Recent Progress on Photocatalytic CO2 Reduction with Ultrathin Nanostructures

doi:10.15541/jim20210368

Abstract

Abstract:

Since the beginning of the 21st century, energy shortage and environmental pollution have been the major challenges faced by human beings. Photocatalytic carbon dioxide (CO₂) reduction is one of the promising strategies to solve the energy crisis and promote the carbon cycle, in which semiconductor captures solar energy to obtain hydrocarbon fuel. However, the low activity and poor selectivity of the products greatly limit the practical application of this technology. Thus, it is of great significance to regulate product selectivity, improve photocatalytic efficiency, and deeply understand the mechanism of CO₂ reduction reaction. In recent years, ultrathin materials have attracted extensive attention from researchers due to their high specific surface area, abundant unsaturated coordination surface atoms, shortened charge migration path from inside to surface, and tailorable energy band structure, and have achieved promising results in the field of photocatalytic CO₂ reduction. In this paper, the reaction mechanism of photocatalytic CO₂ reduction is firstly summarized. Next, the research results of promoting electron hole separation and regulating charge transport path of ultrathin nanostructures by constructing heterostructures, designing Z-scheme systems, introducing co-catalysts, and defect engineering are introduced. Finally, the prospect and challenge of improving the efficiency of photocatalytic CO₂ reduction and optimizing the product selectivity are pointed out.

Key words: photocatalytic CO₂ reduction, ultrathin heterostructures, cocatalysts, reaction mechanism, review

CLC Number:

TQ174

GAO Wa, XIONG Yujie, WU Congping, ZHOU Yong, ZOU Zhigang. Recent Progress on Photocatalytic CO₂ Reduction with Ultrathin Nanostructures[J]. Journal of Inorganic Materials, 2022, 37(1): 3-14.

Figures/Tables 12

Fig. 1 Different CO2 adsorption modes on the surface of photocatalysts[4]

Table 1 Standard potentials of convert CO2 to various C1 and C2 products in aqueous solutions at standard conditions (1.01×105 Pa and 25 ℃) [34]

Half electrochemical thermodynamic reactions	Standard potential /V (vs SHE)
CO₂(g) + 2H⁺ + 2e^- = HCOOH(1)	-0.250
CO₂(g) + 2H⁺ + 2e^- = CO(g)+ H₂O (1)	-0.106
2CO₂(g) + 2H⁺ + 2e^- = H₂C₂O₄(aq)	-0.500
2CO₂(g) + 2e^- = C₂O₄^2-(aq)	-0.590
CO₂(g) + 4H⁺ + 4e^- = C(s) + 2H₂O(1)	0.210
CO₂(g) + 4H⁺ + 4e^- = CH₂O(1) + H₂O(1)	-0.070
CO₂(g) + 6H⁺ + 6e^- = CH₃OH(1) + H₂O(1)	0.016
CO₂(g) + 8H⁺ + 8e^- = CH₄(g) + 2H₂O(1)	0.169
2CO₂(g) + 12H⁺ + 12e^- = CH₂CH₂(g) + 4H₂O(1)	0.064
2CO₂(g) + 12H⁺ + 12e^- = CH₃CH₂OH(1) + 3H₂O(1)	0.084

Fig. 2 Possible reaction paths for CO2 reduction to produce HCHO, CH3OH, and CH4[35,36] (A) A thermodynamic analysis; (B) A combined thermodynamic and kinetic analysis; (C) Glyoxal route

Fig. 3 Possible reaction paths for CO2 reduction to produce C2H4, CH3CHO, and C2H5OH[35] (A) Coupling of two *CH2 species or CO insertion in a Fischer-Tropsch-like step; (B) *CO dimerization

Fig. 4 (a) Calculated band positions of the WO3 nanosheet and commercial WO3, relative to the redox potential of CO2/CH4 in the presence of water, and (b) CH4 generation over the nanosheet and commercial powder as a function of visible light irradiation time (λ≥420 nm)[38]

Fig. 5 Height images of (a) atomically thin InVO4 nanosheet, (b) nanocube, and (c) bulk materials obtained by conventional solid-state reaction, surface photovoltage spectroscopy (SPV) images in (a′), (b′), and (c′) displaying differential images between potential images under light and in the dark, and (d) surface photovoltage change by subtracting the potential under dark conditions from that under illumination (SPV, ΔCPD = CPDdark - CPDlight)[13]

Fig. 6 Band structures of PCMT@In2O3/ZIS[47]

Fig. 7 Photocatalytic (a) CO and (b) CH4 output changing with light irradiation time, (c) comparison of photocatalytic activity over different samples, (d)schematic illustration of the photocatalytic CO2 reduction for ZnIn2S4/BiVO4 nanocomposite, schematic representation of (e) Z-scheme electron-hole transfer mechanisms, and (f) heterojunction-type electron-hole transfer mechanisms under light irradiation[50]

Fig. 8 TEM images of (a, b) poly(methylmethacrylate) spheres coated with (protonic polyethylenimine (PEI)/Ti0.91O2/ PEI/GO)5, (c, d) (G-Ti0.91O2)5 hollow spheres, and (e)comparation of the average product formation rates[53]

Fig. 9 (a, b) SEM images of InVO4/Ti3C2Tx at higher magnification, (c) HRTEM images of InVO4/Ti3C2Tx, (d)scheme for spatial charge separation and transport during the photocatalytic reduction of CO2 over hierarchical InVO4/Ti3C2Tx heterosystem, and (e)energy level alignment of InVO4/Ti3C2Tx hybrid[56]

Fig. 10 Schematic illustration of the preparation procedure of the Au-TiO2 composites (b), schematic illustration of charge separation and transfer in the Au-TiO2 system and photoreduction of CO2 into different products[57]

Fig. 11 (a) Scheme of the electronic band structures of Vo-rich WO3 atomic layers and WO3 atomic layers, and (b) in situ FT-IR spectra for the IR light-driven CO2 reduction process on the Vo-rich WO3 atomic layers[60]

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Recent Progress on Photocatalytic CO₂ Reduction with Ultrathin Nanostructures

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