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202. Efficient solar-driven CO2-to-fuel conversion via Ni/MgAlOx@SiO2nanocomposites at low temperature

Author

Liu, Xianglei, Ling, Yueyue, Sun, Chen, Shi, Hang, Zheng, Hangbin, Song, Chao, Gao, Ke, Dang, Chunzhuo, Sun, Nan, Xuan, Yimin, and Ding, Yulong

Abstract

Solar-driven CO2-to-fuel conversion assisted by another major greenhouse gas CH4is promising to concurrently tackle energy shortage and global warming problems. However, current techniques still suffer from drawbacks of low efficiency, poor stability, and low selectivity. Here, a novel nanocomposite composed of interconnected Ni/MgAlOxnanoflakes grown on SiO2particles with excellent spatial confinement of active sites is proposed for direct solar-driven CO2-to-fuel conversion. An ultrahigh light-to-fuel efficiency up to 35.7%, high production rates of H2(136.6 mmol min−1g−1) and CO (148.2 mmol min−1g−1), excellent selectivity (H2/CO ratio of 0.92), and good stability are reported simultaneously. These outstanding performances are attributed to strong metal-support interactions, improved CO2absorption and activation, and decreased apparent activation energy under direct light illumination. MgAlOx@SiO2support helps to lower the activation energy of CH* oxidation to CHO* and improve the dissociation of CH4to CH3* as confirmed by DFT calculations. Moreover, the lattice oxygen of MgAlOxparticipates in the reaction and contributes to the removal of carbon deposition. This work provides promising routes for the conversion of greenhouse gasses into industrially valuable syngas with high efficiency, high selectivity, and benign sustainability.

Published
2024
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214. Air to fuel: Direct capture of CO2 from air and in-situ solar-driven conversion into syngas via Nix/NaA nanomaterials.

Author

Tian, Cheng, Liu, Xianglei, Liu, Chenxi, Li, Shaoyang, Li, Qiyan, Sun, Nan, Gao, Ke, Jiang, Zhixing, Chang, Kun, and Xuan, Yimin

Abstract

Ever-increasing CO2 emissions and atmospheric concentration mainly due to the burning of traditional fossil fuels have caused severe global warming and climate change problems. Inspired by nature's carbon cycle, we propose a novel dual functional catalyst-sorbent to tackle energy and environmental problems simultaneously via direct capture of CO2 from air and in-situ solar-driven conversion into clean fuels. Economically and operationally advantageous, the planned coupling reaction can be carried out in a single reactor without the requirement for an extra trapping device. The great CO2 capture and conversion performance in an integrated step is shown by the CO2 capacity of up to 0.38 mmol·g−1 for adsorption from 500 ppm CO2 at 25 °C and the CO2 conversion rate of up to 95%. Importantly, the catalyst-sorbent is constituted of a nonprecious metal Ni catalyst and an inexpensive commercially available CO2 sorbent, viz, zeolite NaA. Furthermore, this designed dual functional material also exhibits outstanding stability performance. This work offers a novel pathway of capturing CO2 in the air at room temperature and converting it by CH4 into fuel, contributing to the new era of carbon neutrality. [ABSTRACT FROM AUTHOR]

Published
2023
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235. Hydrophobic Ni@N‐Doped TiO2 Nanosheet Arrays‐Carbon Paper Photocatalyst for CO2 Photoreduction at Tri‐Phase Interfaces.

Author

Zhao, Dawei, Dang, Chunzhuo, Xuan, Yimin, and Zhu, Qibin

Subjects
PHOTOREDUCTION, HYDROGEN evolution reactions, CARBON paper, MASS transfer, NICKEL oxide, MAGNETRON sputtering, PHOTOCATALYSTS
Abstract

Rational interphase reaction provides a feasible method to overcome the matters of insufficient adsorption of CO2 molecules at the catalytic sites and competitive hydrogen evolution reaction (HER), which can increase the formation rate and selectivity of carbon derivatives in photocatalytic CO2 reduction. Herein, a hydrophobic photocatalyst with TiO2 nanosheet arrays grown on hydrophobic carbon paper (TiO2‐HCP) is fabricated using a combination of magnetron sputtering and hydrothermal method, and its unique structure not only endows it excellent light absorption and effective carrier spatial separation but also avoids the hydrophobic reagent covering reactive sites. When the interphase reaction shifts from solid–liquid diphase to gas‐liquid‐solid tri‐phase, the photocatalytic CO2 reduction over TiO2‐HCP mainly generates CO molecules and effectively suppresses HER due to the HCP suppressing the mass transfer of H2O molecules to active sites. Notably, amounts of H2 byproduct can further react with CO2/CO to produce high value‐added CH4 resultant by modifying the N‐doped TiO2‐HCP with nickel/nickel oxide species. In the tri‐phase interfacial CO2 photoreduction system, the CH4 formation rate of Ni@N‐doped TiO2‐HCP reaches 134.17 µmol m−2 h−1 (about 74.6% selectivity) and total carbon derivatives selectivity is about 93%. [ABSTRACT FROM AUTHOR]

Published
2023
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