Improved NH3-N conversion efficiency to N2 activated by BDD substrate on NiCu electrocatalysis process
Improved NH3-N conversion efficiency to N2 activated by BDD substrate on NiCu electrocatalysis process
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提高 NiCu 电催化过程中 BDD 底物活化的 NH3-N 转化为 N2 的效率
DOI：
10.1016/j.seppur.2021.119350
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发表时间：
2021-12
影响因子：
8.6
通讯作者：
Bin Yang
中科院分区：
文献类型：
--
作者：
Jingjin Song;Yang Yinhai;Yingna Jia;Tingting Wang;Jun Wei;Mingming Wang;Shaodong Zhou;Bin Yang;Yang Hou;Lecheng Lei;Bin Yang
NiCu/BDD用于提高nh3 -N的转化效率和对n2的选择性。•NiCu/BDD由于OER的抑制而表现出优异的电子转移性能。•BDD为N-H键激活过程提供了合适的氢受体。Cu/Ni-N协同相互作用稳定了中间体的相对能量。采用电化学共沉积法对双金属NiCu催化剂进行改性，制备了一种新型掺硼金刚石（BDD）电极，提高了nh3 -N在水溶液中的转化效率和对n2的选择性。结果表明，氨氧化反应（AOR）的n2选择性达到88.62%，nh3 -N在6 h内的氧化效率为44.8%，在1.2 V （vs Ag/AgCl）下电流效率高达84.17%，能耗为8.19 kW·h/(kgN)。利用原位拉曼光谱、x射线光电子能谱（XPS）和电子自旋共振（ESR）对反应机理进行了研究。实验证明，BDD底物不仅在提高电子传输速率方面起着至关重要的作用，而且在生成丰富的羟基自由基（·OH）方面也起着至关重要的作用，这些羟基自由基为N-H键的激活过程提供了合适的氢受体。理论计算进一步揭示了Cu(OH) 2与NiOOH的掺杂作用，构建了Cu/Ni协同金属-氮相互作用，稳定了中间体的相对能量，从而促进了反应。本研究为nh3 -N选择性电化学氧化机理的研究提供了新的思路，为废水处理提供了一种创新的催化阳极设计技术。
• NiCu/BDD was developed to enhance NH 3 -N conversion efficiency and selectivity to N 2 . • NiCu/BDD shows excellent electron transfer property due to the inhibition of OER. • BDD provides proper hydrogen acceptors for the N-H bond activation processes. • The concerted Cu/Ni-N interaction stabilizes the relative energy of intermediates. We developed a novel boron-doped diamond (BDD) electrode by the modification of bimetallic NiCu catalysts via electrochemical co-deposition method for improving the NH 3 -N conversion efficiency and selectivity to N 2 in aqueous solution. It shows that the N 2 selectivity of ammonia oxidation reaction (AOR) reached 88.62% with the NH 3 -N oxidation efficiency of 44.8% in 6 h. The high current efficiency of 84.17% was achieved at 1.2 V (vs Ag/AgCl), and the energy consumption was 8.19 kW·h/(kgN). Furthermore, the reaction mechanism has been investigated by in-situ Raman spectra, X-ray photoelectron spectroscopy (XPS) and electron spin resonance (ESR) during the reaction. It is verified that the BDD substrate plays a crucial role not only in the improvement of electronic transmission rate and but also the generation of abundant hydroxyl radicals ( · OH) which provide proper hydrogen acceptors for the N-H bond activation processes. Theoretical calculations further reveal the doping effect of Cu(OH) 2 with NiOOH that constructs the Cu/Ni concerted metal-nitrogen interaction, which stabilizes the relative energies of the intermediates thus promoting the reaction. This work sheds new light on the mechanism of selective electrochemical oxidation of NH 3 -N and develops an innovative technology of catalytic anode design toward wastewater treatment.
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