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Unassisted photoelectrochemical CO₂-to-liquid fuel splitting over 12% solar conversion efficiency.

ABSTRACT: The increasing need to control anthropogenic CO₂ emissions and conversion to fuels features the necessity for innovative solutions, one of which is photoelectrochemical system. This approach, capable of yielding gaseous production progressively, is facing challenges for liquid fuels generation due to optical, electrical, and catalytic properties. This study employs a standalone photoelectrochemical setup, in which InGaP/GaAs/Ge photoanode is integrated with tin-modified bismuth oxide cathode to convert CO₂ into liquid formic acid. In unassisted two-electrode assembly, setup exemplifies its operational durability for 100 h, during which it maintains an average Faradaic efficiency of 88% with 17.3 mmol L^-1 h^-1 of yield, thereby excelling in average solar-to-fuel conversion efficiency at 12% with 60% of electrical energy efficiency under one sun illumination. This significant performance is further associated with metal-semiconductor interface formation between tin and bismuth oxide, which bridges electronic structures and generates an electric field at their interfaces. This study outperforms conventional solar-driven systems in operational durability and liquid fuel production.

SUBMITTER: Khan B

PROVIDER: S-EPMC11324881 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature

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Unassisted photoelectrochemical CO<sub>2</sub>-to-liquid fuel splitting over 12% solar conversion efficiency.

Khan Bilawal B Faheem M Bilal MB Peramaiah Karthik K Nie Jinlan J Huang Hao H Li Zhongxiao Z Liu Chen C Huang Kuo-Wei KW He Jr-Hau JH

Nature communications 20240814 1

The increasing need to control anthropogenic CO<sub>2</sub> emissions and conversion to fuels features the necessity for innovative solutions, one of which is photoelectrochemical system. This approach, capable of yielding gaseous production progressively, is facing challenges for liquid fuels generation due to optical, electrical, and catalytic properties. This study employs a standalone photoelectrochemical setup, in which InGaP/GaAs/Ge photoanode is integrated with tin-modified bismuth oxide ...[more]

PMID: 39143057

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Project description:Biochemical networks use reaction cascades to selectively reduce CO2 using energy from sunlight, but can similar selectivity be achieved by applying a cascade approach to an engineered system? Here, we report the design and implementation of a two-step photoelectrochemical (PEC) cascade to a liquid solar fuel: reduction of CO2 to CO and subsequent reduction of CO to methanol. The potentials required to perform the reductions were generated using custom-made III-V-based three-terminal tandem (3TT) solar cells. Cobalt phthalocyanine immobilized on multiwalled carbon nanotubes (CoPc/MWCNT) catalyzed both reactions. Multiphysics simulations of electrolyte flow and nonilluminated electrochemical measurements were used to narrow the operating parameters for the CoPc/MWCNT 3TT photocathodes. The champion integrated photocathode produced methanol with 3.8 ± 0.4% Faradaic efficiency (FE), with tested photocathodes having 0.7-3.8% methanol FE. Products were quantified by nuclear magnetic resonance spectroscopy and gas chromatography. The current output of the tested photocathodes was highly stable, and methanol production continued over multiple experiments. The low methanol yield is attributed to insufficient CO flux to, and CO2 depletion at, the methanol-producing subcell when both contacts are active, which is supported by the observation that a control photoelectrode slightly outperformed the methanol production of the 3TT device. Methanol production ceased when the 3TT subcell driving CO reduction was deactivated, supporting the assignment of a cascade mechanism. The major factors resulting in low methanol FE by the CoPc/MWCNT 3TT photocathodes are insufficient CO2 depletion at the methanol-producing contact and uncertainty in operating potential selection using the 3TT design. Although the CoPc/MWCNT 3TT photocathode is not yet highly selective, this work develops the basic science principles underlying the PEC cascade, demonstrates the co-design of a 3TT-based photoelectrode to produce carbon-based fuels, and finally discusses routes for improving product yields with this concept, including CO2 supply optimization and alternative photoelectrode and catalyst materials.

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Unassisted photoelectrochemical CO₂-to-liquid fuel splitting over 12% solar conversion efficiency.

Publications

Unassisted photoelectrochemical CO<sub>2</sub>-to-liquid fuel splitting over 12% solar conversion efficiency.

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Dataset Information

Unassisted photoelectrochemical CO2-to-liquid fuel splitting over 12% solar conversion efficiency.

Publications

Unassisted photoelectrochemical CO<sub>2</sub>-to-liquid fuel splitting over 12% solar conversion efficiency.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

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Unassisted photoelectrochemical CO₂-to-liquid fuel splitting over 12% solar conversion efficiency.