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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
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
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。