Recent advances in the built-in electric-field-assisted photocatalytic dry reforming of methane

doi:10.1016/S1872-2067(23)64520-6

Chinese Journal of Catalysis ›› 2023, Vol. 53: 72-101.DOI: 10.1016/S1872-2067(23)64520-6

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Recent advances in the built-in electric-field-assisted photocatalytic dry reforming of methane

Yiming Lei^a^,^b, Jinhua Ye^c, Jordi García-Antón^b^,^*(), Huimin Liu^a^,^*()

^aSchool of Chemical and Environmental Engineering, Liaoning University of Technology, Jinzhou 121001, Liaoning, China
^bDepartament de Química (Unitat de Química Inorgànica), Facultat de Ciències, Universitat Autònoma de Barcelona (UAB), Cerdanyola del Valles, 08193 Barcelona, Spain
^cInternational Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, 305-0044 Ibaraki, Japan

Received:2023-07-03 Accepted:2023-09-08 Online:2023-10-18 Published:2023-10-25
Contact: E-mail: iuhuimin08@tsinghua.org.cn (H. Liu), Jordi.GarciaAnton@uab.es (J. García-Antón).
About author:Jordi García-Antón received his Ph.D. in Chemistry in 2003 from the Universitat Autònoma de Barcelona (UAB). Then, he pursued a postdoctoral stay at the Laboratoire de Chimie de Coordination (Dr. Chaudret group; Toulouse, France), where his work dealt with the synthesis and characterization of metallic nanoparticles and the study of their surface coordination chemistry. In 2006, Dr. García‐Antón joined the UAB as a lecturer in chemistry, and in 2014 he became an associate professor. His research interest focuses on the preparation of metallic or metal‐oxide nanoparticles through the organometallic approach and their use as (photo)catalysts in artificial photosynthesis processes.
Huimin Liu is a professor at Liaoning University of Technology in the School of Chemical and environmental engineering. She received her Ph.D. degree from Tsinghua University, China (2013), and then joined Kansai University (2013-2014), National Institute for Materials Science (2014-2017), and University of Sydney (2017) as a post-doctoral researcher. Her research interests are photochemistry, environmental chemistry, and heterogeneous catalyst design.
Supported by:
The National Natural Science Foundation of China(21902116);Scientific Research Foundation of Technology Department of Liaoning Province of China(2022-MS-379);The Spanish Ministry of Science and Innovation(MICINN);The Spanish Ministry of Science and Innovation(PID2019-104171RB-I00);The Spanish Ministry of Science and Innovation(TED2021-129237B-I00);China Scholarship Council(CSC);China Scholarship Council(202206250016)

Abstract

Abstract:

Methane (CH₄) and carbon dioxide (CO₂) are two major greenhouse gases that contribute to global warming. The dry reforming of methane (DRM) is an ideal method for dealing with the greenhouse effect because it simultaneously consumes CH₄ and CO₂ to produce syngas. However, conventional technologies require high temperatures to trigger the DRM process owing to the high energy barriers associated with activating CH₄ and CO₂. While the development of photocatalysts provides opportunities for initiating the DRM under mild conditions, photocatalytic efficiency nonetheless remains unsatisfactory, which is largely attributable to rapid photoexcited charge-carrier recombination. A promising strategy for overcoming this deficiency involves constructing a built-in electric field that enhances the separation and transfer dynamics of charge carriers. This review introduces reaction mechanisms and thermal catalysts for DRM applications. The advantages of photocatalytic DRM (PDRM) and potential photocatalysts are also summarized. Recent advances have enhanced PDRM by introducing electric fields through the fabrication of photocatalysts that exhibit ferroelectric effects (ferroelectric-based photocatalysts), have heterojunction structures, or undergo localized surface plasmon resonance (LSPR). In addition, significant advanced in-situ-characterization studies and theoretical calculations are introduced along with their potential impact to provide young researchers engaged in the PDRM field with simple guidance. Finally, current challenges facing the built-in electric-field-assisted PDRM field are discussed and possible strategies proposed to encourage more in-depth research in this area.

Key words: Photocatalytic dry reforming of methane, Built-in electric field, Ferroelectric materials, Heterojunction photocatalyst, Localized surface plasmon resonance effect

Yiming Lei, Jinhua Ye, Jordi García-Antón, Huimin Liu. Recent advances in the built-in electric-field-assisted photocatalytic dry reforming of methane[J]. Chinese Journal of Catalysis, 2023, 53: 72-101.

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Figures/Tables 26

Fig. 1. (a) Fundamental steps involved in photocatalysis. Step 1: exciting the charge-carrier; Step 2: electron/hole separation/transfer; Step 3: reduction and oxidation reactions. (b) Spontaneous polarization in a ferroelectric material induces a built-in electric field that promotes the separation of photoexcited carriers and their reactions. (c) Type-II heterojunction photocatalyst. (d) Direct Z-scheme heterojunction photocatalyst. (e) Schematic depicting plasmon oscillation on a plasmonic metal sphere. (f) Number of publications according to “Web of Science” acquired by searching the keyword: “photocatalysis” with “electric field” or “heterojunction” between 2000 and 2022.

Fig. 2. Schematic depicting the PDRM reaction over a semiconductor-based photocatalyst.

Fig. 3. CH4- and CO2-activation steps in the DRM reaction: (a) Dissociative adsorption of CH4 and desorption of H2. (b) Adsorption of CO2 on the metal, metal-support interface, and support, and the direct formation and desorption of CO.

Fig. 4. (a) Two-dimensional volcano plot of turnover frequency (log10) as functions of O- and C-adsorption energies. T = 500 °C, P = 1 bar; 10% conversion. Error bars include estimated 0.2 eV uncertainties in adsorption energy. Reprinted with permission from Ref. [64]. Copyright 2008, Elsevier. (b) CO2 conversions as functions of time on stream (700 °C) [58]. Reprinted with permission from Ref. [58]. Copyright 2011, Elsevier.

Fig. 5. (a) Energy band structure of various TiO2 samples. Here, the band structure is drawn with respect to the top edge of the VB of TiO2 ST-01 for comparison [72]. Reprinted with permission from Ref. [72] Copyright 2022, Elsevier. (b) Quantum efficiencies (QEs) as functions of temperature (T) [74]. Reprinted with permission from Ref. [74]. Copyright 2016, American Chemical Society.

Fig. 6. Production rates (a) and light-to-fuel efficiencies (b) of CRM catalysts under focused full solar spectrum light from a Xe lamp. (c) Diffusive reflectance absorption spectra of Pt/CeO2-MNR. Reprinted with permission from Ref. [84]. Copyright 2018, Royal Society of Chemistry.

Fig. 7. (a-d) HAADF-STEM elemental-distribution maps for the Cu-Ni-11@CN catalyst. (e) Comparing the amounts of CO2-reduction products over the synthesized catalysts after 5 h of irradiation with light. (f) Reusability testing CH4 generation over the Cu-Ni-11@CN catalyst. Reprinted with permission from Ref. [94]. Copyright 2022 Elsevier B.V.

Fig. 8. (a) Diffusive reflectance spectrum of hm-Ni/Al2O3. (b) Specific H2- and CO-production rates for light-driven catalytic DRM on the samples when illuminated by concentrated UV-vis-IR light (345.6 kW m?2). Reprinted with permission from Ref. [102]. Copyright 2023 Wiley.

Fig. 10. (a) PL spectra of BaTiO3, Fe2O3, and BaTiO3/Fe2O3 with various molar ratios. (b) Efficiencies of various photocatalysts used to reduce CO2 within 4 h. (c) Comparing the photocatalytic performance of the BF31 heterojunction with a physical mixture of BaTiO3 and Fe2O3 with the same molar ratio. Reprinted with permission from Ref. [126]. Copyright 2019, Springer Nature.

Fig. 11. (a) CBED pattern of TaN, which provides asymmetric contrast between (0001) and (0001) diffraction spots that reveals the polarity of the (0001) plane for a non-symmetric crystal structure, such as TaN in the P-62m space group. Catalytic performance of Pt/ZrN (b) and Pt/TiN (c) for the DRM under various reaction conditions. Reprinted with permission from Ref. [127]. Copyright 2018, Wiley.

Fig. 12. Schematic illustrating charge-carrier transfer in a type-I heterojunction with a straddling gap structure (a), a type-II heterojunction with a staggered gap structure (b), and a type-III heterojunction with a broken gap structure (c).

Fig. 13. (a) UV-vis spectra of TiO2, g-C3N4, Ti3AlC2, Ti3C2 24 H 39, Ti3C2 96 H 49, and CN/TCT. (b) PL spectra of TiO2, Ti3C2 24 H 39, Ti3C2 24 H 49, Ti3C2 96 H 39, Ti3C2 96 H 49, and CN/TCT. Photocatalytic production of CO (c) and H2 (d) by Ti3C2 24 H 39, Ti3C2 24 H 49, Ti3C2 96 H 39, Ti3C2 96 H 49, and CN/TCT. (e) Schematic showing the PDRM toward CO and H2 by the CN/TCT photocatalyst. Reprinted with permission from Ref. [144]. Copyright 2021, Elsevier.

Sample	Bandgap (eV)	Valance band (eV)	Conduction band (eV)
g-C₃N₄	2.83	1.47	−1.36
TiO₂ anatase	3.2	2.70	−0.50
TiO₂ rutile	3.1	2.81	−0.29
CN/TCT	2.86	1.57	−1.29

Fig. 14. Schematic depicting charge-carrier transfer in a conventional Z-scheme photocatalyst (A and D stand for electron acceptor and donor, respectively) (a), an all-solid-state Z-scheme photocatalyst (b), and a direct Z-scheme photocatalyst (c).

Fig. 15. Ex-situ and in-situ high-resolution Ti 2p (a), O 1s (b), C 1s (c), and N 1s (d) XPS spectra. (e) PL emission spectra of g-C3N4, TiO2/g-C3N4, and (25)TiO2-TiC/g-C3N4(400). (f) CO2-photoreduction performance of g-C3N4, TiO2-TiC, TiO2/g-C3N4, and (25)TiO2-TiC/g-C3N4(400). Reaction conditions: P = 40 kPa; CH4:CO2 = 1:2; ambient temperature. Reprinted with permission from Ref. [149]. Copyright 2022, Royal Society of Chemistry (RSC).

Fig. 16. Comparative performance of CoAl-LDH, g-C3N4, Ti3AlC2, CoAl-LDH/g-C3N4, and CoAl-LDH/g-C3N4/Ti3AlC2 for syngas production using the PDRM process: CO (a) and H2 (b) production (a = g-C3N4, b = CoAl-LDH, c = Ti3AlC2, d = 5% CoAl-LDH/g-C3N4, e =?10% CoAl-LDH/g-C3N4, f = 15% CoAl-LDH/g-C3N4, g=?25% CoAl-LDH/g-C3N4, and h?=?15% CoAl-LDH-15% Ti3AlC2/g-C3N4). Comparing the performance of the CoAl-LDH/g-C3N4/Ti3AlC2 composite in PDRM and PBRM processes: CO (c) and H2 (d) production. Reprinted with permission from Ref. [151]. Copyright 2023, Elsevier.

Fig. 17. Schematic depicting the three mechanisms responsible for enhancing plasmonic materials: (i) light absorption and scattering, (ii) hot-electron injection, and (iii) PIRET. Reprinted with permission from Ref. [165]. Copyright 2015, Wiley.

Fig. 18. (a,c) Acquired photocurrent enhancement spectra (black symbols) and electromagnetic simulations (blue lines). (b,d) Full-field electromagnetic simulations of the plasmon-enhanced absorption in a probe region near the Au particle and at the H2O/Fe2O3 interface, which predict strong enhancements near the surface plasmon resonance. The dashed white lines indicate the surface plasmon resonance wavelength for a 50-nm Au nanoparticle located on top of or embedded in semi-infinite Fe2O3, respectively. Reprinted with permission from Ref. [170]. Copyright 2011, American Chemical Society (ACS). (e) H2 and O2 production upon illuminating N-TiO2 (black symbols) and Ag/N-TiO2 (blue symbols) photocatalysts with visible light, as determined by mass spectrometry. (f) Photocurrent responses (per macroscopic electrode area) upon illumination with a broadband visible-light source (400-900 nm). (g) Average electric field enhancement around a Ag cube with a 120-nm edge length as a function of the distance d from the cube, calculated using FDTD simulations. Inset: Local enhancement of the electric field calculated from an FDTD simulation of a 120-nm Ag cube in water. Reprinted with permission from Ref. [173]. Copyright 2011, American Chemical Society (ACS).

Fig. 19. (a) Specific activities over different amounts of Ag-containing composites under simulated solar light. (b) Photocatalytic CO2- and CH4-reformation performance: effect of the light source (visible light, simulated sunlight, and ultraviolet light) over 1%Ag/TiO2 as the catalyst. High-resolution Ag XPS spectra before (c), after (d) reaction under visible light, after reaction under simulated solar light (e), and after irradiation with ultraviolet light (f). Reprinted with permission from Ref. [176]. Copyright 2019, American Chemical Society (ACS). FDTD-simulated spatial distributions of electric field intensity enhancements at wavelengths of 350 and 530 nm: (g,h) Pt/SiO2, (i,j) Au/SiO2, and (k,l) Pt-Au/SiO2. Reprinted with permission from Ref. [177]. Copyright 2018, American Chemical Society (ACS).

Fig. 20. In-situ QXANES spectra recorded during H2-TPR (10?°C min-1, up to 800 °C, for 30 min) of as-prepared 8Ni5Fe/MgAl2O4 at the Fe K edge (a) and the Ni K edge (b). In-situ Fe K edge QXANES spectra recorded during DRM (750 °C, 1 atm, 30 min) of reduced 8Ni5Fe/MgAl2O4 with CH4/CO2 =? 1/2 (c), 1/1.5 (d) and 1/1 (e). Solid lines: experimental spectra; dashed lines: reference spectra; bold arrows highlight spectral evolution during the DRM. Reprinted with permission from Ref. [183]. Copyright 2021, Elsevier.

Fig. 21. In-situ XPS spectra of Ni-Si/ZrO2 and Ni-Zr/SiO2 catalysts after reduction using flowing mixtures of H2 and Ar (F(H2) = F(Ar) = 30 mL min-1 at 450 °C), and CH4 and CO2 (F(CH4) = F(CO2) = 30 mL min-1 at 400 °C): Ni 2p (a,b), Zr 3d (c,d), and O 1s (e,f) for Ni-Si/ZrO2 (a-c) and Ni-Zr/SiO2 (d-f). Reprinted with permission from Ref. [186]. Copyright 2018, American Chemical Society.

Fig. 22. (a) Cobalt-containing-phase weight fractions as functions of temperature during H2-TPR on a 10 wt% Co-CeO2 catalyst. (b) Sequential in-situ XRD patterns acquired during H2-TPR on a 10 wt% Co-CeO2 catalyst. Reprinted with permission from Ref. [191] Copyright 2018, American Chemical Society.

Fig. 23. In-situ DRIFTS spectra acquired in dark DRM reactions on Pt-Ce (a) and Pt-Al-Ce (c). Dark-light comparisons on Pt-Ce (b) and Pt-Al-Ce (d). Reprinted with permission from Ref. [195]. Copyright 2022 Royal Society of Chemistry.

Table 2 State-of-the-art thermal-/photo(thermal)-catalysts for the DRM reaction, including product-evolution rates and specific reaction conditions.

Catalyst	Type	Reaction condition	Catalytic performance	Ref.
Rh-Ni/Al₂O₃	thermal catalyst	catalyst: 100 mg, total gas flow rate: 0.83 N cm³ s⁻¹, gas hourly space velocity (GHSV) = 6000 h⁻¹_, CH₄/CO₂/He = 20/20/60, temperature: 699.85 °C pressure: 1 atm	CO₂ conversion: ~85% CH₄ conversion: ~65% H₂/CO: ~0.85	[58]
Pt/CeO₂	photocatalyst	catalyst: 50 mg, light source: 500 W Xe lamp, total gas flow rate: 120.5 mL min⁻¹, CH₄/CO₂/Ar = 10/10/80	units: mmol min⁻¹ g⁻¹, CO₂ conversion: ~3.2 CH₄ conversion: ~2.7 H₂: 5.7 CO: 6.0	[83]
BaZr_0.05Ti_0.95O₃	ferroelectric non-thermal plasmonic catalyst	catalyst: 0.5 g, DC pulse voltage: 13 kV frequency = 20000 Hz, discharge gap = 5 mm, total gas flow rate: 100 mL min⁻¹, GHSV: 8500 h⁻¹, CH₄/CO₂ = 1/1	CO₂ conversion: 79.0% conversion CH₄ conversion: 84.2% H₂ selectivity: 87.5% CO selectivity: 69.2%	[124]
BaTiO₃/Fe₂O₃	ferroelectric photocatalyst	Hg lamp 125 W, CO₂/CH₄/He = 45/45/10 pressure: 40 pa, temperature: 30 ± 5 °C	CO₂ conversion: 22.3%
Pt/TaN	ferroelectric photocatalyst	catalyst: 0.10 g, light source: Xe lamp, total flow rate: 20.0 mL/min, CH₄/CO₂ = 1/1, temperature: 500 °C	units :μmol min⁻¹ g⁻¹, CO₂ conversion: ~700 CH₄ conversion: ~550 H₂: 1100, CO: 1200	[126]
Ti₃C₂/TiO₂/g-C₃N₄	type-II heterojunction photocatalyst	catalyst: 100 mg, light source: 35 W Xenon lamp, light intensity: 20 mW cm⁻², CO₂/CH₄: 2/1 (10/5 mL min⁻¹), pressure: 0.10 bar	unit: μmol g⁻¹ h⁻¹, H₂: 45.69 CO: 87.34, CO selectivity: 65.6% H₂ selectivity: 34.40%	[143]
TiO₂-TiC/g-C₃N₄	all-solid-state Z-scheme heterojunction photocatalyst	catalyst: 50 mg, light source: Xe lamp, light intensity: 335 mW cm⁻², pressure: 40 kPa CH₄ /CO₂ = 1/2, temperature: room temperature	units: μmol g⁻¹ h⁻¹ CO: 11.3 H₂: 2.15	[148]
CoAl-LDH/g-C₃N₄/Ti₃AlC₂	direct Z-scheme heterojunction photocatalyst	catalyst: 100 mg, light source: 35 W Xe lamp, light intensity: 20 mW cm⁻², total flow rate: 20 mL min⁻¹, CH₄ /CO₂ = 1/1, pressure: 0.3 bar	units: μmol g⁻¹ h⁻¹ CO: 22.5 H₂: 4.74	[150]
Ag/TiO₂	plasmonic photocatalyst	catalyst: 100 mg, light source: Xe lamp, light intensity: 84.2 mW cm⁻², CO₂/CH₄/Ar = 7.5/7.5/85, pressure: 2 MPa	units: μmol g⁻¹ h⁻¹ CO: 1149 C₂H₄: 686	[175]
Pt/Au-SiO₂	plasmonic photocatalyst	catalyst: 20 mg, light source: Xe lamp, total flow rate: 20.0 mL min^-1, CO₂/CH₄ = 1/1	units: μmol g⁻¹ h⁻¹, CO₂ conversion: ~68.6 CH₄ conversion: ~55.0, CO: ~120 H₂: ~90	[176]

Table 2 State-of-the-art thermal-/photo(thermal)-catalysts for the DRM reaction, including product-evolution rates and specific reaction conditions.

Catalyst	Type	Reaction condition	Catalytic performance	Ref.
Rh-Ni/Al₂O₃	thermal catalyst	catalyst: 100 mg, total gas flow rate: 0.83 N cm³ s⁻¹, gas hourly space velocity (GHSV) = 6000 h⁻¹_, CH₄/CO₂/He = 20/20/60, temperature: 699.85 °C pressure: 1 atm	CO₂ conversion: ~85% CH₄ conversion: ~65% H₂/CO: ~0.85	[58]
Pt/CeO₂	photocatalyst	catalyst: 50 mg, light source: 500 W Xe lamp, total gas flow rate: 120.5 mL min⁻¹, CH₄/CO₂/Ar = 10/10/80	units: mmol min⁻¹ g⁻¹, CO₂ conversion: ~3.2 CH₄ conversion: ~2.7 H₂: 5.7 CO: 6.0	[83]
BaZr_0.05Ti_0.95O₃	ferroelectric non-thermal plasmonic catalyst	catalyst: 0.5 g, DC pulse voltage: 13 kV frequency = 20000 Hz, discharge gap = 5 mm, total gas flow rate: 100 mL min⁻¹, GHSV: 8500 h⁻¹, CH₄/CO₂ = 1/1	CO₂ conversion: 79.0% conversion CH₄ conversion: 84.2% H₂ selectivity: 87.5% CO selectivity: 69.2%	[124]
BaTiO₃/Fe₂O₃	ferroelectric photocatalyst	Hg lamp 125 W, CO₂/CH₄/He = 45/45/10 pressure: 40 pa, temperature: 30 ± 5 °C	CO₂ conversion: 22.3%
Pt/TaN	ferroelectric photocatalyst	catalyst: 0.10 g, light source: Xe lamp, total flow rate: 20.0 mL/min, CH₄/CO₂ = 1/1, temperature: 500 °C	units :μmol min⁻¹ g⁻¹, CO₂ conversion: ~700 CH₄ conversion: ~550 H₂: 1100, CO: 1200	[126]
Ti₃C₂/TiO₂/g-C₃N₄	type-II heterojunction photocatalyst	catalyst: 100 mg, light source: 35 W Xenon lamp, light intensity: 20 mW cm⁻², CO₂/CH₄: 2/1 (10/5 mL min⁻¹), pressure: 0.10 bar	unit: μmol g⁻¹ h⁻¹, H₂: 45.69 CO: 87.34, CO selectivity: 65.6% H₂ selectivity: 34.40%	[143]
TiO₂-TiC/g-C₃N₄	all-solid-state Z-scheme heterojunction photocatalyst	catalyst: 50 mg, light source: Xe lamp, light intensity: 335 mW cm⁻², pressure: 40 kPa CH₄ /CO₂ = 1/2, temperature: room temperature	units: μmol g⁻¹ h⁻¹ CO: 11.3 H₂: 2.15	[148]
CoAl-LDH/g-C₃N₄/Ti₃AlC₂	direct Z-scheme heterojunction photocatalyst	catalyst: 100 mg, light source: 35 W Xe lamp, light intensity: 20 mW cm⁻², total flow rate: 20 mL min⁻¹, CH₄ /CO₂ = 1/1, pressure: 0.3 bar	units: μmol g⁻¹ h⁻¹ CO: 22.5 H₂: 4.74	[150]
Ag/TiO₂	plasmonic photocatalyst	catalyst: 100 mg, light source: Xe lamp, light intensity: 84.2 mW cm⁻², CO₂/CH₄/Ar = 7.5/7.5/85, pressure: 2 MPa	units: μmol g⁻¹ h⁻¹ CO: 1149 C₂H₄: 686	[175]
Pt/Au-SiO₂	plasmonic photocatalyst	catalyst: 20 mg, light source: Xe lamp, total flow rate: 20.0 mL min^-1, CO₂/CH₄ = 1/1	units: μmol g⁻¹ h⁻¹, CO₂ conversion: ~68.6 CH₄ conversion: ~55.0, CO: ~120 H₂: ~90	[176]

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Recent advances in the built-in electric-field-assisted photocatalytic dry reforming of methane

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