Zhang Ling, Wang Runzhi, Liang Li Guo, Niu Hexu, Bai Yiling, Jiao Tianao, Zhang Xuehua, Liu Rongji, Streb Carsten, Yuan Menglei, Zhang Guangjin
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, PR China; Center of Materials Science and Optoelectronics Engineering, Chinese Academy of Sciences, Beijing 100049, PR China; CAS Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, PR China.
Center of Materials Science and Optoelectronics Engineering, Chinese Academy of Sciences, Beijing 100049, PR China; CAS Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, PR China.
J Colloid Interface Sci. 2024 Dec 15;676:636-646. doi: 10.1016/j.jcis.2024.07.164. Epub 2024 Jul 21.
The electrocatalytic nitrate reduction reaction (NO RR) has immense potential to alleviate the problem of groundwater pollution and may also become a key route for the environmentally benign production of ammonia (NH) products. Here, the unique effects of interfacial electric fields arising from asymmetric chemical potentials and local defects were integrated into the binary BiS-BiO sublattices for enhancing electrocatalytic nitrate reduction reactions. The obtained binary system showed a superior Faraday efficiency (FE) for ammonia production of 94 % and an NH yield rate of 89.83 mg gh at -0.4 V vs. RHE. Systematic experimental and computational results confirmed that the concerted interplay between interfacial electric fields and local defects not only promoted the accumulation and adsorption of NO, but also contributed to the destabilization of *NO and the subsequent deoxygenation hydrogenation reaction. This work will stimulate future designs of heterostructured catalysts for efficient electrocatalytic nitrate reduction reactions.
电催化硝酸盐还原反应（NO RR）在缓解地下水污染问题方面具有巨大潜力，并且也可能成为环境友好型氨（NH）产品生产的关键途径。在此，由不对称化学势和局部缺陷产生的界面电场的独特效应被整合到二元BiS-BiO亚晶格中，以增强电催化硝酸盐还原反应。所获得的二元体系在相对于可逆氢电极（RHE）为-0.4 V时，对氨生产表现出94%的优异法拉第效率（FE）和89.83 mg g h的NH产率。系统的实验和计算结果证实，界面电场与局部缺陷之间的协同相互作用不仅促进了NO的积累和吸附，而且有助于*NO的去稳定化以及随后的脱氧氢化反应。这项工作将激发未来用于高效电催化硝酸盐还原反应的异质结构催化剂的设计。
