期刊
ACS ENERGY LETTERS
卷 -, 期 -, 页码 1281-1288出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.2c02882
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In this study, p-block Sb and Bi single-atom catalysts were designed and showed high efficiency in electrocatalytic NO reduction to NH3, with great potential for commercial applications.
Electrocatalytic NO reduction to NH3 (NORR) offers a prospective approach to attain both harmful NO removal and efficient NH3 electrosynthesis. Main-group p-block metals are promising NORR candidates but still lack adequate exploration. Herein, p-block Sb single atoms confined in amorphous MoO3 (Sb1/a-MoO3) are designed as an efficient NORR catalyst, exhibiting the highest NH3 yield rate of 273.5 mu mol h-1 cm-2 and a NO-to-NH3 Faradaic efficiency of 91.7% at -0.6 V vs RHE. In situ spectroscopic characterizations and theoretical computations reason that the outstanding NORR performance of Sb1/ a-MoO3 arises from the isolated Sb1 sites, which can optimize the adsorption of *NO/*NHO to lower the reaction energy barriers and simultaneously exhibit a higher affinity to NO than to H2O/H species. Moreover, our strategy can be extended to prepare Bi1/a-MoO3, showing a high NORR property, demonstrating the immense potential of p-block metal single-atom catalysts toward the high-performing NORR electrocatalysis.
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