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Enhanced Electrocatalytic Nitrate-to-Ammonia Performance from Mott-Schottky Design to Induce Electron Redistribution
Chemical Science ( IF 7.6 ) Pub Date : 2024-11-18 , DOI: 10.1039/d4sc06818a Ruikai Qi, Qiuling Jiang, Li Deng, Xianqiang Yu, Bingyan Shi, Mengxiao Zhong, Ying Wang, Xiaofeng Lu
Chemical Science ( IF 7.6 ) Pub Date : 2024-11-18 , DOI: 10.1039/d4sc06818a Ruikai Qi, Qiuling Jiang, Li Deng, Xianqiang Yu, Bingyan Shi, Mengxiao Zhong, Ying Wang, Xiaofeng Lu
Constructing highly efficient electrocatalysts via interface manipulation and structural design to facilitate rapid electron transfer in electrocatalytic nitrate-to-ammonia conversion is crucial to attaining superior NH3 yield rate. Here, a Mott-Schottky type electrocatalyst of Co/In2O3 with a continuous fiber structure has been designed to boost the electrocatalytic nitrate-to-ammonia performance. The optimized Co/In2O3-1 catalyst exhibits an impressive NH3 yield rate of 70.1 mg cm-2 h-1 at –0.8 V vs. reversible hydrogen electrode (RHE), along with a NH3 faradaic efficiency (FE) of 93.34% at 0 V vs. RHE, greatly outperforming the single-component Co and In2O3 samples. The yield rate of the Co/In2O3-1 is also superior to most currently reported Co-based catalysts and heterostructured ones. Evidences from experiments and theoretical results confirm the formation of Mott-Schottky heterojunction, which achieves a Co site enriched with electrons, coupled with In2O3 facet enriched with holes, inducing an electron redistribution to promote the utilization of electroactive sites. Consequently, the reaction energy barrier for nitrate-to-ammonia is significantly reduced, further enhancing its yield efficiency.
中文翻译:
通过 Mott-Schottky 设计增强电催化硝酸盐制氨性能以诱导电子再分布
通过界面操作和结构设计构建高效的电催化剂,以促进电催化硝酸盐到氨转化中的快速电子转移,对于获得卓越的 NH3 产率至关重要。这里设计了一种具有连续纤维结构的 Co/In2O3 Mott-Schottky 型电催化剂,以提高电催化硝酸盐制氨的性能。与可逆氢电极 (RHE) 相比,优化后的 Co/In2O3-1 催化剂在 –0.8 V 下的 NH3 产率高达 70.1 mg cm-2 h-1,在 0 V 与 RHE 相比,NH3 法拉第效率 (FE) 为 93.34%,大大优于单组分 Co 和 In2O3 样品。Co/In2O3-1 的产率也优于目前报道的大多数 Co 基催化剂和异质结构催化剂。实验证据和理论结果证实了 Mott-Schottky 异质结的形成,它实现了富含电子的 Co 位点,再加上富含空穴的 In2O3 面,诱导电子重新分布,促进电活性位点的利用。因此,硝酸盐制氨的反应能垒显著降低,进一步提高了其产率效率。
更新日期:2024-11-18
中文翻译:
通过 Mott-Schottky 设计增强电催化硝酸盐制氨性能以诱导电子再分布
通过界面操作和结构设计构建高效的电催化剂,以促进电催化硝酸盐到氨转化中的快速电子转移,对于获得卓越的 NH3 产率至关重要。这里设计了一种具有连续纤维结构的 Co/In2O3 Mott-Schottky 型电催化剂,以提高电催化硝酸盐制氨的性能。与可逆氢电极 (RHE) 相比,优化后的 Co/In2O3-1 催化剂在 –0.8 V 下的 NH3 产率高达 70.1 mg cm-2 h-1,在 0 V 与 RHE 相比,NH3 法拉第效率 (FE) 为 93.34%,大大优于单组分 Co 和 In2O3 样品。Co/In2O3-1 的产率也优于目前报道的大多数 Co 基催化剂和异质结构催化剂。实验证据和理论结果证实了 Mott-Schottky 异质结的形成,它实现了富含电子的 Co 位点,再加上富含空穴的 In2O3 面,诱导电子重新分布,促进电活性位点的利用。因此,硝酸盐制氨的反应能垒显著降低,进一步提高了其产率效率。