Enabling circular economy by N-recovery: Electrocatalytic reduction of nitrate with cobalt hydroxide nanocomposites on copper foam treating low conductivity groundwater effluents
Enabling circular economy by N-recovery: Electrocatalytic reduction of nitrate with cobalt hydroxide nanocomposites on copper foam treating low conductivity groundwater effluents
复制标题
通过氮回收实现循环经济：用氢氧化钴纳米复合材料在泡沫铜上电催化还原硝酸盐，处理低电导率地下水废水
DOI：
10.1016/j.scitotenv.2023.163938
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发表时间：
2023
影响因子：
9.8
通讯作者：
Garcia-Segura, Sergi
中科院分区：
文献类型：
--
作者：
Cerrón-Calle, Gabriel Antonio;Fajardo, Ana S.;Liu, Jingyue;Sánchez-Sánchez, Carlos M.;Garcia-Segura, Sergi
肥料在粮食-能源-水的关系中发挥着至关重要的作用。传统的人工固氮制氨方法是一个高能耗的集中式过程，由于氮素释放到水中，导致氮循环的不平衡。电催化硝酸盐还原（ENR）是一种很有前途的氮资源回收替代方案，可以使氨在分散的环境中循环再利用。然而，主要的挑战是确定选择性和负担得起的电催化剂。需要识别依赖于铂族金属以外的东西的电极，以克服与使用昂贵和濒危元素相关的障碍。在这项研究中，地球丰富的催化剂，Cu/Co（OH）x，制备和优化的电沉积，表现出上级氨生产。在30 mg NO3−-N L−1的环境相关条件下，Cu/Co（OH）x比原始Cu泡沫（分别为0.7和0.3 mmol NH3 gcat −1h−1）显示出更高的氨产量。实验评价表明，在Cu/Co（OH）xsites的直接还原和催化加氢机制。浸出分析表明，Cu/Co（OH）x具有突出的稳定性，可以忽略不计的金属浓度低于最大污染物水平的Cu和Co。这些结果提供了一个框架，使用地球丰富的材料在ENR具有可比的效率和能源消耗的铂族材料。
Fertilizers play a vital role in the food-energy-water nexus. The traditional method of artificial nitrogen fixation to produce ammonia is a high-energy intensive centralized process that has caused an imbalance of the N-cycle due to the release of N-species to water. Electrocatalytic nitrate reduction (ENR) to ammonia is a promising N-resource recovery alternative that can enable the circular reuse of ammonia in decentralized settings. However, the primary challenge is identifying selective and affordable electrocatalysts. Identifying electrodes that rely on something other than platinum-group metals is required to surpass barriers associated with using expensive and endangered elements. In this study, an earth-abundant bimetallic catalyst, Cu/Co(OH)x, prepared and optimized by electrodeposition, demonstrates superior ammonia production. Under environmentally relevant conditions of 30 mg NO3−-N L−1, Cu/Co(OH)xshowed higher ammonia production than pristine Cu foam with 0.7 and 0.3 mmol NH3gcat−1h−1, respectively. The experimental evaluation demonstrated direct reduction and catalytic hydrogenation mechanisms in Cu/Co(OH)xsites. Leaching analyses suggest that Cu/Co(OH)xhas outstanding stability with negligible metal concentration below the maximum contaminant level for both Cu and Co. These results provide a framework for using earth-abundant materials in ENR with comparable efficiency and energy consumption to platinum-group materials.