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28. Synergistic Photocatalytic CO2 Reduction and Methanol Oxidation via Self-Photogenerated Oxygen Vacancy-Rich TiO2 Nanostructures.

Author

Mao, Haoning, Tan, Yu, Chen, Qiwen, Cai, Minying, Xu, Chao, Yang, Tianzhen, Gao, Qiongzhi, Zhang, Shengsen, Fang, Yueping, Liu, Shijun, Peng, Feng, and Yang, Siyuan

Abstract

Integrating CO2 reduction with methanol oxidation presents a promising alternative strategy to store solar energy in CO2 reduction and produce more sustainable clean fuels and chemicals products, while identifying the carbon sources in the final products and elucidating the interactions between CO2 and methanol within such a mixed system is still particularly challenging. Herein, this study explores the efficiency of synergistic photocatalytic CO2 reduction and methanol oxidation via self-photogenerated oxygen vacancy-rich TiO2 nanostructures. Employing NMR spectroscopy and GC–MS analysis for 13CO2 isotope tracing samples, the exact carbon sources in both liquid and gas-phase products were clearly figure out. Moreover, through in situ DRIFTS analysis and DFT calculations, the crucial role of oxygen vacancies in enhancing catalytic activity and selectivity is revealed, and the CO2 reduction and methanol oxidation pathway on oxygen vacancy-rich TiO2 nanostructures are proposed. Consequently, our findings offer profound implications for advancing the field of synergistic photocatalytic processes, aiming to generate high-value chemical fuels sustainably. [ABSTRACT FROM AUTHOR]

Published
2024
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41. Operando Reconstruction of Porous Carbon Supported Copper Selenide Promotes the C2 Production from CO2RR.

Author

Li, Simeng, Yu, Jun, Zhang, Shengsen, Qiu, Weitao, Tang, Xing, Lin, Zedong, Cai, Rongming, Fang, Yueping, Yang, Shihe, and Cai, Xin

Subjects
ELECTROLYTIC reduction, COUPLING reactions (Chemistry), SCISSION (Chemistry), DENSITY functional theory, ATOMIC structure, SURFACE reconstruction, COPPER, COPPER surfaces
Abstract

Precisely regulating surface reconstruction of copper (Cu) chalcogenides‐based catalysts to promote the multicarbon (C2+)selectivity of the electrochemical CO2 reduction reaction (CO2RR) is hampered by the challenging control of the intractable anions and the optimal Cuδ+ reduction (0 < δ < 1). Herein, a porous carbon‐supported copper selenides electrocatalyst that can remarkably improve the C2‐product yield and especially unveil the time‐revolved electrochemical CO2RR reconstruction process to enable the high C2‐selectivity, most notably for ethanol is constructed. The Faradic efficiency (FE) of C2‐products achieved is as high as ≈85.2% with a partial current density of 229.5 mA cm−2. Operando infrared spectroscopy and density functional theory (DFT) calculations unravel that the surface Se vacancies (VSe) formation brings closer the neighboring Cu+ atoms and activates the Cu sites, thereby rendering efficient generation of the key intermediates (*CO and *CHO) and lowering the C–C coupling barrier for C2 production. The appearance of metallic Cu can shorten the next‐nearest Cu0–Cu+ distance for O atom to bridge in, leading to the preferential formation of *OC2H4 towards ethanol instead of C–O bond cleavage to form ethylene. This work opens the avenue of designing suitable local atomic structures catalysts to engage the intermediates for targeted CO2RR products. [ABSTRACT FROM AUTHOR]

Published
2024
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