Efficient hydrogen production from high-concentration aqueous formic acid over bio-based γ-Mo2N catalysts

IF 6.4 3区环境科学与生态学 Q2 ENERGY & FUELS

Carbon Resources Conversion Pub Date : 2023-12-28 DOI:10.1016/j.crcon.2023.100209

Zeyu Liu , Song Yang , Yanyan Yang , Wenyao Guo , Jianfei Wang , Bixi Wang , Xin Gao , Ting Wang , Shoujun Liu , Zhongliang Yu

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Abstract

Formic acid is regarded to be one of the most prospective hydrogen carriers. Effective screening of the fitting non-noble-metal-based heterogeneous catalysts to substitute the expensive noble-metal-based ones for FA dehydrogenation is considered as a key to the commercial application for hydrogen economics. Herein, dehydrogenation of liquid neat FA achieved a gas production value of 1753.5 mL/g_cat./h at 94 °C by using a biomass-derived γ-Mo₂N based catalyst synthesized from the earth-abundant molybdenum and soybean with a facile pyrolysis process. The effect of material ratio, pyrolysis temperature on the catalytic performance of FA dehydrogenation were studied in details. In particular, the catalyst obtained at a pyrolysis temperature of 700 °C, weight ratios of ammonium molybdate to soybean of 0.2/1 exhibited the highest activity. In addition, the catalytic activity increased with the increase of FA concentration, but conversely, the dehydrogenation selectivity decreased with the increasing FA concentration. Moreover, it was found that the Bio-Mo₂N catalyst was rather stable over the 40 h continuous reaction period.

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在生物基 γ-Mo2N 催化剂上从高浓度甲酸水溶液中高效制氢

甲酸被认为是最具潜力的氢载体之一。有效筛选合适的非贵金属基异相催化剂来替代昂贵的贵金属基催化剂用于甲酸脱氢被认为是氢经济商业应用的关键。在本文中，使用一种基于生物质的γ-Mo2N催化剂，该催化剂由地球上丰富的钼和大豆通过简便的热解工艺合成，在94 °C条件下，液态纯FA的脱氢产气量达到1753.5 mL/gcat./h。详细研究了材料配比、热解温度对 FA 脱氢催化性能的影响。其中，热解温度为 700 ℃、钼酸铵与大豆的重量比为 0.2/1 时得到的催化剂活性最高。此外，催化活性随脂肪酸浓度的增加而增加，但相反，脱氢选择性随脂肪酸浓度的增加而降低。此外，研究还发现 Bio-Mo2N 催化剂在 40 小时的连续反应期间相当稳定。

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来源期刊

Carbon Resources Conversion Materials Science-Materials Science (miscellaneous)

CiteScore

9.90

自引率

11.70%

发文量

审稿时长

10 weeks

期刊介绍： Carbon Resources Conversion (CRC) publishes fundamental studies and industrial developments regarding relevant technologies aiming for the clean, efficient, value-added, and low-carbon utilization of carbon-containing resources as fuel for energy and as feedstock for materials or chemicals from, for example, fossil fuels, biomass, syngas, CO2, hydrocarbons, and organic wastes via physical, thermal, chemical, biological, and other technical methods. CRC also publishes scientific and engineering studies on resource characterization and pretreatment, carbon material innovation and production, clean technologies related to carbon resource conversion and utilization, and various process-supporting technologies, including on-line or off-line measurement and monitoring, modeling, simulations focused on safe and efficient process operation and control, and process and equipment optimization.