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Mott–Schottky contact synergistically boosts the electroreduction of nitrate to ammonia under low-nitrate concentration
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2024-03-19 , DOI: 10.1039/d4ee00715h
Xiaojuan Zhu 1, 2 , Chaoqun Ma 3 , Yi-Chi Wang 4 , Kaiyu Qu 1, 2 , Leyang Song 1, 2 , Jing Wang 1, 2 , Yushuang Gong 1, 2 , Xiang Liu 1, 2 , Jintao Zhang 1 , Qipeng Lu 3 , An-Liang Wang 1, 2
Affiliation  

The electrocatalytic nitrate reduction reaction (NO3RR) holds tremendous potential for remediating NO3 pollution in groundwater and obtaining clean ammonia (NH3). However, the currently reported NO3RR catalysts face challenges in achieving high conversion efficiency at low NO3 concentrations due to sluggish reaction kinetics. Herein, we present a highly efficient Mott–Schottky electrocatalyst, composed of an amorphous Co–B nanochain embedded in amorphous CoOx nanosheets (Co–B@CoOx). In 100 ppm NO3–N, the Co–B@CoOx catalyst exhibits remarkable performance, achieving over 95% NO3 removal within 40 min at −0.90 V vs. reversible hydrogen electrode and nearly 100% NH3 selectivity at −0.80 V, surpassing the performance of both Co–B and CoOx catalysts. Furthermore, Co–B@CoOx demonstrates an ultra-low energy consumption of 0.39 kW h molNO3−1, establishing it as one of the most active catalysts available. Comprehensive experimental investigations and theoretical calculations indicate that the high conversion efficiency of Co–B@CoOx originates from the formation of local nucleophilic/electrophilic regions at the Co–B/CoOx Mott–Schottky interface, which effectively optimizes the targeted adsorption behavior of NO3 at the Co–B site and H2O at the CoOx site, thereby enhancing simultaneously NO3 affinity and active hydrogen availability. Furthermore, a novel Zn–NO3 battery utilizing the Co–B@CoOx catalyst delivers a remarkable power density of 4.78 mW cm−2, outperforming most recently reported Zn–NO3 batteries.

中文翻译:

莫特-肖特基接触协同促进低硝酸盐浓度下硝酸盐电还原为氨

电催化硝酸盐还原反应(NO 3 RR)在修复地下水中NO 3 -污染和获得清洁氨(NH 3)方面具有巨大潜力。然而,由于反应动力学缓慢,目前报道的NO 3 RR催化剂在低NO 3 -浓度下实现高转化效率面临挑战。在此,我们提出了一种高效的莫特-肖特基电催化剂,由嵌入非晶 CoO x纳米片中的非晶 Co-B 纳米链组成(Co-B@CoO x)。在100 ppm NO 3 –N 中,Co-B@CoO x催化剂表现出卓越的性能,在-0.90 V 条件下(相对于可逆氢电极)40 分钟内实现了超过 95% 的 NO 3 去除率,在 − 条件下实现了近 100% 的 NH 3选择性。 0.80 V,超越了 Co-B 和 CoO x催化剂的性能。此外,Co–B@CoO x表现出0.39 kW h mol NO 3 -1的超低能耗,使其成为最活跃的催化剂之一。综合实验研究和理论计算表明,Co-B@CoO x的高转换效率源于Co-B/CoO x Mott-Schottky界面上局部亲核/亲电子区域的形成,这有效优化了Co-B@CoO x 的靶向吸附行为。 NO 3 -位于 Co-B 位点,H 2 O 位于 CoO x位点,从而同时增强 NO 3 -亲和力和活性氢可用性。此外,利用Co-B@CoO x催化剂的新型Zn-NO 3 -电池可提供4.78 mW cm -2的显着功率密度,优于最近报道的Zn-NO 3 -电池。
更新日期:2024-03-19
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