Wang Jian, Tao Junyu, Dong Xiaoshan, Liu Zibiao, Hou Donghao, Hu Yongjie, Yan Beibei, Su Hong, Chen Guanyi
School of Environmental Science and Engineering, Tianjin University, Tianjin, 300350, China.
School of Mechanical Engineering, Tianjin University of Commerce, Tianjin, 300134, China.
J Environ Manage. 2022 Oct 15;320:115827. doi: 10.1016/j.jenvman.2022.115827. Epub 2022 Aug 6.
A hydrothermal oxygen uncoupling (HTOU) method which combines aqueous phase reforming (APR) and oxygen uncoupling was proposed to treat biogas slurry (BS). Based on Le Chatelier's principle, this novel approach was constructed and realized by Cu-α-FeO·α-MoO catalyst with van der Waals heterojunction-redox property. Additionally, the catalyst was synthesized by integrating a simple one-pot sol-gel method and thermal hydrogenating. Results indicated that the optimal removal efficiencies of non-purgeable organic carbon (NPOC) (76.29%), total nitrogen (TN) (45.56%), and ammonia nitrogen (AN) (29.03%) were achieved on the Cu-α-FeO·α-MoO catalyst at 225.00 °C for 30.00 min, respectively. The significant performance of Cu-α-FeO·α-MoO could be attributed to three aspects. (1) The α-MoO nanosheets with van der Waals heterostructures obtained at the calcination temperature of 600.00 °C, which can provide the superior performance of APR for hydrogen generation. (2) The adsorbed oxygen species were eliminated by thermal hydrogenating which had a surface passivation effect. (3) The effect of oxygen uncoupling in the lattice oxygen and gaseous oxygen release reaction was beneficial to the degradation of organic matter. Moreover, the reuse of catalysts studies further revealed that the deactivation of catalysts originated from carbon deposition of aromatic polymers and heavy metals oxides pollution. Overall, these findings disclosed that the HTOU could be a promising alternative to the treatment of high-concentration organic wastewater.
提出了一种将水相重整(APR)与氧解耦相结合的水热氧解耦(HTOU)方法来处理沼液(BS)。基于勒夏特列原理,这种新方法是通过具有范德华异质结-氧化还原特性的Cu-α-FeO·α-MoO催化剂构建并实现的。此外,该催化剂是通过简单的一锅溶胶-凝胶法和热氢化法合成的。结果表明,在225.00℃下,Cu-α-FeO·α-MoO催化剂对不可吹扫有机碳(NPOC)(76.29%)、总氮(TN)(45.56%)和氨氮(AN)(29.03%)的最佳去除效率分别在30.00分钟内实现。Cu-α-FeO·α-MoO的显著性能可归因于三个方面。(1)在600.00℃煅烧温度下获得的具有范德华异质结构的α-MoO纳米片,可为制氢提供优异的APR性能。(2)通过具有表面钝化作用的热氢化消除吸附的氧物种。(3)晶格氧和气态氧释放反应中的氧解耦效应有利于有机物的降解。此外,催化剂的重复使用研究进一步表明,催化剂的失活源于芳香族聚合物的碳沉积和重金属氧化物污染。总体而言,这些发现表明HTOU可能是处理高浓度有机废水的一种有前途的替代方法。