Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-04-12 , DOI: 10.1016/j.apcatb.2020.118984 Xuesong Xu , Xiujuan Tian , Benteng Sun , Zhangqian Liang , Hongzhi Cui , Jian Tian , Minhua Shao
Herein, 1T-phase MoS2 nanodots (NDs) anchored to g-C3N4 (1T-MoS2/g-C3N4) are firstly developed to operate as a highly efficient catalyst for electrochemical N2 fixation with superior selectivity. 1T-MoS2/g-C3N4 composite presents outstanding NRR performance with a FE of 20.48 % and a NH3 yield rate of 29.97 μg h−1 mg−1cat. at -0.3 V vs. RHE. Furthermore, 1T-MoS2/g-C3N4 composite also shows outstanding electrochemical stability and durability. 15N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N2 in electrolyte rather than the decomposition of g-C3N4. DFT calculations reveal the optimal reaction path of NRR with both associative distal and alternating pathways. This work may offer a hopeful lead for designing effective non-noble-metal NRR electrocatalysts.
中文翻译:
1个T相硫化钼纳米点可在环境条件下有效地进行电催化固氮
在此,首先开发了锚定到gC 3 N 4(1T-MoS 2 / gC 3 N 4)的1T相MoS 2纳米点(NDs),以具有优异的选择性作为电化学固定N 2的高效催化剂。1T-MoS 2 / gC 3 N 4复合材料具有出色的NRR性能,FE为20.48%,NH 3产率为29.97μgh -1 mg -1猫。在-0.3V时与RHE。此外,1T-MoS 2 / gC 3 N 4复合材料还显示出出色的电化学稳定性和耐久性。15 N同位素标记实验证实,产生的氨中的氮源自电解质中的N 2而不是gC 3 N 4的分解。DFT计算揭示了NRR与远端和交替路径相关的最佳反应路径。这项工作可能为设计有效的非贵金属NRR电催化剂提供希望。