Exhaustive Conversion of Inorganic Nitrogen to Nitrogen Gas Based on a Photoelectro-Chlorine Cycle Reaction and a Highly Selective Nitrogen Gas Generation Cathode
Exhaustive Conversion of Inorganic Nitrogen to Nitrogen Gas Based on a Photoelectro-Chlorine Cycle Reaction and a Highly Selective Nitrogen Gas Generation Cathode
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基于光电氯循环反应和高选择性氮气发生阴极的无机氮彻底转化为氮气
DOI：
10.1021/acs.est.7b04626
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发表时间：
2018
影响因子：
11.4
通讯作者：
Zhou Baoxue
中科院分区：
文献类型：
--
作者：
Zhang Yan;Li Jinhua;Bai Jing;Shen Zhaoxi;Li Linsen;Xia Ligang;Chen Shuai;Zhou Baoxue
提出了一种将无机氮完全转化为氮气的新方法。该系统设计的关键特性包括在Cl-存在的情况下进行彻底的光电化学循环反应，其中光空穴氧化Cl-产生的Cl·选择性地将NH 4+转化为氮气和一些NO3-或NO2-。NO3-或NO2-最终在高选择性的Pd-Cu-改性的泡沫镍（Pd-Cu/NF）阴极上还原为氮气，以实现无机氮向氮气的彻底转化。结果表明，当无机氮浓度为30 mg L-1（NO3-、NH 4+、NO3-/NH 4 += 1：1和NO2-/NO3-/NH 4 += 1：1：1）时，90 min内总氮去除率分别为98.2%、97.4%、93.1%和98.4%，延长反应时间可使剩余氮完全去除。硝酸盐的快速还原归因于Pd-Cu/NF的电容特性，其在双电层的存在下促进硝酸盐吸附，消除阴极和阴离子之间的排斥。硝酸盐的有效去除速率常数为0.050 min-1，这是33倍以上的铂阴极。该系统具有处理效率高、成本低、能源清洁等优点，在无机氮处理方面具有很大的应用潜力。
A novel method for the exhaustive conversion of inorganic nitrogen to nitrogen gas is proposed in this paper. The key properties of the system design included an exhaustive photoelectrochemical cycle reaction in the presence of Cl–, in which Cl· generated from oxidation of Cl–by photoholes selectively converted NH4+to nitrogen gas and some NO3–or NO2–. The NO3–or NO2–was finally reduced to nitrogen gas on a highly selective Pd–Cu-modified Ni foam (Pd–Cu/NF) cathode to achieve exhaustive conversion of inorganic nitrogen to nitrogen gas. The results indicated total nitrogen removal efficiencies of 30 mg L–1inorganic nitrogen (NO3–, NH4+, NO3–/NH4+= 1:1 and NO2–/NO3–/NH4+= 1:1:1) in 90 min were 98.2%, 97.4%, 93.1%, and 98.4%, respectively, and the remaining nitrogen was completely removed by prolonging the reaction time. The rapid reduction of nitrate was ascribed to the capacitor characteristics of Pd–Cu/NF that promoted nitrate adsorption in the presence of an electric double layer, eliminating repulsion between the cathode and the anion. Nitrate was effectively removed with a rate constant of 0.050 min–1, which was 33 times larger than that of Pt cathode. This system shows great potential for inorganic nitrogen treatment due to the high rate, low cost, and clean energy source.