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Enhancement of activity and selectivity to nitrogen in catalytic nitrate reduction by use of conductive carbon catalytic supports and control of hydrogen mass transfer regime
Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2021-09-21 , DOI: 10.1016/j.jece.2021.106419
D.T. González 1 , A. Marí 1 , J.A. Baeza 1 , L. Calvo 1 , M.A. Gilarranz 1
Affiliation  

Carbon materials with different structural properties (activated carbon, carbon nanofibers, reduced graphene oxide, graphite, and carbon black) were used as supports of Pd-Cu (5 wt%) catalysts for the catalytic reduction of NO3- in batch reactors. In general, those catalyst with smaller metal nanoparticles and carbon supports with higher specific surface area were more active, although remarkable activity was also observed for catalysts with relatively large nanoparticles and conductive supports. Conductivity of carbon supports also contributed to a lower selectivity to NH4+, which can be ascribed to higher charge transfer between metal and support reducing activation of intermediate species. The decrease of H2 feed into the reaction system resulted in external (gas-liquid) mass transfer constrains, as evidenced by the parameters describing control regime, and led to diminished NH4+ selectivity, particularly in the case of catalysts with conductive supports. Approaches combining control of mass transfer regime and conductive carbon catalytic supports can be useful to enhance selectivity to N2, which is a major challenge in catalytic NO3- reduction.



中文翻译:

通过使用导电碳催化载体和控制氢传质机制提高催化硝酸盐还原中对氮的活性和选择性

具有不同的结构特性(活性炭,碳纳米纤维,还原氧化石墨烯,石墨,炭黑等)碳材料用作钯-铜(5重量%)的催化剂NO的催化还原的载体3 -在间歇式反应器。一般来说,那些具有较小金属纳米颗粒和具有较高比表面积的碳载体的催化剂活性更高,尽管对于具有相对较大纳米颗粒和导电载体的催化剂也观察到显着的活性。碳载体的导电性也有助于降低对 NH 4 + 的选择性,这可以归因于金属和载体之间更高的电荷转移减少了中间物种的活化。H 2的减少进料到反应系统中导致外部(气-液)传质约束,正如描述控制方案的参数所证明的那样,并导致 NH 4 +选择性降低,特别是在具有导电载体的催化剂的情况下。结合控制传质机制和导电碳催化载体的方法可用于提高对 N 2 的选择性,这是催化 NO 3 -还原的主要挑战。

更新日期:2021-09-27
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