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Rapid Conversion of Co2+ to Co3+ by Introducing Oxygen Vacancies in Co3O4 Nanowire Anodes for Nitrogen Removal with Highly Efficient H2 Recovery in Urine Treatment
Environmental Science & Technology ( IF 11.4 ) Pub Date : 2022-06-24 , DOI: 10.1021/acs.est.2c00729
Yan Zhang 1 , Xiaoya Huang 1 , Jinhua Li 1 , Jing Bai 1, 2 , Changhui Zhou 1 , Lei Li 1 , Jiachen Wang 1 , Mingce Long 1 , Xinyuan Zhu 3 , Baoxue Zhou 1, 2
Affiliation  

Urine is a nitrogenous waste biomass but can be used as an appealing alternative substrate for H2 recovery. However, urine electrolysis suffers from sluggish kinetics and requires alkaline condition. Herein, we report a novel system to decompose urine to H2 and N2 under neutral conditions mediated by Cl using oxygen-vacancy-rich Co3O4 nanowire (Ov-Co3O4) anodes and CuO nanowire cathodes. The Co2+/Co3+ cycle in Co3O4 activates Cl in urine to Cl, which rapidly and selectively converts urea into N2. Thus, electron transfer is boosted for H2 production, eliminating the kinetic limitations. The shuttle of Co2+ to Co3+ is the key step for Cl yield, which is accelerated due to the introduction of Ov. Electrochemical analysis shows that Ov induces positive charge on the Co center; therefore, Co2+ loses electrons more efficiently to form Co3+. H2 production in this system reaches 716 μmol h–1, which is 320% that of non-radical-mediated urine electrolysis. The utilization of Ov-Co3O4 further enhances H2 generation, which is 490 and 210% those of noble Pt and RuO2, respectively. Moreover, urine is effectively degraded in 90 min with the total nitrogen removal of 95.4%, and N2 is the final product. This work provides new insights for efficient and low-cost recovery of H2 and urine remediation.

中文翻译:

通过在 Co3O4 纳米线阳极中引入氧空位来快速将 Co2+ 转化为 Co3+,以在尿液处理中高效回收氢气以去除氮

尿液是一种含氮废物生物质,但可用作 H 2回收的有吸引力的替代底物。然而,尿液电解具有缓慢的动力学并且需要碱性条件。在此,我们报告了一种在Cl •介导的中性条件下使用富氧空位Co 3 O 4纳米线(O v -Co 3 O 4 ) 阳极和CuO 纳米线阴极将尿液分解为H 2和N 2的新系统。Co 3 O 4中的 Co 2+ /Co 3+循环将尿液中的Cl -活化为 Cl ,其快速和选择性地将尿素转化为 N 2因此,H 2产生的电子转移得到促进,消除了动力学限制。Co 2+到Co 3+的穿梭是Cl 收率的关键步骤,由于O v的引入而加速。电化学分析表明,O v在Co中心产生正电荷;因此,Co 2+更有效地失去电子以形成Co 3+。该系统中的H 2产量达到 716 μmol h -1,是非自由基介导的尿液电解的 320%。O v的利用-Co 3 O 4进一步提高了H 2的产生,分别是贵金属Pt和RuO 2的490%和210% 。此外,尿液在90 min内被有效降解,总氮去除率为95.4%,最终产物为N 2 。这项工作为高效和低成本的 H 2回收和尿液修复提供了新的见解。
更新日期:2022-06-24
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