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Silicon photocathode functionalized with osmium complex catalyst for selective catalytic conversion of CO₂ to methane.

ABSTRACT: Solar-driven CO₂ reduction to yield high-value chemicals presents an appealing avenue for combating climate change, yet achieving selective production of specific products remains a significant challenge. We showcase two osmium complexes, przpOs, and trzpOs, as CO₂ reduction catalysts for selective CO₂-to-methane conversion. Kinetically, the przpOs and trzpOs exhibit high CO₂ reduction catalytic rate constants of 0.544 and 6.41 s^-1, respectively. Under AM1.5 G irradiation, the optimal Si/TiO₂/trzpOs have CH₄ as the main product and >90% Faradaic efficiency, reaching -14.11 mA cm^-2 photocurrent density at 0.0 V_RHE. Density functional theory calculations reveal that the N atoms on the bipyrazole and triazole ligands effectively stabilize the CO₂-adduct intermediates, which tend to be further hydrogenated to produce CH₄, leading to their ultrahigh CO₂-to-CH₄ selectivity. These results are comparable to cutting-edge Si-based photocathodes for CO₂ reduction, revealing a vast research potential in employing molecular catalysts for the photoelectrochemical conversion of CO₂ to methane.

SUBMITTER: Li XY

PROVIDER: S-EPMC11246507 | biostudies-literature | 2024 Jul

REPOSITORIES: biostudies-literature

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Silicon photocathode functionalized with osmium complex catalyst for selective catalytic conversion of CO2 to methane.

Li Xing-Yi XY Zhu Ze-Lin ZL Dagnaw Fentahun Wondu FW Yu Jie-Rong JR Wu Zhi-Xing ZX Chen Yi-Jing YJ Zhou Mu-Han MH Wang Tieyu T Tong Qing-Xiao QX Jian Jing-Xin JX

Nature communications 20240713 1

Solar-driven CO2 reduction to yield high-value chemicals presents an appealing avenue for combating climate change, yet achieving selective production of specific products remains a significant challenge. We showcase two osmium complexes, przpOs, and trzpOs, as CO2 reduction catalysts for selective CO2-to-methane conversion. Kinetically, the przpOs and trzpOs exhibit high CO2 reduction catalytic rate constants of 0.544 and 6.41 s-1, respecti ...[more]

PMID: 39003268

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Project description:The effect of the phase transformation of a FePO4 catalyst material from the tridymite-like (tdm) FePO4 to the α-domain (α-Fe3(P2O7)2) during the direct selective oxidation of methane to methanol was studied using oxidant species O2, H2O and N2O. The main reaction products were CH3OH, carbon dioxide and carbon monoxide, whereas formaldehyde was produced in rather minute amounts. Results showed that the single-step non-syngas activation of CH4 to oxygenate(s) on a solid FePO4 phase-specific catalyst was influenced by the nature of the oxidizer used for the CH4 turnover. Fresh and activated FePO4 powder samples and their modified physicochemical surface and bulk properties, which affected the conversion and selectivity in the partial oxidation (POX) mechanism of CH4, were investigated. Temperature-programmed re-oxidation (TPRO) profiles indicated that the type of moieties utilised in the procedures, determined the re-oxidizing pathway of the reduced multiphase FePO4 system. Mössbauer spectroscopy measurements along with X-ray diffraction (XRD) examination of neat, hydrogenated and spent catalytic compounds, demonstrated a variation of the phosphate into a mixture of crystallites, which depended on operating process conditions (for example time-on-stream). The Mössbauer spectra revealed the change of the initial ferric orthophosphate, FePO4 (tdm), to the divalent metal form, iron(ii) pyrophosphate (Fe2P2O7); thereafter, reactivity was governed by the interaction (strength) with individual oxidizing agents. The Fe3+ ↔ Fe2+ chemical redox cycle can play a key mechanistic role in tailored multistep design, while the advantage of iron-based heterogeneous catalysis primarily lies in being inexpensive and comprising non-critical raw resources. When compared to the other catalysts reported in the literature, the FePO4-tdm phase catalysts showed in this work exhibited a high activity towards methanol i.e., 12.3 × 10-3 μmolMeOH gcat h-1 using N2O as an oxidant. This catalyst also showed a high activity with O2 as an oxidant (5.3 × 10-3 μmolMeOH gcat h-1). Further investigations will include continuous reactor unit engineering optimisation.

Dataset Information

Silicon photocathode functionalized with osmium complex catalyst for selective catalytic conversion of CO₂ to methane.

Publications

Silicon photocathode functionalized with osmium complex catalyst for selective catalytic conversion of CO<sub>2</sub> to methane.

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