An efficient screening strategy towards multifunctional catalysts for the simultaneous electroreduction of NO3−, NO2− and NO to NH3. Issue 17 (4th April 2022)

• Record Type: Journal Article
• Authors: Lv, Peng; Wu, Donghai; He, Bingling; Li, Xue; Zhu, Rui; Tang, Gang; Lu, Zhansheng; Ma, Dongwei; Jia, Yu
• Is Part Of: Journal of materials chemistry. Volume 10:Issue 17(2022)
• Page Start: 9707
• Page End: 9716
• Publication Date: 2022-04-04
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/d2ta00192f
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : An efficient strategy focusing on the key protonation process was confirmed to screen multifunctional electrocatalysts for the NORR, NO2 RR and NO3 RR. Abstract : Multifunctional electrocatalysts that simultaneously reduce all NO x species (NO3 −, NO2 − and NO) to NH3 can deliver superior efficiency compared with that for individual species. Herein, by using the first-principles method, an efficient strategy was proposed to screen NO x RR multifunctional electrocatalysts, which focuses on the key protonation process of the essential NORR for the NO x RR. Taking double-atom catalysts (DACs) with transition-metal dimer (M1/M2 = V, Cr, Mn, Fe, Co, Ni, and Cu) embedded N-doped graphene as examples, we showed that the proposed strategy was effective for electrocatalyst screening, and we identified Cu2 @NG as the best one, with rather low limiting potentials of −0.36, −0.32, and −0.30 V for the NO3 RR, NO2 RR, and NORR, respectively. Furthermore, a simple descriptor for evaluating electrocatalytic activity was established. And the physical mechanism in terms of the electronic structures was analyzed for the Cu2 DAC case in view of NO activation. Finally, from the screening test in some 4d and 5d late transition-metal based DACs, the proposed strategy was confirmed to be feasible to find another NO x RR multifunctional electrocatalyst. Our work provides a procedure for efficiently screening multifunctional electrocatalysts to simultaneously reduce all NO x species to synthesize NH3 and sheds light on the atomic mechanisms for NO x electroreduction as well.