He Y X, Wang Z L, Jiang Q
Key Laboratory of Automobile Materials, Ministry of Education, and School of Materials Science and Engineering, Jilin University, Changchun, 130022, China.
Chemphyschem. 2025 Mar 15;26(6):e202400788. doi: 10.1002/cphc.202400788. Epub 2025 Jan 14.
Electrochemical reduction of nitrate to ammonia (NORR) offers a promising strategy for renewable ammonia (NH) synthesis and wastewater treatment, but still suffers from limited activity and NH selectivity due to the lack of effective electrocatalyst. Here, we perform a four-steps screening strategy to screen high performance NORR catalyst by density functional theory calculations using 23 single transition metals atom doped on 1T-WS/graphene (TM@1T-WS/graphene) as candidates. The results show that Cu@1T-WS/graphene exhibits the highest NORR performance among 23 candidates with a low rate determining step energy barrier of 0.12 eV, which is much lower than that of the most of recently reported NORR catalysts. Moreover, the Cu@1T-WS/graphene also possesses excellent NH selectivity by suppressing competing hydrogen evolution reaction. This work provides a new avenue for the design of effective electrocatalysts for NORR.
将硝酸盐电化学还原为氨（NORR）为可再生氨（NH₃）合成和废水处理提供了一种很有前景的策略，但由于缺乏有效的电催化剂，其活性和NH₃选择性仍然有限。在此，我们采用四步筛选策略，通过密度泛函理论计算，以23种单过渡金属原子掺杂在1T-WS₂/石墨烯（TM@1T-WS₂/石墨烯）上作为候选物来筛选高性能的NORR催化剂。结果表明，Cu@1T-WS₂/石墨烯在23种候选物中表现出最高的NORR性能，其速率决定步骤的能垒低至0.12 eV，远低于最近报道的大多数NORR催化剂。此外，Cu@1T-WS₂/石墨烯还通过抑制竞争性析氢反应而具有优异的NH₃选择性。这项工作为设计用于NORR的有效电催化剂提供了一条新途径。
