Tuning single metal atoms anchored on graphdiyne for highly efficient and selective nitrate electroreduction to ammonia under aqueous environments: A computational study

Catalytic active centers beyond transition metals: atomically dispersed alkaline-earth metals for the electroreduction of nitrate to ammonia

“…5, interestingly, which also exhibits a prototypical volcanoshaped correlation, similar to the case of SACs with TM as the active center. 45,[47][48][49]52 One can see that, on the le branch of the volcano diagram, too strong adsorption of NO 3 − oen leads to the last hydrogenation step (*OH / * + H 2 O) as PDS, while the relatively weak adsorption of NO 3 − results in the early 5) possessing acceptable U L , which are comparable to the reported TM catalysts, marked by the purple circle in Fig. 5.…”

“…[45][46][47][48][49][50] Furthermore, it is noted that DG(*NO 3 ) of the above AE-SACs stand in the range from −1.3 to −2.5 eV, similar to the systems with TM active centers. [45][46][47][48][49][50] To get more insight into the reaction mechanism, the eNO 3 RR pathways on DV-BaN 3 C and DV-SrN 3 C are plotted in Fig. 6, and those for other systems are depicted in Fig.…”

“…Therefore, *NO will further undergo electrochemical hydrogenation on DV-BaN 3 C and DV-SrN 3 C. On the other side, the NO dimer (N 2 O 2 ) with cis O]N-N]O structure is the vital precursor to form N 2 O and N 2 , which could be formed by the coupling of two NO. 49,76,77 Obviously, the isolated single-atom active site cannot accommodate two NO 3 − simultaneously, and thus Langmuir-Hinshelwood mechanism for the formation of NO dimer can be excluded. 78 For the Eley-Rideal mechanism, the *NO needs to combine with a solvated NO molecule to form a NO dimer.…”

“…[40][41][42] For eNO 3 RR, several SACs have been reported experimentally 32,38,43,44 or theoretically. [45][46][47][48][49][50][51][52] Interestingly, for these SACs, it is predicted that the binding strength of NO 3 − could serve as a descriptor to predict the activity trend, and the active center with the adsorption-free energy for NO 3…”

Revealing the pH-dependent mechanism of nitrate electrochemical reduction to ammonia on single-atom catalysts

“…25 In addition, Zhou 26 identified that Ru/g-C 3 N 4 , among all the SACs on g-C 3 N 4 , is the most promising catalyst for NO 3 RR to NH 3 and provides a stimulating impetus for further experimental exploration. Zhao 27 identified that Os/GDY is an ideal NO 3 RR catalyst with a low limiting potential (−0.37 V) and great suppression effect on the competing reactions. And Hu 28 found that O-vacant Ti 3 C 2 O 2 MXene is the most effective MXene-based NRA electrocatalyst after systematic consideration of thermodynamics, reaction kinetics, and competitive relationship with the HER.…”