The advantages of TiO2 photocatalyst in CO2 conversion reactions.

Fig. 4. Illustrations of the applications of TiO2 in photocatalysis, photoelectrochemical reactions, and the photothermal catalysis, and the corresponding strategies to improve the conversion efficiency.

Fig. 5. The reduction of carbon dioxide via photocatalysis. Several paths are included in the reaction. (1) Excitation; (2) charge carrier transfer; (3) volume recombination; (4) CO2 adsorption; (5) water oxidation with holes; (6) surface recombination; (7) competing to the surface reaction is the H+ reduction; (8) re-oxidation of the reduced products.

Fig. 6. (a) Schematic drawing of the charge carrier relaxation: (1) the electronic relaxation within CB; (2) trapping into deep states (DT) and shallow states (ST); (3) band edge electron-hole recombination; (4) the trapped electron-hole recombination; (5) exciton-exciton annihilation. (b) The lifetime photo-induced reactions of TiO2.

Fig. 7. The energy diagram of n-type TiO2 semiconductor in contact with second phase for the case (a) Ef > Eredox or Ef > ΦM leading to Schottky barrier (Us) with width W, ΦM is the work function of the metal, and (b) after applying anodic bias (+ΔU), further modifying Us and W. (c-e) Accumulation of charge carrier on the surface and form three different space charge region.

Table 1 Standard molar enthalpy, ΔHo298, and the Gibbs free energy, ΔGo298, for the reduction reactions of CO2.

Reaction	ΔH^o₂₉₈ (kJ mol^‒1)	ΔG^o₂₉₈ (kJ mol^‒1)
Reduction reactions of CO₂ with H₂O
H₂O(l) → H₂(g) + 1/2O₂(g)	—	237
CO₂(g) → CO(g) + 1/2O₂(g)	—	257
CO₂(g) + H₂O(l) → HCOOH(l) + 1/2O₂(g)	541	275
CO₂(g) + H₂O(l) → HCHO(l) + O₂(g)	795.8	520
CO₂(g) + H₂O(l) → CH₃OH(l) + 3/2O₂(g)	727.1	703
CO₂(g) + H₂O(l) → CH₄(g) + 2O₂(g)	890.9	818
CO₂ hydrogenation reduction [66]
CO₂ + H₂ → CO + H₂O(g)	41.2	28.6
CO₂ + H₂ → HCOOH(l)	-31.2	33.0
CO₂ + 3H₂ → CH₃OH + H₂O(l)	-131.0	-9.0
CO₂ + 4H₂ → CH₄ + 2H₂O(g)	-164.9	-113.5
2CO₂ + 6H₂ → C₂H₄ + 4H₂O(g)	-127.91	-57.52
3CO₂ + 9H₂ → C₃H₆ + 6H₂O(g)	-249.84	-125.69
4CO₂ + 12H₂ → C₄H₈ + 8H₂O(g)	-360.44	-179.95

Fig. 8. An overview of the methodology that improves the photocatalytic performance of TiO2 for CO2 reduction.

Table 2 Records in literature of TiO2 for photocatalytic CO2 reduction.

Photocatalyst	Synthesis method	Light source	Reaction condition	Yield of product (μmol·g^-1·h^-1)	Sel. to CH₄ (%)
Hollow anatase TiO₂	solvothermal	300 W Xe lamp	G.P., 50 mg cat., 0.06 MPa	CH₄ (1.72)	100 [53]
Porous TiO₂ (B)	micro-wave-assisted solvothermal	300 W Xe light	L.P. (84 mg NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 100 mg cat., 80 °C	CH₄ (0.77), CH₃OH (0.27)	74.03 [97]
0D TiO₂ nanotubes	hydrothermal	300 W Xe lamp	L.P. (100 mL DI water), 50 mg cat., 101 kPa, 25 °C	CH₄ (19.31)	100 [98]
F-TiO_2-_x	template, hydrothermal	300 W Xe lamp (AM 1.5)	L.P. (1 mL UP H₂O), 50 mg cat.; 10 kPa, 40 °C	CO (6.52) CH₄ (4.31)	60.2 [99]
N-TiO₂	hydrothermal	300 W Xe lamp	L.P. (0.12 g NaHCO₃ + 0.3 mL 4 mol L^?1 HCl) 100 mg cat.	CH₃OH (0.36)	0 [73]
Mo/TiO₂	one-step hydrothermal	300 W Xe lamp	G.P. (20 mL CO₂), L.P. (20 μL H₂O), 298 K	CO (8.2), CH₄ (9.8)	54.4 [100]
Co/TiO₂ (Co:Ti=0.15)	in situ grow&cal.	300 W Xe lamp	L.P. (3 mL H₂O), 100 mg cat., 80 kPa	CO (0.34), CH₄ (0.18)	34.6 [101]
Eu/TiO₂	sol-gel	300 W Xe lamp	L.P. (100 mL H₂O), 50 mg cat., 101 kPa, 25 °C	CO (4.77), CH₄ (7.28)	60.41 [102]
Ag/TiO₂	in situ growth, calcination	300 W Xe lamp (AM 1.5)	G.P. (CO₂ + 0.5% water vapor) cat. plates, 25 °C	CH₄ (4.93)	100 [103]
Black TiO₂@Cu	atomic layer deposition	300 W Xe lamp	L.P. (1 mL H₂O), 10 mg cat., 20 °C	CO (23.25), CH₄ (4.3)	15.6 [104]
Ag-Mo-TiO₂	impregnation, photodeposition	mercury lamp (365 nm)	G.P. (CO₂ + 4.7% water vapor) 10 mg cat., 45 °C	CH₄ (37.18)	100 [105]
CuO-TiO₂	in situ growth, calcination	mercury lamp	L.P. (30 mL methanol), 30 mg cat., 25 °C	CH₃OOCH (1600)	0 [106]
brookite TiO₂/g-C₃N₄	in situ grow & calcination	300 W Xe lamp	L.P. (1.5 g Na₂CO₃ + 5 mL 4 nol/L H₂SO₄), 60 mg cat.	(λ > 400 nm) CO (0.84) CH₄ (5.21) UV-vis light CO (1.27) CH₄ (6.49)	86.15 [107] 79.7 [107]
TiO_2-_x/W₁₈O₄₉	template, calcination, alkaline hydrothermal	optical fiber lamp	G.P. (CO₂ gas with a flow rate of 0.42 mL min^?1), 10 mg cat., 80 °C	CO (0.54)	0 [108]
Photocatalyst	Synthesis method	Light source	Reaction condition	Yield of products (μmol g^-1 h^-1)	Sel. to CH₄ (%)
TiO₂/ZnIn₂S₄	template, in situ growth	300 W Xe lamp	L.P. (10 mL deionized water; 1 mmol NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 25 mg cat., 80 °C	CO (9.28) CH₄ (4.26) CH₃OH (4.78)	23.25 [109]
Pt-Cu₂O/TiO₂	solvothermal, co-deposition	300 W Xe lamp	L.P. (10 mL deionized water) 20 mg cat. positioned on a plate, 71 kPa, 20 °C	CO (0.05) CH₄ (1.42)	96.6 [110]
TiO₂/N‐doped graphene	solvothermal, calcination	300 W Xe lamp	L.P. (10 mL deionized water; 0.084 g NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 20 mg cat.	CO (8.68) CH₄ (3.76) CH₃OH (5.67)	20.76 [111]
Au/TiO₂/BiVO₄	hydrothermal, wet chemical	300 W Xe lamp	L.P. (10 mL deionized water), 200 mg cat.	CO (2.5) CH₄ (7.5)	75 [112]
TiO₂/polydopamine	template, and calcination	300 W Xe lamp	L.P. (10 mL deionized water; 0.084 g NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 50 mg cat.	CH₄ (1.4) CH₃OH (0.26)	83.33 [96]
TiO₂/CsPbBr₃	electrostatic self-assembly, solvothermal	300 W Xe lamp	L.P. (30 mL acetonitrile+100 μL water) 10 mg cat.	CO (3.97)	100 [113]
TiO₂/MXene Ti₃C₂	chemical etching, calcination	300 W Xe arc lamp	L.P. (84 mg NaHCO₃ + 0.3 mL 4 mol L^?1 HCl), 50 mg cat., 80 °C	CH₄ (4.4)	100 [114]
Pt@CdS/TiO₂	gas bubbling-assisted membrane reduction-precipitation	300 W Xe lamp	G.P. (CO₂ + water vapor), 20 mg cat., 0.1 MPa, 20 °C	CO (0.7) CH₄ (36.8)	90.1 [115]
TiO₂/CuInS₂	electrostatic self-assembly, hydrothermal, calcination	350 W Xe lamp	L.P. (10 mL deionized water; 0.12 g NaHCO₃ + 0.25 mL 2 mol/L H₂SO₄), 50 mg cat.	CH₄ (2.5) CH₃OH (0.86)	74.4 [116]
TiO₂/CdS	anodization-calcination, successive ionic layer adsorption and reaction	300 W Xe lamp	L.P. (84 mg NaHCO₃ + 0.3 mL 4 mol L^?1 HCl), 4 cm² cat pieces	CH₄ (11.9 mmol·h^-1·m^-2)	100 [57]
TiO₂/C₃N₄/Ti₃C₂	hydrothermal-induced solvent-confined monomicelle self-assembly, electrostatic self-assembly	350 W Xe lamp	L.P. (0.84 mg NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 30 mg cat.	CO (4.39) CH₄ (1.20)	21.47 [117]
MOFs/TiO₂	hydrothermal, solvothermal	350 W Xe lamp	L.P. (5 mL ultra-pure water), 1 mg cat., 45 °C	CO (11) CH₄ (1.1)	9.0 [44]
TiO₂-PdH_0.43	Solvothermal	300 W Xe lamp with UV light	L.P. (1 mL H₂O), 15 cat., 0.15 MPa	CO (3.92) CH₄ (16.41)	73.4 [118]
MoS₂/TiO₂/ graphene	hummers, hydrothermal & photodeposition	350 W Xe lamp	L.P. (4 mL D.I. water), cat. 40 °C	CO (92.33) CH₄ (1.693) C₃H₈ (1.155)	1.8 [91]

Table 2 Records in literature of TiO2 for photocatalytic CO2 reduction.

Photocatalyst	Synthesis method	Light source	Reaction condition	Yield of product (μmol·g^-1·h^-1)	Sel. to CH₄ (%)
Hollow anatase TiO₂	solvothermal	300 W Xe lamp	G.P., 50 mg cat., 0.06 MPa	CH₄ (1.72)	100 [53]
Porous TiO₂ (B)	micro-wave-assisted solvothermal	300 W Xe light	L.P. (84 mg NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 100 mg cat., 80 °C	CH₄ (0.77), CH₃OH (0.27)	74.03 [97]
0D TiO₂ nanotubes	hydrothermal	300 W Xe lamp	L.P. (100 mL DI water), 50 mg cat., 101 kPa, 25 °C	CH₄ (19.31)	100 [98]
F-TiO_2-_x	template, hydrothermal	300 W Xe lamp (AM 1.5)	L.P. (1 mL UP H₂O), 50 mg cat.; 10 kPa, 40 °C	CO (6.52) CH₄ (4.31)	60.2 [99]
N-TiO₂	hydrothermal	300 W Xe lamp	L.P. (0.12 g NaHCO₃ + 0.3 mL 4 mol L^?1 HCl) 100 mg cat.	CH₃OH (0.36)	0 [73]
Mo/TiO₂	one-step hydrothermal	300 W Xe lamp	G.P. (20 mL CO₂), L.P. (20 μL H₂O), 298 K	CO (8.2), CH₄ (9.8)	54.4 [100]
Co/TiO₂ (Co:Ti=0.15)	in situ grow&cal.	300 W Xe lamp	L.P. (3 mL H₂O), 100 mg cat., 80 kPa	CO (0.34), CH₄ (0.18)	34.6 [101]
Eu/TiO₂	sol-gel	300 W Xe lamp	L.P. (100 mL H₂O), 50 mg cat., 101 kPa, 25 °C	CO (4.77), CH₄ (7.28)	60.41 [102]
Ag/TiO₂	in situ growth, calcination	300 W Xe lamp (AM 1.5)	G.P. (CO₂ + 0.5% water vapor) cat. plates, 25 °C	CH₄ (4.93)	100 [103]
Black TiO₂@Cu	atomic layer deposition	300 W Xe lamp	L.P. (1 mL H₂O), 10 mg cat., 20 °C	CO (23.25), CH₄ (4.3)	15.6 [104]
Ag-Mo-TiO₂	impregnation, photodeposition	mercury lamp (365 nm)	G.P. (CO₂ + 4.7% water vapor) 10 mg cat., 45 °C	CH₄ (37.18)	100 [105]
CuO-TiO₂	in situ growth, calcination	mercury lamp	L.P. (30 mL methanol), 30 mg cat., 25 °C	CH₃OOCH (1600)	0 [106]
brookite TiO₂/g-C₃N₄	in situ grow & calcination	300 W Xe lamp	L.P. (1.5 g Na₂CO₃ + 5 mL 4 nol/L H₂SO₄), 60 mg cat.	(λ > 400 nm) CO (0.84) CH₄ (5.21) UV-vis light CO (1.27) CH₄ (6.49)	86.15 [107] 79.7 [107]
TiO_2-_x/W₁₈O₄₉	template, calcination, alkaline hydrothermal	optical fiber lamp	G.P. (CO₂ gas with a flow rate of 0.42 mL min^?1), 10 mg cat., 80 °C	CO (0.54)	0 [108]
Photocatalyst	Synthesis method	Light source	Reaction condition	Yield of products (μmol g^-1 h^-1)	Sel. to CH₄ (%)
TiO₂/ZnIn₂S₄	template, in situ growth	300 W Xe lamp	L.P. (10 mL deionized water; 1 mmol NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 25 mg cat., 80 °C	CO (9.28) CH₄ (4.26) CH₃OH (4.78)	23.25 [109]
Pt-Cu₂O/TiO₂	solvothermal, co-deposition	300 W Xe lamp	L.P. (10 mL deionized water) 20 mg cat. positioned on a plate, 71 kPa, 20 °C	CO (0.05) CH₄ (1.42)	96.6 [110]
TiO₂/N‐doped graphene	solvothermal, calcination	300 W Xe lamp	L.P. (10 mL deionized water; 0.084 g NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 20 mg cat.	CO (8.68) CH₄ (3.76) CH₃OH (5.67)	20.76 [111]
Au/TiO₂/BiVO₄	hydrothermal, wet chemical	300 W Xe lamp	L.P. (10 mL deionized water), 200 mg cat.	CO (2.5) CH₄ (7.5)	75 [112]
TiO₂/polydopamine	template, and calcination	300 W Xe lamp	L.P. (10 mL deionized water; 0.084 g NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 50 mg cat.	CH₄ (1.4) CH₃OH (0.26)	83.33 [96]
TiO₂/CsPbBr₃	electrostatic self-assembly, solvothermal	300 W Xe lamp	L.P. (30 mL acetonitrile+100 μL water) 10 mg cat.	CO (3.97)	100 [113]
TiO₂/MXene Ti₃C₂	chemical etching, calcination	300 W Xe arc lamp	L.P. (84 mg NaHCO₃ + 0.3 mL 4 mol L^?1 HCl), 50 mg cat., 80 °C	CH₄ (4.4)	100 [114]
Pt@CdS/TiO₂	gas bubbling-assisted membrane reduction-precipitation	300 W Xe lamp	G.P. (CO₂ + water vapor), 20 mg cat., 0.1 MPa, 20 °C	CO (0.7) CH₄ (36.8)	90.1 [115]
TiO₂/CuInS₂	electrostatic self-assembly, hydrothermal, calcination	350 W Xe lamp	L.P. (10 mL deionized water; 0.12 g NaHCO₃ + 0.25 mL 2 mol/L H₂SO₄), 50 mg cat.	CH₄ (2.5) CH₃OH (0.86)	74.4 [116]
TiO₂/CdS	anodization-calcination, successive ionic layer adsorption and reaction	300 W Xe lamp	L.P. (84 mg NaHCO₃ + 0.3 mL 4 mol L^?1 HCl), 4 cm² cat pieces	CH₄ (11.9 mmol·h^-1·m^-2)	100 [57]
TiO₂/C₃N₄/Ti₃C₂	hydrothermal-induced solvent-confined monomicelle self-assembly, electrostatic self-assembly	350 W Xe lamp	L.P. (0.84 mg NaHCO₃ + 0.3 mL 2 mol L^?1 H₂SO₄), 30 mg cat.	CO (4.39) CH₄ (1.20)	21.47 [117]
MOFs/TiO₂	hydrothermal, solvothermal	350 W Xe lamp	L.P. (5 mL ultra-pure water), 1 mg cat., 45 °C	CO (11) CH₄ (1.1)	9.0 [44]
TiO₂-PdH_0.43	Solvothermal	300 W Xe lamp with UV light	L.P. (1 mL H₂O), 15 cat., 0.15 MPa	CO (3.92) CH₄ (16.41)	73.4 [118]
MoS₂/TiO₂/ graphene	hummers, hydrothermal & photodeposition	350 W Xe lamp	L.P. (4 mL D.I. water), cat. 40 °C	CO (92.33) CH₄ (1.693) C₃H₈ (1.155)	1.8 [91]

Fig. 9. Scheme of five different TiO2 heterojunctions. (a) Type-I; (b) type-II; (c) p-n heterojunction; (d) direct Z-scheme; (e) indirect Z-scheme; (f) S-scheme. D: electron donor; A: electron acceptor.

Fig. 10. TEM (a) and HRTEM (b) images of 3DOM CeO2/TiO2. (c) Schematic illustration of 3DOM CeO2/TiO2 under simulated visible light irradiation for CO2 photoreduction. Reprinted with permission from Ref. [121]. Copyright 2021, American Chemical Society.

Fig. 11. (a) Schematic illustration of photocatalytic HCOOH formation from CO2 over InP/[MCE]s under simulated visible light irradiation. (b) Photocatalytic production analysis via Isotope tracer. Reprinted with permission from Ref. [143]. Copyright 2011, Journal of the American Chemical Society.

Fig. 12. (a) High-resolution XP spectra measured in dark or under irradiation of UV light. (a) Ti 2p; (b) O 1s; (c) Br 3d. The electrostatic potentials of anatase TiO2 (d), rutile TiO2 (e) and CsPdBr3 (f). (g) Possible photocatalytic mechanism of CsPdBr3/TiO2 under visible light irradiation. (h) Transient adsorption photoluminescent spectra for TiO2 and CsPdBr3/TiO2 under the excitation wavelength of 450 and 520 nm, respectively. Reprinted with permission [113]. Copyright 2020, The authors.

Fig. 13. (a) AFM image of CdS/pyrene-alttriphenylamine. PT composite; Surface potential under dark (b) and surface potential under illumination (c). (d) Distribution of surface potential in the region A and B under dark and illumination, respectively. (e) The schematic illustration of photoirradiation KPFM. Reprinted with permission from Ref. [154]. Copyright 2021, Wiley-VCH.

Fig. 14. Surface physicochemical reactions on TiO2 photocatalyst in the CO2 photoreduction process.

Fig. 15. SEM image (a) and TEM image (b) of Ag@TiO2. (c) CH4 evolution in the reaction cell over time under AM1.5 solar simulator irradiation. (d) Proposed mechanism of CO2 photoconversion to CH4 by Core-Shell Ag@TiO2. Reprinted with permission from Ref. [103]. Copyright 2019, American Chemical Society.

Fig. 16. Photocatalytic activity of CO2 into CH4 (a), and (b) over different Er1 modified carbon nitride. (c) The calculated free-energy diagram for CO2 reduction to CO and CH4 and on the adsorption configurations of intermediates over HD-Er1/CN-NT. Reproduced with permission [72]. Copyright 2020, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fig. 17. (a) Schematic illustration of the basic mechanism of the TiO2 photocatalytic process. (b) Comparison of the photocatalytic activity of the samples with common photocatalysts under visible light, calculated according to the amounts evolved in 6 h. Reprinted with permission from Ref. [101]. Copyright 2015, the Royal Society of Chemistry.

Fig. 18. Mechanism of CO2 photocatalytic reduction over V and W co-doped TiO2 under visible light.

Fig. 19. The reaction mechanisms involved in the CO2 reduction for the Co and Cu-Co-doped TiO2 on the surface.

Fig. 20. (a) The simulated state of CO2 adsorption on the basic oxide (001) surfaces. Total adsorption energy (b) and adsorption energy (c) broken down into strain and bonded components for CO2 adsorption on the basic oxide (MgO, SrO, CaO, and BaO) surfaces. (d) Adsorption energies for intermediate species CO2, COOH, and CO on TiO2, 0.5 ML SrO/TiO2, and 1 ML SrO/TiO2. Reprinted with permission from Ref. [228]. Copyright 2016, Royal Society of Chemistry.

Fig. 21. A schematic illustration for a photoelectrochemical setup for CO2 reduction. Several paths are included in the reaction: (1) excitation, (2) charge carrier transfer, (3) electrons flow from the working electrode to the counter electrode, (4) O2 evolution with holes, (5) CO2 adsorption, and (6) CO2 reduction.

Fig. 22. Schematic illustration of a three-electrode CO2 reduction configuration of a PEC cell. (a) A semiconductor serving as a photocathode. (b) A semiconductor serving as a photoanode. (c) Semiconductors serving as both a photocathode and a photoanode.

Table 3 The possible reactions in the reduction of CO2 and corresponding potentials (vs. NHE. 25 °C, 1 atm).

Reaction	Potential (V) vs. NHE at pH = 7
Oxidation potentials of H₂O
H₂O + 2h⁺ → 1/2O₂ + 2H⁺	0.82	(1.1)
H₂O + h⁺ → •OH + 2H⁺	2.27	(1.2)
Production of C₁ products
CO₂ + e^- → CO₂•	-1.90	(1.3)
CO₂ + 2H⁺ + 2e^- → HCOOH	-0.61	(1.4)
CO₂ + 2H⁺ + 2e^- → CO + H₂O	-0.53	(1.5)
CO₂ + 4H⁺ + 4e^- → HCHO + H₂O	-0.48	(1.6)
CO₂ + 6H⁺ + 6e^- → CH₃OH + 2H₂O	-0.38	(1.7)
CO₂ + 8H⁺ + 8e^- → CH₄ + 2H₂O	-0.24	(1.8)
Production of C₂ products
CO₂ + 9H⁺ + 12e^- → C₂H₅OH + 12OH^-	-0.33	(1.9)
3CO₂ + 13H₂O + 18e^- → C₃H₇OH + 18OH^-	-0.32	(1.10)
2CO₂ + 8H₂O +12e^- → C₂H₄ + 12OH^-	-0.34	(1.11)
2CO₂ + 2H⁺ + 2e^- → H₂C₂O₄	-0.80	(1.12)
2CO₂ + 14H⁺ + 14e^- → C₂H₆ + 4 H₂O	-0.27	(1.13)
Reduction of potentials of H⁺
2H⁺ + 2e^- → H₂	-0.41	(1.10)

Fig. 23. Pourbaix diagram for the formation of HCOOH from CO2 at 25 °C. Redraw from data in reference [243].

Fig. 24. An overview of the methods to improve the photoelectrochemical activity of TiO2 as a schematic illustration.

Table 4 Records in literature of TiO2 for photoelectrochemical CO2 reduction.

Anode	Light source	Product	Reaction rate	Selectivity
FeS₂/TiO₂ NTs	500 W Xe lamp (λ ≥ 420 nm)	CH₃OH	91.7 μmol h^-1 L^-1	100% [244]
Cu₃(BTC)₂@TiO₂	300 W Xe lamp (< 400 nm)	CH₄	56.6 μmol cm^-2 h^-1	100% [245]
TiO₂	Xe-arc lamp 320-410 nm	HCOOH, CH₃COOH, C₂H₅COOH, CH₃OH, CH₃CH₂OH	5040 nmol cm^-2 h^-1	HCOOH 59% [246]
TiO₂ (TNT)	Xe-arc lamp (320-410 nm)	HCOOH, CH₃OH, CH₃COOH, CH₃CH₂OH, C₂H₅COOH	4340 nmol cm^-2 h^-1	HCOOH 40% [247]
InP/TiO₂ NTs	500 W Xe lamp (λ > 420 nm)	CH₃OH	295 μmol cm^-2 L^-1	100% [239]
n-TiO₂-TNT	150 W Xe lamp	CH₄, CO	120 nmol cm^-2 h^-1	CH₄ 86% [242]
TiO₂/Pt	Xe lamp (AM 1.5)	HCOOH	200 nmol cm^-2 h^-1	100% [143]
TiO₂-ZIF-8	125 W mercury vapor lamp	CH₃CH₂OH, CH₃OH	0.6 mmol L^-1	CH₃CH₂OH 50% [248]
CdSeTe NSs/TiO₂ NTs	500 W Xe lamp (λ > 420 nm)	CH₃OH	1166.77 μmol L^-1	100% [249]
Cu-RGO-TiO₂	150 W Xe lamp (AM1.5)	CH₃OH, HCOOH	255 μmol h^-1 cm^-2	CH₃OH57% [250]
Au@TNT	AM 1.5 G	CH₃OH, CH₃CH₂OH	2550 μmol h^-1	CH₃OH78% [251]
Au/N-doped TiO₂	300-W Xe lamp	CH₃COOH, CO	233 nmol h^-1	carbon 91.5% [230]
TiO₂	300 W Hg lamp	CO, HCOOH	6150 ppm	CO 98% [252]
TiO₂ film	400 W Xe lamp	HCOOH	168.8 nmol h^-1	100% [253]
RuO_x/TiO₂/Ta/N	visible light (λ > 400 nm)	CO	39 nmol cm^-2	100% [254]
TiO₂ thin film	AM 1.5 G	HCOOH, CO	27.1 μmol h^-1	HCOOH 91% [255]
Argon-treated TiO₂	AM 1.5 G	HCOOH, CO	108.2 mmol g^-1 h^-1	HCOOH 96.5% [256]
Ti³⁺/TiO₂	UV Lamp (254 nm)	CO, CH₄	CO FE, 50%	CO 82% [257]
Ti/TiO₂-CuP	300 W Xe lamp	CH₃OH, CH₃CH₂OH	CH₃OH 0.35 mmol L^-1	CH₃OH, 91.4% [258]
TiO₂ NRs	AM 1.5 G	CO, CH₄	22 μmol·cm^-2	CO 71% [259]
Ce/CdS QDs/TiO₂ NTs	150 W Xe lamp	HCOOH	106.7 nmol·cm^-2	100% [260]

Fig. 25. (a) A schematic illustration of the PEC cell with an a-Si/TiO2/Au photocathode and a BiVO4/FeOOH/NiOOH photoanode for CO2 reduction to syngas. (b) J-V curves for the photoanode and photocathode in a three-electrode configuration. Syngas production using a two-electrode configuration. (c) ST-4Au||BiVO4. (d) ST-7Au||BiVO4. Reproduced with permission [271]. Copyright 2019, Energy & Environmental Science.

Fig. 29. A typical photothermal scheme for CO2 reduction.

Fig. 30. Reaction mechanism for photothermal reactions.

Table 5 Records in literature of TiO2 for photothermal CO2 reduction.

Catalyst	Preparation	System	Light source	Reaction temperature (°C)	Product	Selectivity to CH₄ (%)	Ref.
TiN@TiO₂@In₂O_3-_x (OH)_y	hydrothermal	vapor-solid	300 W Xe lamp	150	CO	0	[287]
TiO₂-graphene	solvothermal	vapor-solid	300 W Xe lamp	116.4	CO, CH₄	95.3	[288]
Pd NPs/TiO₂	hydrothermal	vapor-solid	500 W Hg lamp (λ > 254 nm)	500	CO	0	[289]
AuNPs/TiO₂	solvothermal and deposition/precipitation method	vapor-solid	375 W IR or UV	181	CO, CH₄	60	[290]
Pt/D-TiO_2-_x	hydrothermal	vapor-liquid-solid	300 W Xe lamp	120	CH₄, CO	87.5	[291]
Ov-TiO₂	hydrothermal	vapor-liquid-solid	150 W Xe lamp	120	CH₄, CO	55	[292]
Ov-TiO₂	hydrothermal and calcination method	vapor-solid	UV-light	120	CO	0	[293]
TiO_2-_x/CoO_x	impregnation and calcination	vapor-liquid-solid	150 W UV lamp	120	CO, CH₄	88.33	[294]
Cu₃(BTC)₂@TiO₂	hydrothermal	vapor-liquid-solid	300 W Xe lamp (λ < 400nm)	40	CH₄	100	[249]
CoO/Co/TiO₂	impregnation	vapor-liquid-solid	300 W Xe lamp	120	CH₃OH	0	[295]
CuS/TiO₂	hydrothermal	vapor-liquid-solid	300 W Xe lamp	138	CO	0	[296]
TiO₂ photonic crystals	template-free anodization calcination method	vapor-liquid-solid	300 W Xe arc lamp	22	CH₄	100	[297]
Ni/TiO₂	MOF-template method	vapor-solid	375W IR lamp	207	CO, CH₄	99.6	[298]
Bi/AgBiS₂/P25	solvothermal	vapor-liquid-solid	300 W Xe lamp	50	CO, CH₄	73.17	[76]

Fig. 31. An overview of the methods to improve the photothermal activity of TiO2 that involves the creation of surface frustrated Lewis pairs, decoration of specific photothermal co-catalysts, plasmonic nanoparticles and conventional co-catalysts.

Fig. 32. (a) Illustration of the mechanism toward the enhanced photocatalytic CO2 reduction over Pt/MgAl-LDO/TiO2 with H2O vapor. (b) HRTEM images of Pt/MgAl-LDO/TiO2. (c) IR spectra of CO2 and adsorption on TiO2 and MgAl-LDO/TiO2. Reproduced with permission [308]. Copyright 2018 Elsevier Inc.

Fig. 33. CO generation rate on different composition of photocatalysts (a) and the most active sample ncIn2O3-x(OH)y supported on different substrates (b). (c) Proposed activation mechanism for the CO2 reduction reaction. Reproduced with permission [287]. Copyright 2021 American Chemical Society.

Fig. 34. Charge density difference of the key intermediates on the catalyst surfaces. CO* (a), HCOOH* (b), HCHO* (c), and CH3OH* (d) on TiO2 and CO* (e), HCOOH* (f), HCHO* (g), and CH3OH* (h) on Au/MgO-aTiO2; (i) Illustration of the reaction mechanism on the catalyst surface. Reprinted with permission from Ref. [314]. Copyright 2021, American Chemical Society.

Fig. 35. Optimized structure of the stable configuration of anatase (101) surface (a) and Pd-loaded anatase (101) surface (b). DOS for anatase (101) (c) and Pd-loaded anatase (101) (d). Reprinted with permission from Ref. [289]. Copyright 2018, American Chemical Society.

Fig. 36. (a) PEC reduction of CO2 at Ti/TiO2NT-CuP in 0.1 mol L-1 Na2SO4 saturated with CO2 under UV-vis irradiation. (b) Different bias voltage different setup for CH3OH and C2H5OH formation at bias potential of -0.80 V. Reprinted with permission from Ref. [258]. Copyright 2022 National Academy of Sciences.

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二氧化钛基光催化剂用于二氧化碳还原和太阳燃料的生产

TiO₂-based photocatalysts for CO₂ reduction and solar fuel generation

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二氧化钛基光催化剂用于二氧化碳还原和太阳燃料的生产

TiO2-based photocatalysts for CO2 reduction and solar fuel generation

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TiO₂-based photocatalysts for CO₂ reduction and solar fuel generation