Inter-plane 2D/2D ultrathin La2Ti2O7/Ti3C2 MXene Schottky heterojunctions toward high-efficiency photocatalytic CO2 reduction

doi:10.1016/S1872-2067(22)64155-X

Abstract

Abstract:

Ascribing to incremental fossil fuels emissions, the utilization and conversion of CO₂ and development of renewable energy is globally essential and significative. Ultrathin 2D/2D heterojunctions with fast photo-generated electrons transmission channels illustrate a better strategy to improve photocatalytic activity. Herein, combing La₂Ti₂O₇ with metallic few-layered Ti₃C₂ MXene to construct inter-plane 2D/2D heterojunction was in situ self-assembled through solvothermal method. Benefiting from the advantages including stability, conductivity, abundant active sites and formation of Schottky junctions, as expected, the ultrathin 2D/2D La₂Ti₂O₇/Ti₃C₂ MXene nanosheets presented much improved photocatalytic ability for CO₂ reduction to CO and CH₄, which is about 4.6 and 11.4 times higher than that of mechanical mixed La₂Ti₂O₇ and Ti₃C₂ MXene. fs-TAS and XPS provided direct evidence that the prominence of La₂Ti₂O₇/Ti₃C₂ MXene in photocatalytic CO₂ reduction reaction over other opponents should be attributed to the synergetic effect of efficient charge carrier mobility and formed 2D/2D Schottky heterojunction interfacial contact between La₂Ti₂O₇ and Ti₃C₂ MXene. Intermediates revealed by in-situ DRIFTS and corresponding atomic-level DFT calculations confirmed the mechanism, pathways and selectivity for photocatalytic CO₂ conversion. This work expanded promising prospects arouses new impetus for deepening the prehension of the mechanism of photocatalytic CO₂ reduction, designing and fabrication of Schottky heterojunctions for application in conversion and utilization of CO₂.

Key words: La₂Ti₂O₇, Ti₃C₂ MXene, Photocatalytic CO₂ reduction, 2D/2D, Schottky heterojunction

Ke Wang, Miao Cheng, Nan Wang, Qianyi Zhang, Yi Liu, Junwei Liang, Jie Guan, Maochang Liu, Jiancheng Zhou, Naixu Li. Inter-plane 2D/2D ultrathin La₂Ti₂O₇/Ti₃C₂ MXene Schottky heterojunctions toward high-efficiency photocatalytic CO₂ reduction[J]. Chinese Journal of Catalysis, 2023, 44: 146-159.

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Figures/Tables 10

Scheme 1. Schematic of the synthetic route of the inter-plane 2D/2D ultrathin La2Ti2O7/Ti3C2 MXene nanosheets.

Fig. 1. FESEM images of La2Ti2O7 nanosheets (a), bulk Ti3C2 (b) and LTM-3 composites (c). AFM images of La2Ti2O7 nanosheets (d), few-layered Ti3C2 MXene (e) and corresponding height cutaway view (f).

Fig. 2. (a) XRD patterns of La2Ti2O7, LTM-3 composite and few-layered Ti3C2 MXene. TEM images of La2Ti2O7 nanosheets (b), few-layered Ti3C2 MXene (c). HRTEM images of LTM-3 composites (d,e) and corresponding lattice spacing of La2Ti2O7 (f) and Ti3C2 MXene (g). (h) HAADF-STEM of LTM-3 and EDX element mapping images of La, Ti, O and C.

Fig. 3. UV-vis spectra (a), and N2 adsorption-desorption isotherms with inset pore size distribution spectra (b).

Fig. 4. XPS spectra of survey spectra (a), and high-resolution XPS spectra of La 3d (b), C 1s (c), O 1s (d), Ti 2p (e), diagram (f) of the bond connection between La2Ti2O7 and Ti3C2 MXene.

Fig. 5. (a) CO, CH4 and H2 products over as-prepared photocatalysts. (b) The CO2 reduction and H4 selectivity. (c) Recycling photocatalytic production experiments over LTM-3. (d) GC-MS spectra of the photocatalytic 13CO2 reduction over LTM-3.

Fig. 6. PL spectra (a), TRPL decay spectra (b), Femtosecond transient absorption spectroscopy (fs-TAS) (c,d), Transient photocurrent response (e) and electrochemical impedance spectroscopy (EIS) Nyquist plots (f) of as-prepared samples.

Fig. 7. In-situ DRIFTS of CO2 reduction reaction on LTO and LTM-3 in the spectral regions of 1000?2000 (a), 2600?3500 (b) and 3400?4000 (c) cm?1. (1)?(5) are black, balance, irradiation of 30, 60 and 90 min, respectively.

Fig. 8. (a) Charge density difference. (b) Planar-averaged charge density difference Δρ(z) LTM. The blue color and yellow color in the plot of charge density difference represent the dissipation and accumulation of the charges. (c) Free energy profiles for CO2 reduction on LTO and LTM. (d) Structures for the intermediates on LTM (see details in the Supporting Information).

Scheme 2. Energy scheme before, after contact and under light irradiation of LTO and Ti3C2 MXene.

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Inter-plane 2D/2D ultrathin La₂Ti₂O₇/Ti₃C₂ MXene Schottky heterojunctions toward high-efficiency photocatalytic CO₂ reduction

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