Photothermal catalysis in CO2 reduction reaction: Principles, materials and applications
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摘要: 碳元素消耗导致了大量的CO2排放,这引起了人们的广泛关注。发展可再生能源和减少CO2排放的技术已成为世界上最迫切需要解决的问题之一。其中,太阳能作为地球上最理想的清洁能源,已成为当前研究的热点。如果可以利用太阳能将CO2转化为有价值的碳基化学品,以上两个问题可以同时解决。光催化法和热催化法在CO2还原中的应用已有许多报道。但关于光热催化还原二氧化碳的研究较少。本文综述了光热催化在CO2还原中的研究现状,介绍了光热催化的概念和原理,催化剂的分类(新型炭材料、氧化物材料、金属硫化物材料、MOF材料、层状双氢氧化物材料)和催化剂的改性,以及其在CO2还原方面的应用。最后,本文对催化剂的发展趋势进行了预测。因此,合理开发碳基化学品可以减少传统能源的消耗、碳排放,实现碳的循环利用。Abstract: Reducing CO2 emission has become one of the most urgent issues in the world. The use of abundant solar energy to convert carbon dioxide into carbon-based chemicals would be a tremendous advance. There are many papers on photocatalysis or thermal catalysis in the reduction of CO2, however, there is little research on photothermal catalysis for this purpose. We summarize our current knowledge of this topic, and the classification of catalysts (new carbon materials, oxide materials, metal sulfide materials, MOF materials, layered double hydroxide materials), their modification and their use in the reduction of CO2 is discussed. Trends in the development of new catalysts are considered.
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Key words:
- Photothermal catalysis /
- CO2 reduction reaction /
- New carbon materials /
- MOF materials /
- Heterojunction
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Figure 2. (a) Functioning principles and categories of photothermal catalysis. Copyright 2021 Elsevier Ltd. (b) Thermal-assisted photocatalysis. Copyright 2014 the authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) Photo-driven thermal catalysis. Copyright 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) Photothermal co-catalysis. Copyright 2020 American Chemical Society
Figure 5. (a) Schematic diagram. (b) TEM images of g-C3N4-Pd nano-cubes (NCs) with Pd(100) facets and g-C3N4-Pd nano-tetrahedrons (NTs) with Pd(111) facets. Copyright the Royal Society of Chemistry 2014. (c) H2 and (d) CO production as a function of reaction time over the sample of g-C3N4-Pdnanocubes and g-C3N4-Pd nano-tetrahedrons under visible light irradiation. Copyright the Royal Society of Chemistry 2014. (e) Illustration of the visible-light-driven CO2 to CO reduction process (BIH is the sacrificial electron donor). (f) Generation of CO (black squares) and H2 (red circles) over 4 days upon visible-light irradiation (λ > 400 nm) of a CO2-saturated ACN solution containing 6 mg Coqpy@mpg-C3N4, 0.05 M BIH (sacrificial donor) and 0.03 mol L−1 PhOH (proton source). (g) Generation of CO (black squares) and H2 (red circles) during four consecutive 24 h irradiation cycles using the same hybrid material. Copyright 2020 American Chemical Society
Figure 6. (a) HRTEM image of Au-Cu/TiO2 material. (b)The top part summarizes the proposal to rationalize the influence of the irradiation wavelength range on the product distribution using (Au, Cu)/TiO2 as photocatalysts. The bottom part presents a plausible route for methane generation in the gas-phase CO2 photoreduction by water. (c) Temporal evolution of H2 and CH4 production throughout 46 h of irradiation time using (Au, Cu)/TiO2 (Au/Cu ratio 1∶2). Copyright 2014 American Chemical Society. (d) Graphical abstract. (e-f) The production rates of CH4 during the photocatalytic CO2 reduction with H2O on STO, B-STO-10, B-STO-20, and B-STO-30. Copyright 2017 Elsevier Ltd
Figure 7. (a) Photocatalytic CO2 reduction coupled with oxidative organic synthesis by semiconductor QDs. (b)The rate of photocatalytic CO2 reduction reaction using different semiconductor QDs as the photocatalysts. (c) Photocatalytic CO2 reduction of CdSe QDs modified with a different atomic thickness of CdS shell under the same conditions. (d) Long-time photocatalytic CO2 reduction experiment using CdSe/CdS QDs as photocatalysts and TEA as an electron donor under Xe lamp irradiation (300 mW with 400 nm filter). (e) GC-MS chromatogram of gas products obtained by photocatalytic reaction under CO2 atmosphere with different irradiation times. (f) Growth kinetics of CO and the corresponding decay kinetics of CO2 along with 450 nm LEDs irradiation obtained from GC quantization. Copyright 2019 Elsevier Inc
Figure 8. (a) Schematic diagram. (b) The amount of HCOO− produced as a function of the time of visible-light irradiation. Copyright 2015 American Chemical Society. (c) Schematic diagram. (d) Plots of CO evolution turnover number CO-TON versus time in the photocatalytic CO2 reduction with MOF-4 (blue square) and homogeneous H2L4 (red circle). Copyright 2011 American Chemical Society
Figure 9. (a) Illustration of the different CoFe-x catalysts formed by hydrogen reduction of a CoFeAl-LDH nanosheet precursor at different temperatures. (b) Time course of CO2 conversion and product selectivity for CO2 hydrogenation over CoFe-650 under UV–vis irradiation. (c) The hydrocarbon product distribution was obtained over CoFe-650 under UV–vis irradiation for 2 h. Copyright 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Figure 11. (a) Band structures of some representative photocatalysts. Copyright 2020 Elsevier Inc. (b) Schematic illustration of TiO2/CsPbBr3 heterojunction: internal electric field (IEF)-induced charge transfer, separation, and the formation of S-scheme heterojunction under UV–visible-light irradiation for CO2 photoreduction. Copyright 2020 Springer Nature Inc. (c) Schematics illustrating the photo-excited electron-hole separation process of BiW heterostructures in photothermal catalysis. Copyright 2019 Elsevier Inc. (d) Schematic representation of the preparation of COF-318-SCs via the condensation of COF-318 and semiconductor. Copyright 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
Figure 12. Crystal structure of MoO3-x and MoO3: (a) XRD patterns. (b) TEM of the MoO3. (c) TEM of the MoO3-x. (d) HRTEM of the MoO3, and (e)HRTEM of the MoO3-x. Copyright the Royal Society of Chemistry 2019. Photothermal catalytic activities of CO2 conversion over TiO2(AB) treated with SPP for 0 and 2 h (samples T-0 h and T-2 h, respectively) upon (f) 100 mW·cm−2 solar and (g) visible (
$\lambda $ ≥ 420 nm) light irradiation (N/D: not detected). Acetaldehyde degradation and CO2 evolution over T-0 h and T-2 h: (h) under visible light at room temperature and (i) under UV light with heating at 70 °C. Copyright 2020 The Authors Published by WILEY-VCH Verlag GmbH & Co. KGaA, WeinheimFigure 13. (a) The CO2 cycloaddition of photothermally-driven, Copyright 2022 Elsevier Inc. (b) Graphical abstract. Copyright 2021 American Chemical Society. (c) Schematic illustration of the formation mechanism, catalytic process, and advantages for CO2 photothermal reduction into CO over C-In2O3−x.. (d) CO production rates of Vo-poor In2O3, Vo-rich In2O3−x, and C-In2O3−x with different carbon content. (e) Photothermal CO2 conversion test and selectivity of C-In2O3−x. Copyright 2021 Wiley-VCH GmbH
Figure 14. (a) Geometric and electronic structures of a single atom, clusters, and nanoparticles, Copyright 2018 American Chemical Society. (b) Illustration of CO2 conversion mechanism on small and large Cu-Pt nanoclusters on TiO2. (c) Photocatalytic CH4 evolution as a function of time. Copyright the Royal Society of Chemistry 2013. (d) Schematic diagram. Copyright 2013 American Chemical Society
Figure 15. (a) Schematic diagram of enhanced carbon dioxide hydrogenation in photothermal process with Au/CeO2. (b) TEM image of Au/CeO2 sample. The inset figure on top is the corresponding HRTEM image. Estimation of (c) CO2 and (d) hydrogen orders from the dependence of kinetic rate on the reactant partial pressure in photothermal or thermal processes over the Au/CeO2 catalysts at 673 K. (e) CO2 conversion on Au/CeO2 in the photothermal or thermal process. (f) CO2 conversion &CO selectivity on Au/CeO2 or CeO2 catalysts at 400 °C under different conditions. Copyright 2019 Elsevier Inc
Table 1. Lists the electrochemical CO2 reduction potentials versus the NHE at pH=7
Reactions E (V vs NHE, pH=7) CO2+e− →*CO2 −1.9 V CO2+2H+ +2e− →HCOOH −0.61 V CO2+2H+ +2e− → CO+H2O −0.53 V CO2+4H+ +4e− → HCHO+H2O −0.48 V CO2+6H+ +6e−→CH3OH+H2O −0.38 V CO2+8H+ +8e− →CH4+2H2O −0.24 V H2O +2e− →H2 −0.41 V Table 2. Performance of catalyst materials for photothermal reduction reaction of CO2
Photothermalcatalysts Test conditions Yield (CO)
µmol·g−1·h−1Yield (CH4)
µmol·g−1·h−1Yield (others)
µmol·g−1·h−1Ref. Carbon materials gC3N4/ graphdiyne CO2 and H2O under 300 W Xe lamp 23.95 0.40 — [23] TiO2/ graphdiyne CO2, H2O and MeCN under 350 W Xe lamp 50.53 2.80 — [24] Bi2WO6/ Ti3C2 CO2 and H2O under 300 W Xe lamp — 1.78 CH3OH: 0.44 [25] gC3N4/Ti3C2 CO2 and H2O under 300 W Xe lamp with 420 nm filter 2.42 0.04 — [26] gC3N4/Ti3C2Tx CO2 and H2O under 300 W Xe lamp — 2.12 — [27] TiO2/Ti3C2 CO2 and H2O under 300 W Xe lamp — 4.40 — [28] P25/Ti3C2 CO2 and H2O under 300 W Xe lamp 11.74 16.61 — [29] ZnO/Ti3C2 CO2 and H2O under 300 W Xe lamp 30.30 20.33 — [30] Ni/Nb2C CO2 and H2O under 300 W Xe lamp — 72.50 — [31] gC3N4/TiO2/Ti3AlC2 CO2 and H2O under 35 WHID car lamp of 20 mW/cm2 in fixed bed reactor 297.26 2103.50 — [32] TiO2-graphene 300 W Xe lamp, UV- visible light 2.00 25.00 — [33] Oxide materials LaNixCo1-xO3 300 W Xe lamp equipped with a UV-light filter (λ>420 nm); 350 °C — 113.13 CH3OH: 3.47 [34] Pd-TiO2 A mercury lamp (500 W, λ>254 nm); 773 K 11.05 — — [35] Ni/TiO2-CeO2 300 W Xenon arc lamp, UV light; λ>254 — 17.00 — [36] Ni(5)-BaTiO3 300 W Xe lamp, UV–visible light — 103.70 — [37] m-WO3-x 300 W high-pressure Xe lamp (λ>420 nm); 250 °C — 25.77 CH3OH: 4.1 [38] CuS/TiO2 300 W Xe lamp, UV- visible light; 99 °C 25.97 — — [39] (P-R)Ni/TiO2 300 W Xe lamp, UV- visible light; 400 °C — 60 mL — [40] TiO2/H2-150 300 W Xe lamp, UV- visible light; 120 °C 23.00 — — [41] CoO-CuO/TiO2-CeO2 300 W Xe lamp, UV- visible light; 80 °C 5.00 0.50 — [42] BaZr0.5Ce0.3Y0.2O3−δ 300 W Xe lamp, UV- visible light; 350 °C — 39.13 C2H6: 8.64, C3H8: 3.22 [43] Ru/HxMoO3-y 300 W Xe lamp, Vis-NIR light; 140 °C — 20.80 — [44] BiOx/CeO2 300 W Xe lamp, UV- visible light; 400 °C 31.00 — — [45] Pd2Cu/P25 300 W Xe lamp, UV- visible light; 150 °C — — CH3CH2OH: 41 [46] Ni/TiO2 300 W Xe lamp, UV- visible light 1.40 271.90 — [47] Metal sulfides materials CdS/ graphdiyne CO2 and H2O under 300 W Xe lamp of 100 W·cm−2 with AM1.5 16.61 0.32 CH3OH: 1.79 [48] SnS2 CO2 and H2O under 300 W Xe lamp of 100 W·cm−2 with AM1.5 12.28 — — [49] ZnIn2S4-In2O3 CO2 and H2O under 300 W Xe lamp of 100 W·cm−2 with AM1.5 3075 — — [50] In2S3-CdIn2S4 300 W Xe lamp, UV- visible light 825 — — [51] CdSe/CdS 300 W Xe lamp, UV- visible light 412.80 — — [2] MOF materials and derivatives (MOF-253–Ru(CO)2Cl2 300 W Xe lamp, UV- visible light 2.73 — — [52] MOFs 1-6 300 W Xe lamp, UV- visible light 4.35 — — [53] TiO2/C@MOF 300 W Xe lamp, UV- visible light 28.60 — — [54] MOF-525- Co 300 W Xe lamp, UV- visible light 200.60 36.67 — [55] UiO-66/CNSS 300 W Xe lamp, UV- visible light 9.00 — — [56] NH2-MIL-101(Fe) 300 W Xe lamp, UV- visible light — — HCOO: 178 [57] Ren-MOF 300 W Xe lamp, UV- visible light 6.37 — — [58] ZIF-67 300 W Xe lamp, UV- visible light 37.40 — — [59] Layered double hydroxide materials Co-Co LDHs/Ti3C2Tx CO2, MeCN/H2O/TEOA and
[Ru(bpy)3]Cl2 6H2O under 5 W LED lamp1.25×104 — — [60] Niln-LDH/In2S3 300 W Xe lamp, UV- visible light 88.29 — [61] Ni-Zr-Al 300 W Xe lamp, UV- visible light — 150 mL·g−1·h−1 — [62] Mg-Al 300 W Xe lamp, UV- visible light; 350 °C 12.60 — — [63] NiAl-LDH/CdS 300 W Xe lamp, UV- visible light 12.45 — — [64] -
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