Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation

Liu, Bin; Qian, Zheng; Shi, Xiang; Su, Haoqing; Zhang, Wentao; Kludze, Atsu; Zheng, Yuze; He, Chengxing; Yanagi, Rito; Hu, Shu

doi:10.1038/s41467-025-56106-3

Title: Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation

Journal Article · 11 February 2025 · Nature Communications

DOI: https://doi.org/10.1038/s41467-025-56106-3 · OSTI ID:2515684

Liu, Bin; Qian, Zheng; Shi, Xiang; Su, Haoqing;

;

; Zheng, Yuze;

; Yanagi, Rito;

Abstract The direct utilization of dissolved inorganic carbon in seawater for CO ₂ conversion promises chemical production on-demand and with zero carbon footprint. Photoelectrochemical (PEC) CO ₂ reduction (CO ₂ R) devices promise the sustainable conversion of dissolved carbon in seawater to carbon products using sunlight as the only energy input. However, the diffusion-dominant transport mechanism and the near-zero concentration of CO ₂ (aq) (CO ₂ dissolved in aqueous solution) in static seawater has made it extremely challenging to achieve high solar-to-fuel (STF) efficiency and high carbon-product selectivity. Here, where CO ₂ (aq) as a reactant generated in situ by acidification of HCO ₃ ^- flows continuously from BiVO ₄ photoanodes to Si photocathodes, enabling a single-step conversion of dissolved carbon into products. Our PEC device significantly increases the CO selectivity from 3% to 21%, which approaches the 30% theoretical limit according to multi-physics modeling. Meanwhile, the Si/BiVO ₄ PEC CO ₂ R device achieved a STF efficiency of 0.71%. Such flow engineering achieves flow-dependent selectivity, rate, and stability in simulated seawater, thus promising practical solar fuel production at scale.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0021953

OSTI ID:: 2515684

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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