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Oxygen-vacancy-mediated catalytic methanation of lignocellulose at temperatures below 200°C
Joule ( IF 39.8 ) Pub Date : 2021-07-27 , DOI: 10.1016/j.joule.2021.07.001
Hongru Zhou 1 , Min Wang 1 , Feng Wang 2
Affiliation  

Biomethane is a clean energy and a key platform chemical for modern chemical industries. The conversion of biomass, especially the most abundant lignocellulose, into biomethane is challenging and shows low selectivity either in chemical or biological processes. Herein, we report the direct methanation of biomass at temperatures below 200°C with >95% selectivity using interfacial oxygen-vacancy (VO)-mediated catalysis over Ru/TiO2. The biomass feedstock is oxidized by TiO2 to form CO2 and VO, and CO2 is then in situ reduced on Ru sites to CH4, restoring the oxygen to VO simultaneously. Various biomass resources were converted into methane with 82%–99% yields. Even lowering the temperature to 120°C, about 0.24 mmol g−1 h−1 of CH4 with >99% selectivity was steadily produced from 50 wt % aqueous glycerol for 432 h. In situ X-ray photoelectron spectroscopy, infrared spectrometry, and DFT calculation confirm the VO-mediated catalysis process over Ru/TiO2.



中文翻译:

在低于 200°C 的温度下氧空位介导的木质纤维素催化甲烷化

生物甲烷是一种清洁能源,是现代化学工业的关键平台化学品。将生物质,尤其是最丰富的木质纤维素转化为生物甲烷具有挑战性,并且在化学或生物过程中表现出低选择性。在此,我们报告了使用界面氧空位 (V O ) 介导的 Ru/TiO 2催化在低于 200°C 的温度下以 >95% 的选择性对生物质进行直接甲烷化。所述生物质原料通过的TiO氧化2,以形成CO 2和V ø,和CO 2然后在原位上的Ru位点以CH降低4,氧还原到V ö同时。各种生物质资源以 82%–99% 的产率转化为甲烷。即使将温度降低至120°C,在432小时内从50重量%的甘油水溶液稳定地产生约0.24 mmol g -1 h -1的CH 4并且具有>99%的选择性。原位X 射线光电子能谱、红外光谱和 DFT 计算证实了在 Ru/TiO 2 上的 V O介导的催化过程。

更新日期:2021-07-27
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