Photo-thermal cooperation for the conversion of CO2 and CH4 with H2O to C2 oxygenates over SrTiOx supported CuCo

doi:10.1016/S1872-2067(24)60026-4

Abstract

Abstract:

Photosynthesis is a potential strategy to enable endergonic process that usually needs high-temperature in thermochemistry to supply the energy for inert-bond activation and/or strong endothermic reaction. The conversion of CO₂ into value-added C₂-oxygenates is a promising process to realize artificial photosynthesis, but suffers from relatively lower efficiency due to complex multi-electron (≥ 10) transfer processes and sluggish kinetics of C-C coupling. This work proposes an all-new H₂O-promoted strategy for efficient production of C₂ oxygenates from the concurrent activation and subsequent co-conversion of CO₂ with CH₄ under photo-thermal cooperation, in which photocatalytic H₂O-splitting derived active hydrogen species for CO₂ activation, and concomitant active oxygen species for CH₄ activation. A formation rate of as high as 2.05 mmol g^-1 h^-1 for C₂-oxygenates (CH₃CHO and CH₃CH₂OH) in a selectivity of > 86% has been afforded over SrTiO_x supported CuCo under 200 °C and ultraviolet-visible illumination. It has been revealed that SrTiO_x drives photocatalytic H₂O-splitting under the excitation primary from ultraviolet light, paired Cu^I/Cu⁰ sites promote the formation of *CH_xO intermediate from CO₂, Co sites conduct CH₄-to-*CH₃, and C-C coupling of *CH_xO and *CH₃ on adjacent Cu-Co facilitates the generation of C₂-oxygenates.

Key words: Photo-thermal cooperation, Co-conversion of CO₂ and CH₄, SrTiO_x supported Cu-Co, Water-splitting, C₂-oxygenates

Yanru Zhu, Zhijun Zhang, Jian Zhang, Shuangjiang Jiang, Zhe An, Hongyan Song, Xin Shu, Wei Xi, Lirong Zheng, Jing He. Photo-thermal cooperation for the conversion of CO₂ and CH₄ with H₂O to C₂ oxygenates over SrTiO_x supported CuCo[J]. Chinese Journal of Catalysis, 2024, 61: 164-178.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60026-4

https://www.cjcatal.com/EN/Y2024/V61/I6/164

Figures/Tables 7

Fig. 1. Illustration of conversion of CO2 and CH4 with H2O splitting derived oxygen and hydrogen species to produce CH3CHxO (X = 1 or 3) over SrTiOx supported heterojunction Cu-Co.

Fig. 2. (a) Schematic illustration for the preparation of SrTiOx (SrTiOx) supported Cu-Co. TEM image with particle size distributions inserted (b), HR-TEM image (c), and EDX element mapping analysis (d) of Cu0.10-Co-SrTiOx. Fourier-transform of the k3-weighted EXAFS spectra (e,f) and normalized XANES spectra (g,h) for Co K-edge and Cu K-edge.

Fig. 3. Conversion of CO2 with H2O. CO2 conversion rates (A) and product formation rates (B) in the conversion of CO2 with H2O on Cu0.10-Co1-SrTiOx, Co-SrTiOx, Cu-SrTiOx, and SrTiOx at 80 °C under illumination (300 W Xe-lamp). FT-IR spectra recorded activation of CO2 at 80 °C in dark or light, with or without H2O, and with Ar purge followed by H2 exposure on Cu0.10-Co1-SrTiOx in range of 3100-2700 cm-1 (C) and 2150-2050 cm-1 (D). (E) Variation of C2 oxygenates formation rates with CuI/Cu0 ratio and the normalized CHxO formation rate (CHxO formation rate/CO2 conversion rate) with CuI/Cu0 ratio on Cu-Co-SrTiOx in the conversion of CO2 with H2O at 80 °C under illumination.

Fig. 4. Conversion of CH4 with H2O and CO2+CH4 with H2O. (A) Product formation rates in the conversion of CH4 with H2O on Cu0.10-Co1-SrTiOx, Co-SrTiOx, Cu-SrTiOx, and SrTiOx. (B) FT-IR spectra recorded activation of CH4 on Cu0.10-Co1-SrTiOx. (C-F) Conversion of CO2 and CH4 with H2O. (C) Product formation rates on Cu0.10-Co1-SrTiOx, Co-SrTiOx, Cu-SrTiOx, and SrTiOx. (D) Product formation rates on Cu0.10-Co1-SrTiOx under varied conditions. (E) Product formation rates on Cu0.02-Co1-SrTiOx at varied temperatures. (F) Variation of CH3CH2OH/CH3CHO and H2 production rate with reaction temperatures on Cu0.02-Co1-SrTiOx under illumination. Reactions in (A) and (C) were performed at 80 °C under illumination (300 W Xe-lamp).

Fig. 5. Photo-thermal cooperation to decrease the reaction temperature and activation energy. Reaction temperature and activation energy of CO2 and CH4 with H2O with photo-thermal cooperation in this work, and the data in similar thermocatalysis reactions reported [69???-73] in the literatures.

Fig. 6. Mass spectrometry results of the reaction products of isotopically labeled CH4+CO2 with H2O using CD4 (A), 13CO2 (B), D2O (C), or H218O (D) on Cu0.10-Co1-SrTiOx; (left) liquid products, (middle) gaseous products, and (right) proposed reaction pathways. Reaction conditions: 80 °C, 4 h, 300 W Xe-lamp. (E) Summarized reaction network of CH4+CO2 with H2O.

Fig. 7. Illustrations of reaction mechanism for the coupling of CO2 and CH4 with H2O on adjacent Cu-Co supported on SrTiOx.

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Photo-thermal cooperation for the conversion of CO₂ and CH₄ with H₂O to C₂ oxygenates over SrTiO_x supported CuCo

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