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首页> 外文期刊>ACS Sustainable Chemistry & Engineering >Strategies To Valorize the Hydrothermal Liquefaction-Derived Aqueous Phase into Fuels and Chemicals
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Strategies To Valorize the Hydrothermal Liquefaction-Derived Aqueous Phase into Fuels and Chemicals

机译:将水热液化衍生水相的策略变为燃料和化学品

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Valorization of the aqueous phase produced by hydrothermal liquefaction of terrestrial feedstocks is a potential strategy to decrease the minimum fuel selling price of biofuels. In this work, three different strategies were developed focused on upgrading the major molecules present in the aqueous phase, carboxylic acids, via (1) catalytic upgrading into chemicals via condensed-phase ketonization reaction, (2) catalytic upgrading to H2 via direct steam reforming, and (3) catalytic upgrading to H2 via anaerobic digestion (to CH4) followed by steam reforming. Direct catalytic upgrading of the aqueous feed was unsuccessful as the catalyst deactivated, therefore, an aqueous phase cleanup process based on activated carbon absorption followed by liquid-liquid extraction was developed to reduce color and inorganic contaminants while simultaneously concentrating desirable organic constituents. Stable conversion of the cleaned aqueous phase was successfully demonstrated using both condensed-phase ketonization (for ≈100 h) and steam reforming. Steam reforming was also demonstrated by employing a dual-bed catalyst configuration in which carboxylic acids first undergo ketonization over CeO2 in the vapor phase followed by steam reforming of the ketone intermediates over Co/CeO2. The dual-bed approach reduced coke deposition and thus improved catalyst stability compared to the single-bed catalyst configuration. Techno-economic analysis was performed to assess the economic viability of the three different strategies and revealed that the condensed-phase ketonization strategy provided the lowest minimum fuel selling price ($3.49/GGE) because of co-products (olefins) generated for sale. Both the steam reforming and anaerobic digestion processes benefited from onsite production of the H2 needed for biocrude hydrotreatment, thereby avoiding the need for natural gas; however, both processes resulted in similar, higher minimum fuel selling price, $4.23 and $4.25/GGE.
机译:通过陆地原料的水热液化产生的水相的储存是降低生物燃料最低燃料价格的潜在策略。在这项工作中,开发了三种不同的策略,专注于通过浓缩相酮化反应将(1)催化升级为化学品,通过直接蒸汽重整升至H 2,将存在于水相,羧酸,催化升级为化学品中的主要分子(3)(3)通过厌氧消化(至CH 4)催化升级至H2,然后进行蒸汽重整。作为催化剂失活的催化剂的直接催化升级是不成功的,因此,基于活性炭萃取的水相清洁过程,然后开发出液 - 液萃取,以减少颜色和无机污染物,同时浓缩所需的有机成分。使用浓缩相酮化(≈100h)和蒸汽重整成功地证明了清洗水相的稳定转化。还通过采用双床催化剂构型来证明蒸汽重整,其中羧酸首先在气相中的CeO 2上进行酮化,然后通过CO / CeO 2的酮中间体蒸汽重整。双层方法与单床催化剂构型相比,降低焦炭沉积,从而改善了催化剂稳定性。进行了技术经济分析,以评估三种不同策略的经济可行性,并透露,由于销售的共同产品(烯烃),炼金相酮化策略提供了最低的最低燃料销售价格(3.49美元/ GGE)。蒸汽重整和厌氧消化过程既受益于生物沉积加氢处理所需的H2的现场生产,从而避免了天然气的需求;然而,这两个过程导致了相似,最低燃料售价,4.23美元和4.25美元/ GGE。

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