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Ambient sunlight-driven photothermal methanol dehydrogenation for syngas production with 32.9 % solar-to-hydrogen conversion efficiency.

ABSTRACT: Methanol dehydrogenation is an efficient way to produce syngas with high quality. The current efficiency of sunlight-driven methanol dehydrogenation is poor, which is limited by the lack of excellent catalysts and effective methods to convert sunlight into chemicals. Here, we show that atomically substitutional Pt-doped in CeO₂ nanosheets (Pt_s-CeO₂) exhibit excellent methanol dehydrogenation activity with 500-hr level catalytic stability, 11 times higher than that of Pt nanoparticles/CeO₂. Further, we introduce a photothermal conversion device to heat Pt_s-CeO₂ up to 299°C under 1 sun irradiation owning to efficient full sunlight absorption and low heat dissipation, thus achieving an extraordinarily high methanol dehydrogenation performance with a 481.1 mmol g^-1 h^-1 of H₂ production rate and a high solar-to-hydrogen (STH) efficiency of 32.9%. Our method represents another progress for ambient sunlight-driven stable and active methanol dehydrogenation technology.

SUBMITTER: Bai X

PROVIDER: S-EPMC7841357 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Ambient sunlight-driven photothermal methanol dehydrogenation for syngas production with 32.9 % solar-to-hydrogen conversion efficiency.

Bai Xianhua X Yuan Dachao D Li Yaguang Y Song Hui H Lu Yangfan Y San Xingyuan X Lu Jianmin J Fu Guangsheng G Wang Shufang S Ye Jinhua J

iScience 20210109 2

Methanol dehydrogenation is an efficient way to produce syngas with high quality. The current efficiency of sunlight-driven methanol dehydrogenation is poor, which is limited by the lack of excellent catalysts and effective methods to convert sunlight into chemicals. Here, we show that atomically substitutional Pt-doped in CeO2 nanosheets (Pts-CeO2) exhibit excellent methanol dehydrogenation activity with 500-hr level catalytic stability, 11 times higher than tha ...[more]

PMID: 33537660

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Project description:BackgroundIn times of global climate change, the conversion and capturing of inorganic CO2 have gained increased attention because of its great potential as sustainable feedstock in the production of biofuels and biochemicals. CO2 is not only the substrate for the production of value-added chemicals in CO2-based bioprocesses, it can also be directly hydrated to formic acid, a so-called liquid organic hydrogen carrier (LOHC), by chemical and biological catalysts. Recently, a new group of enzymes were discovered in the two acetogenic bacteria Acetobacterium woodii and Thermoanaerobacter kivui which catalyze the direct hydrogenation of CO2 to formic acid with exceptional high rates, the hydrogen-dependent CO2 reductases (HDCRs). Since these enzymes are promising biocatalysts for the capturing of CO2 and the storage of molecular hydrogen in form of formic acid, we designed a whole-cell approach for T. kivui to take advantage of using whole cells from a thermophilic organism as H2/CO2 storage platform. Additionally, T. kivui cells were used as microbial cell factories for the production of formic acid from syngas.ResultsThis study demonstrates the efficient whole-cell biocatalysis for the conversion of H2 + CO2 to formic acid in the presence of bicarbonate by T. kivui. Interestingly, the addition of KHCO3 not only stimulated formate formation dramatically but it also completely abolished unwanted side product formation (acetate) under these conditions and bicarbonate was shown to inhibit the membrane-bound ATP synthase. Cell suspensions reached specific formate production rates of 234 mmol gprotein -1 h-1 (152 mmol gCDW -1 h-1), the highest rates ever reported in closed-batch conditions. The volumetric formate production rate was 270 mmol L-1 h-1 at 4 mg mL-1. Additionally, this study is the first demonstration that syngas can be converted exclusively to formate using an acetogenic bacterium and high titers up to 130 mM of formate were reached.ConclusionsThe thermophilic acetogenic bacterium T. kivui is an efficient biocatalyst which makes this organism a promising candidate for future biotechnological applications in hydrogen storage, CO2 capturing and syngas conversion to formate.

Dataset Information

Ambient sunlight-driven photothermal methanol dehydrogenation for syngas production with 32.9 % solar-to-hydrogen conversion efficiency.

Publications

Ambient sunlight-driven photothermal methanol dehydrogenation for syngas production with 32.9 % solar-to-hydrogen conversion efficiency.

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