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DOE OSTI · 2874879

A Monolithic Artificial Leaf for Solar Methanol Production from CO 2 and H 2 O

Shang, Bo [Yale Univ., New Haven, CT (United States)] (ORCID:0000000222946062)·Yu, Kunpeng [Yale Univ., New Haven, CT (United States)]·Margavio, Hannah R. M. [North Carolina State University, Raleigh, NC (United States)] (ORCID:0000000153273713)·Yang, Haozhou [Yale Univ., New Haven, CT (United States)]·Gao, Yuanzuo [Yale Univ., New Haven, CT (United States)]·Yang, Jindou [Yale Univ., New Haven, CT (United States)]·Li, Jing [Yale Univ., New Haven, CT (United States)]·Li, Min [Yale Univ., New Haven, CT (United States)]·Shi, Jinquan [Yale Univ., New Haven, CT (United States)]·Liu, Mengxia [Yale Univ., New Haven, CT (United States)]·Parsons, Gregory N. [North Carolina State University, Raleigh, NC (United States)] (ORCID:0000000200485859)·Dempsey, Jillian L. [University of North Carolina, Chapel Hill, NC (United States)] (ORCID:0000000294594166)·Meyer, Gerald J. [University of North Carolina, Chapel Hill, NC (United States)] (ORCID:0000000242276393)·Mallouk, Thomas E. [Univ. of Pennsylvania, Philadelphia, PA (United States)] (ORCID:0000000345994208)·Wang, Hailiang [Yale Univ., New Haven, CT (United States)] (ORCID:0000000344092034)
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Abstract

Methanol, an important liquid fuel and chemical feedstock, has yet to be produced using solar energy, H 2 O, and CO 2 as sole inputs in a standalone device. Here, this study directly addresses this longstanding challenge through presenting the first demonstration of unbiased solar methanol production from CO 2 and H 2 O with a monolithic artificial leaf design, surpassing the previous best energy efficiency in solar alcohol production by at least 1 order of magnitude. We first develop a new generation of photocathodes based on Si micropillar arrays and a cobalt tetraaminophthalocyanine molecular catalyst. By integrating a C 60 interlayer that facilitates unidirectional electron transfer through the semiconductor/catalyst interface, we realize a photovoltage of 500 mV, one of the highest recorded for single-junction Si-based photoelectrodes in aqueous CO 2 reduction, as well as unprecedented methanol formation with a Faradaic efficiency of 30% and a partial current density of 6.3 mA cm –2 . We further integrate the photocathode with a multijunction perovskite photovoltaic minimodule to afford a standalone solar fuel system, which demonstrates a light-to-methanol conversion efficiency of 0.8%, 32 times higher than the present record in light-to-alcohol conversion with an artificial leaf.

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Shang, Bo [Yale Univ., New Haven, CT (United States)] (ORCID:0000000222946062), Yu, Kunpeng [Yale Univ., New Haven, CT (United States)], Margavio, Hannah R. M. [North Carolina State University, Raleigh, NC (United States)] (ORCID:0000000153273713), Yang, Haozhou [Yale Univ., New Haven, CT (United States)], Gao, Yuanzuo [Yale Univ., New Haven, CT (United States)], Yang, Jindou [Yale Univ., New Haven, CT (United States)], Li, Jing [Yale Univ., New Haven, CT (United States)], Li, Min [Yale Univ., New Haven, CT (United States)], Shi, Jinquan [Yale Univ., New Haven, CT (United States)], Liu, Mengxia [Yale Univ., New Haven, CT (United States)], Parsons, Gregory N. [North Carolina State University, Raleigh, NC (United States)] (ORCID:0000000200485859), Dempsey, Jillian L. [University of North Carolina, Chapel Hill, NC (United States)] (ORCID:0000000294594166), Meyer, Gerald J. [University of North Carolina, Chapel Hill, NC (United States)] (ORCID:0000000242276393), Mallouk, Thomas E. [Univ. of Pennsylvania, Philadelphia, PA (United States)] (ORCID:0000000345994208), Wang, Hailiang [Yale Univ., New Haven, CT (United States)] (ORCID:0000000344092034). 2026-04-30. A Monolithic Artificial Leaf for Solar Methanol Production from CO 2 and H 2 O. https://doi.org/10.1021/jacs.6c04213

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